Perovskite Light-Emitting Devices - Fundamentals and Working Principles

Perovskite solar cells employing organic charge-transport layers

Thin-film photovoltaics play an important role in the quest for clean renewable energy. Recently, methylammonium lead halide perovskites were identified as promising absorbers for solar cells(1). In the three years since, the performance of perovskite-based solar cells has improved rapidly to reach efficiencies as high as 15%(1-10). To date, all high-efficiency perovskite solar cells reported make use of a (mesoscopic) metal oxide, such as Al2O3, TiO2, or ZrO2, which requires a high-temperature sintering process. Here, we show that methylammonium lead iodide perovskite layers, when sandwiched between two thin organic charge-transporting layers, also lead to solar cells with high power-conve…

Influence of hole transport material ionization energy on the performance of perovskite solar cells

Halide perovskites have shown excellent photophysical properties for solar cell applications which led to a rapid increase of the device efficiency. Understanding the charge carrier dynamics within the active perovskite absorber and at its interfaces will be key to further progress in their development. Here we present a series of fully evaporated devices employing hole transport materials with different ionization energies. The open circuit voltage of the devices, along with their ideality factors, confirm that the former is mainly determined by the bulk and surface recombination in the perovskite, rather than by the energetic offset between the valence band of the perovskite and the highe…

Green Light-Emitting Solid-State Electrochemical Cell Obtained from a Homoleptic Iridium(III) Complex Containing Ionically Charged Ligands

An efficient bluish-green light-emitting Ir(III) complex was prepared by introducing charged side groups onto phenylpyridine ligands. Green light emission with a first maximum at 487 nm (CIE coordinates x = 0.337 and y = 0.501) was observed from a single layer light-emitting electrochemical cell using this new complex; this is the lowest wavelength observed so far for devices based on ionic transition metal complexes.

Tetra-alkoxy substituted PPV derivatives: a new class of highly soluble liquid crystalline conjugated polymers

Two first examples of highly soluble tetra-alkoxy substituted PPV derivatives, poly(2,3,5,6-tetrahexyloxy-1,4-phenylene vinylene) (TH-PPV) and poly[2,3,5,6-tetra(2'-ethyl-hexyloxy)-1,4-phenylene vinylene] TEH-PPV, are presented. Both polymers have been fully characterized and the solubility and UV-Vis absorption characteristics have been studied in various organic solvents. Due to the symmetric nature of the repeating unit, TH-PPV and TEH-PPV have an inherently regioregular nature, which is unusual for PPV-type polymers. Observations from polarized light microscopy and differential scanning calorimetry indicate that TH-PPV exhibits thermally induced order resulting in a liquid crystalline m…

Polymer‐Based Composites for Engineering Organic Memristive Devices

Memristive materials are related to neuromorphic applications as they can combine information processing with memory storage in a single computational element, just as biological neurons. Many of these bioinspired materials emulate the characteristics of memory and learning processes that happen in the brain. In this work, we report the memristive properties of a two-terminal (2-T) organic device based on ionic migration mediated by an ion-transport polymer. The material possesses unique memristive properties: it is reversibly switchable, shows tens of conductive states, presents Hebbian learning demonstrated by spiking time dependent plasticity (STDP), and behaves with both short- (STM) an…

Interfacial Modification for High-Efficiency Vapor-Phase-Deposited Perovskite Solar Cells Based on a Metal Oxide Buffer Layer.

Vacuum deposition is one of the most technologically relevant techniques for the fabrication of perovskite solar cells. The most efficient vacuum-based devices rely on doped organic contacts, compromising the long-term stability of the system. Here, we introduce an inorganic electron-transporting material to obtain power conversion efficiencies matching the best performing vacuum-deposited devices, with open-circuit potential close to the thermodynamic limit. We analyze the leakage current reduction and the interfacial recombination improvement upon use of a thin (<10 nm) interlayer of C60, as well as a more favorable band alignment after a bias/ultraviolet light activation process. This wo…

Efficient Polymer Light‐Emitting Diode Using Air‐Stable Metal Oxides as Electrodes

Poly(phenylenevinylene)‐based organic light‐emitting diodes (OLEDs) are fabricated using air‐stable metal oxides as electrodes, producing very efficient and bright electroluminescent devices. Efficiencies of 8 cd A−1 and luminances above 20000 cd m−2 are obtained, comparable to the values reported for classic OLED structures using reactive metals as cathodes.

Near-UV to red-emitting charged bis-cyclometallated iridium(iii) complexes for light-emitting electrochemical cells

Herein we report a series of charged iridium complexes emitting from near-UV to red using carbene-based N^C: ancillary ligands. Synthesis, photophysical and electrochemical properties of this series are described in detail together with X-ray crystal structures. Density Functional Theory calculations show that the emission originates from the cyclometallated main ligand, in contrast to commonly designed charged complexes using bidentate N^N ancillary ligands, where the emission originates from the ancillary N^N ligand. The radiative process of this series of compounds is characterized by relatively low photoluminescence quantum yields in solution that is ascribed to non-radiative deactivati…

Consistent device simulation model describing perovskite solar cells in steady-state, transient, and frequency domain

​This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials & Interfaces, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acsami.9b04991

Efficient Vacuum Deposited P-I-N Perovskite Solar Cells by Front Contact Optimization.

Hole transport layers HTLs are of fundamental importance in perovskite solar cells PSCs , as they must ensure an efficient and selective hole extraction, and ohmic charge transfer to the corresponding electrodes. In p i n solar cells, the ITO HTL is usually not ohmic, and an additional interlayer such as MoO3 is usually placed in between the two materials by vacuum sublimation. In this work, we evaluated the properties of the MoO3 TaTm TaTm is the HTL N4,N4,N4 amp; 8243;,N4 amp; 8243; tetra [1,1 amp; 8242; biphenyl] 4 yl [1,1 amp; 8242; 4 amp; 8242;,1 amp; 8243; terphenyl] 4,4 amp; 8243; diamine hole extraction interface by selectively annealing either MoO3 prior to the deposition of TaTm o…

Inside Front Cover: Long-Living Light-Emitting Electrochemical Cells - Control through Supramolecular Interactions (Adv. Mater. 20/2008)

Efficient blue emitting organic light emitting diodes based on fluorescent solution processable cyclic phosphazenes

Solution processable blue fluorescent dendrimers based on cyclic phosphazene (CP) cores incorporating amino-pyrene moieties have been prepared and used as emissive layers in organic light emitting diodes (OLEDs). These dendrimers have high glass transition temperatures, are monodisperse, have high purity via common chromatographic techniques, and form defect-free amorphous films via spin/dip coating. The solution processable blue light emitting OLEDs reach current efficiencies of 3.9 cd/A at brightness levels near 1000 cd/m2. Depending on the molecular bridge used to attach the fluorescent dendron to the inorganic core, the emission wavelength changes from 470 to 545 nm, corresponding to bl…

Self-assembled hierarchical nanostructured perovskites enable highly efficient LEDs via an energy cascade

Metal halide perovskites have established themselves as extraordinary optoelectronic materials, exhibiting promise for applications in large area illumination and displays. However, low luminescence, low efficiencies of the light-emitting diodes (LEDs), and complex preparation methods currently limit further progress towards applications. Here, we report on a new and unique mesoscopic film architecture featuring the self-assembly of 3D formamidinium lead bromide (FAPbBr3) nanocrystals of graded size, coupled with microplatelets of octylammonium lead bromide perovskites that enables an energy cascade, yielding very high-performance light-emitting diodes with emission in the green spectral re…

Temperature dependence of Photoluminescence and Amplified Spontaneous Emission in thin films of quasi-2D BA3MA3Pb5Br16 perovskites

Increased conductivity of a hole transport layer due to oxidation by a molecular nanomagnet

Thin film transistors based on polyarylamine poly?N,N?-diphenyl-N,N ?bis?4-hexylphenyl?- ?1,1?biphenyl?-4,4?-diamine ?pTPD? were fabricated using spin coating in order to measure the mobility of pTPD upon oxidation. Partially oxidized pTPD with a molecular magnetic cluster showed an increase in mobility of over two orders of magnitude. A transition in the mobility of pTPD upon doping could also be observed by the presence of a maximum obtained for a given oxidant ratio and subsequent decrease for a higher ratio. Such result agrees well with a previously reported model based on the combined effect of dipolar broadening of the density of states and transport manifold filling. Peer Reviewed

Efficient Green Light-Emitting Electrochemical Cells Based on Ionic Iridium Complexes with Sulfone-Containing Cyclometalating Ligands

A new approach to obtain green-emitting iridiumA complexes is described. The synthetic approach consists of introducing a methylsulfone electron-withdrawing substituent into a 4-phenylpyrazole cyclometalating ligand in order to stabilize the highest- occupied molecular orbital (HOMO). Six new complexes have been synthe- sized incorporating the conjugate base of 1-(4-(methylsulfonyl)phenyl)-1 H- pyrazole as the cyclometalating ligand. The complexes show green emission and very high photoluminescence quantum yields in both diluted and concentrated films. When used as the main active component in light-emit- ting electrochemical cells (LECs), green electroluminance is observed. High efficienci…

Lowest triplet excited states of a novel heteroleptic iridium(III) complex and their role in the emission colour

Abstract The [Ir(ppy-F 2 ) 2 Me 4 phen] +1 complex, where ppy-F 2 is 2-(2′,4′-fluorophenyl)pyridine and Me 4 phen is 3,4,7,8-tetramethyl-1,10-phenanthroline, has been theoretically investigated by means of DFT calculations. The molecular and electronic properties calculated for [Ir(ppy-F 2 ) 2 Me 4 phen] +1 are compared with those obtained for the simpler [Ir(ppy)(bpy)] +1 complex. The introduction of fluorine substituents in the ppy ligands and the use of phenanthroline instead of 2,2′-bipyridine as the diimine ligand increase the HOMO–LUMO energy gap and blue-shift the emission colour. The phenanthroline ligand causes the appearance of two nearly-degenerate LUMO orbitals of different symm…

Dual-source vacuum deposition of pure and mixed halide 2D perovskites: thin film characterization and processing guidelines

The dual-source vacuum deposition of 2D perovskite films of the type PEA2PbX4, (PEA = phenethylammonium and X = I−, Br−, or a combination of both) is presented. Low-temperature deposited 2D perovskite films showed high crystallinity with the expected trend of bandgap as a function of halide type and concentration. Importantly, we observed an unavoidable halide cross-contamination among different deposition runs, as well as a strong dependence of the material quality on the type of halide precursors used. These findings should be taken into account in the development of vacuum processing for low-dimensional mixed halide perovskites.

Perovskite/Perovskite Tandem Solar Cells in the Substrate Configuration with Potential for Bifacial Operation.

Perovskite/perovskite tandem solar cells have recently exceeded the record power conversion efficiency (PCE) of single-junction perovskite solar cells. They are typically built in the superstrate configuration, in which the device is illuminated from the substrate side. This limits the fabrication of the solar cell to transparent substrates, typically glass coated with a transparent conductive oxide (TCO), and adds constraints because the first subcell that is deposited on the substrate must contain the wide-bandgap perovskite. However, devices in the substrate configuration could potentially be fabricated on a large variety of opaque and inexpensive substrates, such as plastic and metal fo…

Advances in Perovskite Optoelectronics: Bridging the Gap Between Laboratory and Fabrication

In 2019, hybrid halide perovskites celebrated their 10th anniversary as a "wonder material" for optoelectronic applications. Although the parent perovskite structures were elucidated in the late 19th century, the seminal work by Miyasaka et al. exploiting organic‐inorganic hybrid halide perovskites sensitizers for visible‐light conversion in solar cells marked the revisit of these materials and has proven to be a game‐changer in this field. Extensive investigations were undertaken to develop new materials (all inorganic and organic‐inorganic hybrids, in the form of films or alternate morphologies) and deposition techniques, explore interfaces and in‐depth characterization, while engineering…

Synthesis and luminescence of poly(phenylacetylene)s with pendant iridium complexes and carbazole groups

Poly(phenylacetylene)s containing pendant phosphorescent iridium complexes have been synthesized and their electrochemical, photo- and electroluminescent properties studied. The polymers have been synthesized by rhodium-catalyzed copolymerization of 9-(4-ethynylphenyl)carbazole (CzPA) and phenylacetylenes (C∧N)2Ir(κ2-O,O′-MeC(O)CHC(O)C6H4CCH-4) (C∧N = κ2-N,C1-2-(pyridin-2-yl)phenyl (IrppyPA) or κ2-N,C1-2-(isoquinolin-1-yl)phenyl (IrpiqPA)). In addition, organic poly(phenylacetylene)s with pendant carbazole groups have been synthesized by rhodium-catalyzed copolymerization of CzPA and 1-ethynyl-4-pentylbenzene. Complex (C∧N)2Ir(κ2-O,O′-MeC(O)CHC(O)Ph) (IrpiqPh; C∧N = 2-(isoquinolin-1-yl)phen…

Host–guest blue light-emitting electrochemical cells

Carbazole, a commonly used hole-transporter for organic electronics, has been modified with an imidazolium cation and a hexafluorophosphate counter-anion to give an ionic hole-transporter. It has been applied as one of the hosts in a host–guest blue light-emitting electrochemical cell (LEC) with the neutral blue emitter FIrPic. We have obtained efficient and bright blue LECs with an electroluminescence maximum at 474 nm and efficacy of 5 cd A−1 at a luminance of 420 cd m−2, thereby demonstrating the potential of the ionic organic charge-transporters and of the host–guest architecture for LECs.

Stable Green Electroluminescence from an Iridium Tris-Heteroleptic Ionic Complex

An ionic tris-heteroleptic iridium complex gives green light-emitting electrochemical cells (LECs) with unprecedented performances for this part of the visible spectrum. The devices are very bright (>1000 cd m–2), efficient (∼3%), and stable (>55 h). The novel complex is prepared using a new and efficient synthetic procedure. We show that there is a mixed orbital formation originating from the two different orthometalating ligands resulting in photophysical properties that lie between those of its two bis-heteroleptic analogs. Therefore, tris-heteroleptic complexes provide new avenues for fine-tunning the emission properties and to bridge gaps between a series of bis-heteroleptic complexes.

Vacuum deposited perovskite solar cells employing dopant-free triazatruxene as the hole transport material

Abstract Planar perovskite solar cells using organic charge selective contacts were fabricated. In a vacuum deposited perovskite-based solar cell, dopant and additive free triazatruxene as the hole transport layer was introduced for device fabrication. High open-circuit voltage of 1090 mV was obtained using methylammonium lead iodide (Eg=1.55 eV) as light harvesting material, thus representing a loss of only 460 mV which is in close vicinity of mature silicon technology (400 mV). The devices showed a very competitive photovoltaic performance, monochromatic incident photon-to-electron conversion efficiency of 80% and the power conversion efficiencies in excess of 15% were measured with a neg…

Making by Grinding: Mechanochemistry Boosts the Development of Halide Perovskites and Other Multinary Metal Halides

Mechanochemical synthesis has recently emerged as a promising route for the synthesis of functional lead halide perovskites as well as other (lead‐free) metal halides. Mechanochemical synthesis presents several advantages with regards to more commonly used solution‐based processes such as an inherent lower toxicity by avoiding organic solvents and a finer control over stoichiometry of the final products. The ease of implementation, either through the use of a simple mortar and pestle or with an electrically powered ball‐mill, and low amount of side products make mechanochemical synthesis appealing for upscaling the production of halide perovskites. Due to the defect tolerance of lead halide…

ChemInform Abstract: Luminescent Ionic Transition Metal Complexes for Light-Emitting Electrochemical Cells

Higher efficiency in the end-use of energy requires substantial progress in lighting concepts. All the technologies under development are based on solid-state electroluminescent materials and belong to the general area of solid-state lighting (SSL). The two main technologies being developed in SSL are light-emitting diodes (LEDs) and organic light-emitting diodes (OLEDs), but in recent years, light-emitting electrochemical cells (LECs) have emerged as an alternative option. The luminescent materials in LECs are either luminescent polymers together with ionic salts or ionic species, such as ionic transition-metal complexes (iTMCs). Cyclometalated complexes of IrIII are by far the most utiliz…

Dumbbell-Shaped Dinuclear Iridium Complexes and Their Application to Light-Emitting Electrochemical Cells

A novel family of dumbbell- shaped dinuclear complexes in which an oligophenyleneethynylene spacer is linked to two heteroleptic iridiumA complexes is presented. The synthesis, as well as the electrochemical and pho- tophysical characterization of the new complexes, is reported. The experimen- tal results are interpreted with the help of density functional theory calcula- tions. From these studies we conclude that the lowest triplet excited state cor- responds to a 3 p-p* state located on the conjugated spacer. The presence of this state below the 3 MLCT/ 3 LLCT emitting states of the end-capping Ir III complexes explains the low quantum yields observed for the dinuclear com- plexes (one or…

Simultaneous determination of carrier lifetime and electron density-of-states in P3HT:PCBM organic solar cells under illumination by impedance spectroscopy

We report new insights into recombination kinetics in poly(3-hexylthiophene):methanofullerene (P3HT:PCBM) bulk heterojunction (BHJ) solar cells, based on simultaneous determination of the density of states (DOS), internal recombination resistance, and carrier lifetime, at different steady states, by impedance spectroscopy. A set of measurements at open circuit under illumination was performed aiming to better understand the limitations to the photovoltage, which in this class of solar cells remains far below the theoretical limit which is the difference between the LUMO level of PCBM and the HOMO of P3HT (∼1.1 eV). Recombination kinetics follows a bimolecular law, being the recombination ti…

Self-absorption in a light-emitting electrochemical cell based on an ionic transition metal complex

We report on the quantitative and qualitative effects of self-absorption in light-emitting electrochemical cells (LECs) based on ionic transition metal complexes (iTMCs), as measured in-situ during electric driving. A yellow-emitting iTMC-LEC comprising an active material thickness of 95 nm suffers a 4% loss of the emission intensity to self-absorption, whereas the same type of device but with a larger active-material thickness of 1 mu m will lose a significant 40% of the light intensity. We also find that the LEC-specific effect of doping-induced self-absorption can result in a drift of the emission spectrum with time for iTMC-LECs, but note that the overall magnitude of doping-induced sel…

Vapor-Deposited Perovskites: The Route to High-Performance Solar Cell Production?

Summary High-quality semiconducting perovskites can be easily synthesized through several methods. The ease of fabrication has favored the adoption of lab-scale solution-processing techniques, which have yielded the highest performing devices. Most of these processes, however, are not directly applicable to larger scale and volume preparations, hindering the consolidation and market entry of this technology. Vapor-based methods, a mature technology widely adopted in the coating and semiconductor industry, could change this trend. Their application to perovskite solar cells includes a large amount of fabrication approaches, offering versatility in the employed materials as well as in the cha…

Potential and limitations of CsBi3I10 as a photovoltaic material

Herein we demonstrate the dry synthesis of CsBi3I10 both as a free-standing material and in the form of homogeneous thin films, deposited by thermal vacuum deposition. Chemical and optical characterization shows high thermal stability, phase purity, and photoluminescence centered at 700 nm, corresponding to a bandgap of 1.77 eV. These characteristics make CsBi3I10 a promising low-toxicity material for wide bandgap photovoltaics. Nevertheless, the performance of this material as a semiconductor in solar cells remains rather limited, which can be at least partially ascribed to a low charge carrier mobility, as determined from pulsed-radiolysis time-resolved microwave conductivity. Further dev…

Use of Hydrogen Molybdenum Bronze in Vacuum‐Deposited Perovskite Solar Cells

Herein, the dehydration of a hydrogen molybdenum bronze (HYMoO3), converting it to molybdenum oxide (MoOX), is explored toward the development of perovskite solar cells (PSCs) for the first time. H0.11MoO3 bronze is synthesized, characterized, and deposited on indium tin oxide (ITO) under different concentrations and annealing conditions for in situ conversion into MoOX with appropriate oxygen vacancies. Vacuum‐deposited PSCs are fabricated using the as‐produced MoOX hole injection layers, achieving a power conversion efficiency of 17.3% (average) for the optimal device. The latter has its stability and reproducibility tested, proving the robustness and affordability of the developed hole t…

Green light-emitting electrochemical cells based on platinum(ii) complexes with a carbazole-appended carbene ligand

This article is part of the themed collections: Paul R. Raithby at 70: in celebration of a life in chemistry, Recent Open Access Articles and 2022 Journal of Materials Chemistry C Most Popular Articles.

Green phosphorescence and electroluminescence of sulfur pentafluoride-functionalized cationic iridium(III) complexes

EZ-C acknowledges the University of St Andrews for financial support. We report four cationic iridium(III) complexes [Ir(C^N)2(dtBubpy)](PF6) that have sulfurpentafluoride-modified 1-phenylpyrazole and 2-phenylpyridine cyclometalating (C^N) ligands (dtBubpy = 4,4'-di-tert-butyl-2,2'-bipyridyl). Three of the complexes were characterized by single-crystal X-ray structure analysis. In cyclic voltammetry, the complexes undergo reversible oxidation of iridium(III) and irreversible reduction of the SF5 group. They emit bright green phosphorescence in acetonitrile solution and in thin films at room temperature, with emission maxima between 482–519 nm and photoluminescence quantum yields of up to 7…

Observation of electroluminescence at room temperature from a ruthenium(II) bis-terpyridine complex and its use for preparing light-emitting electrochemical cells.

A terpyridine ruthenium (II) complex containing a substituted and an unsubstituted terpyridine ligand was synthesized, and its luminescence properties were studied in a solid-state single-layer light-emitting electrochemical cell. The obtained devices emitted light of a very deep red color (CIE, x = 0.717 y = 0.282) at low external applied bias. It is the first example of an electroluminescence device based on a bis-chelated ruthenium complex. Its ambient atmosphere decay is remarkably different from analogous devices using tris-chelated ruthenium complexes.

Thienylpyridine-based cyclometallated iridium(III) complexes and their use in solid state light-emitting electrochemical cells

The synthesis and characterization of four iridium(iii) complexes [Ir(thpy)2(N^N)][PF6] where Hthpy = 2-(2'-thienyl)pyridine and N^N are 6-phenyl-2,2'-bipyridine (1), 4,4'-di-(t)butyl-2,2'-bipyridine (2), 4,4'-di-(t)butyl-6-phenyl-2,2'-bipyridine (3) or 4,4'-dimethylthio-2,2'-bipyridine (4) are described. The single crystal structures of ligand 4 and the complexes containing the [Ir(thpy)2(1)](+) and [Ir(thpy)2(4)](+) cations have been determined. In [Ir(thpy)2(1)](+), the pendant phenyl ring engages in an intra-cation π-stacking interaction with one of the thienyl rings in the solid state, and undergoes hindered rotation on the NMR timescale in [Ir(thpy)2(1)](+) and [Ir(thpy)2(3)](+). The …

Solution, structural and photophysical aspects of substituent effects in the N^N ligand in [Ir(C^N)2(N^N)]+ complexes

The syntheses and properties of a series of eleven new [Ir(ppy)2(N^N)][PF6] complexes (Hppy = 2-phenylpyridine) are reported. The N^N ligands are based on 2,2-bipyridine (bpy), substituted in the 6- or 5-positions with groups that are structurally and electronically diverse. All but two of the N^N ligands incorporate an aromatic ring, designed to facilitate intra-cation face-to-face π-interactions between the N^N and one [ppy](-) ligand. Within the set of ligands, 6-(3-tolyl)-2,2'-bipyridine (5), 4,6-bis(4-nitrophenyl)-2,2'-bipyridine (9), and 4,6-bis(3,4,5-trimethoxyphenyl)-2,2'-bipyridine (10) are new and their characterization includes single crystal structures of 9, and two polymorphs o…

Controlling the dynamic behavior of light emitting electrochemical cells

Abstract Light emitting electrochemical cells (LECs) present an attractive route towards cost efficient lighting applications. By utilizing ionic phosphorescent transition metal complexes, efficient electroluminescence can be realized from a single layer device using air stable electrodes. These devices achieve efficient charge carrier injection due to ion accumulation at the interface upon driving, resulting in a dynamic response upon device operation. Here we investigate the device operation by using fast current and luminance versus voltage sweeps during normal fixed bias operating. A universal set of JL–V curves can be identified in which different regimes are observable. The speed and …

Ionic liquid modified zinc oxide injection layer for inverted organic light-emitting diodes

Abstract We have demonstrated a novel approach for fabricating efficient hybrid organic–inorganic light emitting diodes (HyLEDs) by introducing dopants into solutions processable metal oxides as an interfacial layer. The doped ZnO is prepared by adding ionic liquid (IL) to a precursor solution for the ZnO. In this way a heavily doped ZnO:ILs cathode was obtained that enhances the electron injection properties and assures a good wetting of the organic active materials.

Inverted Solution Processable OLEDs Using a Metal Oxide as an Electron Injection Contact.

A new type of bottom-emission electroluminescent device is described in which a metal oxide is used as the electron-injecting contact. The preparation of such a device is simple. It consists of the deposition of a thin layer of a metal oxide on top of an indium tin oxide covered glass substrate, followed by the solution processing of the light-emitting layer and subsequently the deposition of a high-workfunction (air-stable) metal anode. This architecture allows for a low-cost electroluminescent device because no rigorous encapsulation is required. Electroluminescence with a high brightness reaching 5700 cd m–2 is observed at voltages as low as 8 V, demonstrating the potential of this new a…

ChemInform Abstract: Hybrid Organic-Inorganic Light-Emitting Diodes

The demonstration of colour tunability and high efficiency has brought organic light-emitting diodes (OLEDs) into the displays and lighting market. However, high production costs due to expensive deposition techniques and the use of reactive materials still limit their market entry, highlighting the need for novel concepts. This has driven the research towards the integration of both organic and inorganic materials into devices that benefit from their respective peculiar properties. The most representative example of this tendency is the application of metal oxides in organic optoelectronics. Metal oxides combine properties such as high transparency, good electrical conductivities, tuneable…

Hybrid organic-inorganic light-emitting diodes.

The demonstration of colour tunability and high efficiency has brought organic light-emitting diodes (OLEDs) into the displays and lighting market. However, high production costs due to expensive deposition techniques and the use of reactive materials still limit their market entry, highlighting the need for novel concepts. This has driven the research towards the integration of both organic and inorganic materials into devices that benefit from their respective peculiar properties. The most representative example of this tendency is the application of metal oxides in organic optoelectronics. Metal oxides combine properties such as high transparency, good electrical conductivities, tuneable…

Bright and stable light-emitting electrochemical cells based on an intramolecularly π-stacked, 2-naphthyl-substituted iridium complex

The synthesis and characterization of a new cationic bis-cyclometallated iridium(III) complex and its use in solid-state light-emitting electrochemical cells (LECs) are described. The complex [Ir(ppy)2(Naphbpy)][PF6], where Hppy = 2-phenylpyridine and Naphbpy = 6-(2-naphthyl)-2,2′-bipyridine, incorporates a pendant 2-naphthyl unit that π-stacks face-to-face with the adjacent ppy− ligand and acts as a peripheral bulky group. The complex presents a structureless emission centred around 595–600 nm both in solution and in thin film with relatively low photoluminescence quantum yields compared with analogous systems. Density functional theory calculations support the charge transfer character of…

External quantum efficiency measurements used to study the stability of differently deposited perovskite solar cells

The instability exhibited by perovskite solar cells when exposed to the environment under illumination is one of the major obstacles for the entry of perovskite technology in the photovoltaic market. In this work, we use the external quantum efficiency (EQE) technique to study the photoinduced degradation of two types of solar cells having CH3NH3PbI3 as an absorber layer: one deposited by spin coating with an n-i-p architecture and the other deposited by evaporation with an inverted p-i-n structure. We also study the effect of different encapsulants to protect the cells against atmospheric agents. We find that EQE provides information regarding the areas of the cell most susceptible to degr…

Highly Stable Red-Light-Emitting Electrochemical Cells

The synthesis and characterization of a series of new cyclometalated iridium(III) complexes [Ir(ppy) 2 (N ∧ N)][PF 6 ] in which Hppy = 2-phenylpyridine and N ∧ N is (pyridin-2-yl)benzo[ d ]thiazole ( L1 ), 2-(4-( tert -butyl)pyridin-2-yl)benzo[ d ]thiazole ( L2 ), 2-(6-phenylpyridin-2-yl)benzo[ d ]thiazole ( L3 ), 2-(4-( tert -butyl)-6-phenylpyridin-2-yl)benzo[ d ]thiazole ( L4 ), 2,6-bis(benzo[ d ]thiazol-2-yl)pyridine ( L5 ), 2-(pyridin-2-yl)benzo[ d ]oxazole ( L6 ), or 2,2′-dibenzo[ d ]thiazole ( L7 ) are reported. The single crystal structures of [Ir(ppy) 2 ( L1 )][PF 6 ]·1.5CH 2 Cl 2 , [Ir(ppy) 2 ( L6 )][PF 6 ]·CH 2 Cl 2 , and [Ir(ppy) 2 ( L7 )][PF 6 ] have been determined. The new com…

A comparative study of Ir(III) complexes with pyrazino[2,3-f][1,10]phenanthroline and pyrazino[2,3-f][4,7]phenanthroline ligands in light-emitting electrochemical cells (LECs).

We report the comparative study of the electrochemical and photoluminescent properties of two Ir(iii) complexes described as [Ir(F2ppy)2(N^N)][PF6], where the F2ppy ligand is 2-(2,4-difluorophenyl)pyridine and the N^N ligands are pyrazino[2,3-f][1,10]phenanthroline (ppl) and pyrazino[2,3-f][4,7]phenanthroline (ppz). The complexes were used for the fabrication of light-emitting electrochemical cells (LECs). The structures of the complexes have been corroborated by X-ray crystallography. Theoretical calculations were performed to understand the photophysical behavior of the complexes. Both in solution and solid state, the photoluminescence spectra shows that emission is significantly red-shif…

Short photoluminescence lifetimes in vacuum-deposited ch3nh3pbI3 perovskite thin films as a result of fast diffusion of photogenerated charge carriers

It is widely accepted that a long photoluminescence (PL) lifetime in metal halide perovskite films is a crucial and favorable factor, as it ensures a large charge diffusion length leading to a high power conversion efficiency (PCE) in solar cells. It has been recently found that vacuumevaporated CH3NH3PbI3 (eMAPI) films show very short PL lifetimes of several nanoseconds. The corresponding solar cells, however, have high photovoltage (>1.1 V) and PCEs (up to 20%). We rationalize this apparent contradiction and show that eMAPI films are characterized by a very high diffusion coefficient D, estimated from modeling the PL kinetics to exceed 1 cm2/s. Such high D values are favorable for long di…

Large area perovskite light-emitting diodes by gas-assisted crystallization:

Halide perovskites have been gaining considerable attention recently for use in light-emitting applications, due to their bandgap tunability, color purity and low cost fabrication methods. However, current fabrication techniques limit the processing to small-area devices. Here, we show that a facile N 2 gas-quenching technique can be used to make methylammonium lead bromide-based perovskite light-emitting diodes (PeLEDs) with a peak luminance of 6600 cd m −2 and a current efficiency of 7.0 cd A −1 . We use this strategy to upscale PeLEDs to large-area substrates (230 cm 2 ) by developing a protocol for slot-die coating combined with gas-quenching. The resulting large area devices (9 device…

Thickness scaling of space-charge-limited currents in organic layers with field- or density-dependent mobility

An exact solution is provided for the current density-voltage (J –V) characteristics of space-charge limited transport of a single carrier in organic layers with field-dependent mobility of the type μ (E) = μ0 exp (γ √E. The general scaling relationship for field-dependent mobility occurs in terms of the variables JL and V /L. For the density-dependence of the mobility found in organic field-effect transistor measurements, the thickness scaling occurs in terms of different variables, J1/βL and V /L. The proposed scaling is a useful test for distinguishing field- and carrier density-dependent mobility in disordered organic semiconductors. (© 2006 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

Aqueous electrolyte-gated ZnO transistors for environmental and biological sensing

Electrolyte-gated transistors (EGTs) based on ZnO thin films, obtained by solution processing of suspensions of nanoparticles, have a low turn-on voltage (<0.5 V), a high on/off ratio and transconductance exceeding 0.2 mS. Importantly, the ZnO surface can be functionalized with a large variety of molecular recognition elements, making these devices ideal transducers in physiological and environmental monitoring. We present simple glucose-sensing and ion-selective EGTs, demonstrating the versatility of such devices in biosensing.

Subphthalocyanines as narrow band red-light emitting materials

A series of new light emitting subphthalocyanines, lower homologues of phthalocyanines, were synthesized having color points covering the red-orange region of the visible spectrum. Additionally, they were found to be of potential use as narrow band emitters for red-light emitting diodes.

Lithium salt additives and the influence of their counterion on the performances of light-emitting electrochemical cells

In this work we study the effect of the addition of lithium salts to light-emitting electrochemical cells (LECs), and in particular the effect of the lithium counterion. We found that the chosen lithium salts can substantially improve the device turn-on time as well as the overall lifetime, with respect to reference LECs using the pure emitter. A correlation between the lithium counterion and the corresponding device performance is established, and efficient LECs with lifetimes approaching 2000 hours are presented.

Room-Temperature Cubic Phase Crystallization and High Stability of Vacuum-Deposited Methylammonium Lead Triiodide Thin Films for High-Efficiency Solar Cells

Methylammonium lead triiodide (MAPI) has emerged as a high-performance photovoltaic material. Common understanding is that at room temperature it adopts a tetragonal phase and it only converts to the perfect cubic phase around 50-60 ºC. Most MAPI films are prepared using a solution-based coating process, yet they can also be obtained by vapor phase deposition methods. Vapor phase processed MAPI films have significantly different characteristics compared to their solvent processed analogous, such as a relatively small crystal grain sizes and short excited state lifetimes. Yet solar cells based on vapor phase processed MAPI films exhibit high power conversion efficiencies. Surprisingly, after…

Optimization of Polymer Blue-Light-Emitting Devices by Introducing a Hole-Injection Layer Doped with the Molecular Nanomagnet [Mn12O12(H2O)4(C6F5COO)16]

Flexible light-emitting electrochemical cells with single-walled carbon nanotube anodes

Abstract In this work, we demonstrate flexible solution processed light emitting electrochemical cells (LECs) which use single-walled carbon nanotubes (SWCNTs) films as the substrate. The SWCNTs were synthesized by an integrated aerosol method and dry-transferred on the plastic substrates at room temperature. The addition of a screen printed poly (3,4-ethylene dioxythiophene) doped with poly (styrene sulfonate) (PEDOT:PSS) film onto the nanostructured electrode further homogenizes the surface and enlarges the work function, enhancing the hole injection into the active layer. By using an efficient phosphorescent ionic transition metal complex (iTMC) as the active material, efficacies up to 9…

Luminescent osmium(II) bi-1,2,3-triazol-4-yl complexes: photophysical characterisation and application in light-emitting electrochemical cells

The series of osmium(II) complexes [Os(bpy)3-n(btz)n][PF6]2 (bpy = 2,2’-bipyridyl, btz = 1,1’-dibenzyl-4,4’-bi-1,2,3-triazolyl, 1 n = 0, 2 n = 1, 3 n = 2, 4 n = 3), have been prepared and characterised. The progressive replacement of bpy by btz leads to blue-shifted UV-visible electronic absorption spectra, indicative of btz perturbation of the successively destabilised bpy-centred LUMO. For 4, a dramatic blue-shift relative to the absorption profile for 3 is observed, indicative of the much higher energy LUMO of the btz ligand over that of bpy, mirroring previously reported data on analogous ruthenium(II) complexes. Unlike the previously reported ruthenium systems, heteroleptic complexes 2…

Tunable Wide‐Bandgap Monohalide Perovskites

Herein the mechanochemical synthesis of inorganic as well as hybrid organic-inorganic monohalide perovskites with tunable bandgaps is reported. It is shown that the bandgap bowing known for iodide mixed Sn-Pb perovskites is also present in the pure bromide analogous. This results in technologically very interesting materials with bandgaps in the range of 1.7-1.9 eV. Similar bandgap perovskites are typically achieved by mixing two halides that are prone to segregate over time. This limits the achievable open circuit voltage. For monohalide perovskites this problem is eliminated, making these materials especially promising wide bandgap absorbers for tandem solar cells. Perovskite Thin-film Ph…

Crystal Reorientation and Amorphization Induced by Stressing Efficient and Stable P–I–N Vacuum‐Processed MAPbI 3 Perovskite Solar Cells

Herein, the long-term stability of vacuum-deposited methylammonium lead iodide (MAPbI(3)) perovskite solar cells (PSCs) with power conversion efficiencies (PCEs) of around 19% is evaluated. A low-temperature atomic layer deposition (ALD) Al2O3 coating is developed and used to protect the MAPbI(3) layers and the solar cells from environmental agents. The ALD encapsulation enables the MAPbI(3) to be exposed to temperatures as high as 150 degrees C for several hours without change in color. It also improves the thermal stability of the solar cells, which maintain 80% of the initial PCEs after aging for approximate to 40 and 37days at 65 and 85 degrees C, respectively. However, room-temperature…

[Ir(C^N)2(N^N)]+ emitters containing a naphthalene unit within a linker between the two cyclometallating ligands

The synthesis of four cyclometallated [Ir(C^N) 2 (N^N)][PF 6 ] compounds in which N^N is a substituted 2,2’- -bipyridine (bpy) ligand and the naphthyl-centred ligand 2,7-bis(2-(2-(4-(pyridin-2-yl)phenoxy)ethoxy) ethoxy)naphthalene provides the two cyclometallating C^N units is reported. The iridium( III ) complexes have been characterized by 1 H and 13 C NMR spectroscopies, mass spectrometry and elemental analysis, and their electrochemical and photophysical properties are described. Comparisons are made with a model [Ir(ppy) 2 (N^N)][PF 6 ] compound (Hppy = 2-phenylpyridine). The complexes containing the naphthyl-unit exhibit similar absorption spectra and excitation at 280 nm leads to an …

Charge Noise in Organic Electrochemical Transistors

Organic electrochemical transistors (OECTs) are increasingly studied as transducers in sensing applications. While much emphasis has been placed on analyzing and maximizing the OECT signal, noise has been mostly ignored, although it determines the resolution of the sensor. The major contribution to the noise in sensing devices is the 1/f noise, dominant at low frequency. In this work, we demonstrate that the 1/f noise in OECTs follows a charge-noise model, which reveals that the noise is due to charge fuctuations in proximity or within the bulk of the channel material. We present the noise scaling behavior with gate voltage, channel dimensions and polymer thickness. Our results suggest the …

Removing Leakage and Surface Recombination in Planar Perovskite Solar Cells

Thin-film solar cells suffer from various types of recombination, of which leakage current usually dominates at lower voltages. Herein, we demonstrate first a three-order reduction of the shunt loss mechanism in planar methylammonium lead iodide perovskite solar cells by replacing the commonly used hole transport layer poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) with a better hole-selective polyarylamine. As a result, these cells exhibit superior operation under reduced light conditions, which we demonstrate for the extreme case of moonlight irradiance, at which open-circuit voltages of 530 mV can still be obtained. By the shunt removal we also observe the VOC to dro…

Operational Mechanism of Conjugated Polyelectrolytes

Conjugated polyelectrolytes (CPEs) are versatile materials used in a range of organic optoelectronic applications. Because of their ionic/electronic nature, characterizing these materials is nontrivial, and their operational mechanism is not fully understood. In this work we use a methodology that combines constant-voltage-driven current-density transient measurements with fast current vs voltage scans to allow decoupling of ionic and electronic phenomena. This technique is applied to diodes prepared with cationic CPEs having different charge-compensating anions. Our results indicate that the operational mechanism of these devices is governed by electrochemical doping of the CPE. On the bas…

Comprehensive defect suppression in perovskite nanocrystals for high-efficiency light-emitting diodes

Electroluminescence efficiencies of metal halide perovskite nanocrystals (PNCs) are limited by a lack of material strategies that can both suppress the formation of defects and enhance the charge carrier confinement. Here we report a one-dopant alloying strategy that generates smaller, monodisperse colloidal particles (confining electrons and holes, and boosting radiative recombination) with fewer surface defects (reducing non-radiative recombination). Doping of guanidinium into formamidinium lead bromide PNCs yields limited bulk solubility while creating an entropy-stabilized phase in the PNCs and leading to smaller PNCs with more carrier confinement. The extra guanidinium segregates to th…

Efficient and Long-Living Light-Emitting Electrochemical Cells

Three new heteroleptic iridium complexes that combine two approaches, one leading to a high stability and the other yielding a high luminescence efficiency, are presented. All complexes contain a phenyl group at the 6-position of the neutral bpy ligand, which holds an additional, increasingly bulky substituent on the 4-position. The phenyl group allows for intramolecular π–π stacking, which renders the complex more stable and yields long-living light-emitting electrochemical cells (LECs). The additional substituent increases the intersite distance between the cations in the film, reducing the quenching of the excitons, and should improve the efficiency of the LECs. Density functional theory…

A Supramolecularly-Caged Ionic Iridium(III) Complex Yielding Bright and Very Stable Solid-State Light-Emitting Electrochemical Cells

A new iridium(III) complex showing intramolecular interligand pi-stacking has been synthesized and used to improve the stability of single-component, solid-state light-emitting electrochemical cell (LEC) devices. The pi-stacking results in the formation of a very stable supramolecularly caged complex. LECs using this complex show extraordinary stabilities (estimated lifetime of 600 h) and luminance values (average luminance of 230 cd m-2) indicating the path toward stable ionic complexes for use in LECs reaching stabilities required for practical applications.

Perimeter leakage current in polymer light emitting diodes

Observation of leakage current paths through the device perimeter in standard poly(phenylene vinylene)-based light-emitting devices is reported. Perimeter leakage currents govern the diode performance in reverse and low positive bias and exhibit an ohmic character. Current density correlates with the perimeter-to-area ratio thus indicating that leakage currents are mainly confined on polymer regions in the vicinity of metallic contact limits (device perimeter). © 2008 Elsevier B.V. All rights reserved.

Remote Modification of Bidentate Phosphane Ligands Controlling the Photonic Properties in Their Complexes: Enhanced Performance of [Cu(RN‐xantphos)(N ^ N)][PF 6 ] in Light‐Emitting Electrochemical Cells

A series of copper(I) complexes of the type [Cu(HN-xantphos)(N^N)][PF6] and [Cu(BnN-xantphos)(N^N)][PF6], in which N^N = bpy, Mebpy and Me2bpy, HN-xantphos = 4,6-bis(diphenylphosphanyl)-10H-phenoxazine and BnN-xantphos = 10-benzyl-4,6-bis(diphenylphosphanyl)-10H-phenoxazine is described. The single crystal structures of [Cu(HN-xantphos)(Mebpy)][PF6] and [Cu(BnN-xantphos)(Me2bpy)][PF6] confirm the presence of N^N and P^P chelating ligands with the copper(I) atoms in distorted coordination environments. Solution electrochemical and photophysical properties of the BnN-xantphos-containing compounds (for which the highest-occupied molecular orbital is located on the phenoxazine moiety) are repor…

Ion-Selective Organic Electrochemical Transistors

Ion-selective organic electrochemical transistors with sensitivity to potassium approaching 50 μA dec(-1) are demonstrated. The remarkable sensitivity arises from the use of high transconductance devices, where the conducting polymer is in direct contact with a reference gel electrolyte and integrated with an ion-selective membrane.

Ionically Assisted Charge Injection in Hybrid Organic−Inorganic Light-Emitting Diodes

We have developed hybrid organic−inorganic light-emitting diodes (HyLEDs) featuring a buffer layer of a conjugated polyelectrolyte (CPE) sandwiched between a light emitting polymer (LEP) film and a ZnO electron injection layer. Efficacies exceeding 5 cd/A and the possibility of employing various LEPs are demonstrated. These improvements, compared to HyLEDs without any interlayer, are attributed to the redistribution of ions in the CPE film, causing hole accumulation at the CPE/LEP interfaces and enhanced electron injection from the ZnO into the electroluminescent polymer. The intrinsic air-stability of the electrodes used in HyLEDs, together with the solution processability of the ZnO/CPE/L…

Determination of charge carrier mobility of hole transporting polytriarylamine-based diodes

Hole transport properties of three different side chain poly(triarylamines) have been determined by means of the analysis of steady-state current-voltage characteristics using co-planar diode structures. The interpretation is based on space-charge limited models with field-dependent mobility. Mobilities between ~ 10- 8 and 10- 6 cm2 V- 1 s- 1 are obtained. The highest mobility is achieved for poly(tetraphenylbenzidine) devices and the lowest for poly(triphenylamine) devices. Electron-rich methoxy substituents increase the mobility of poly(triphenylamine)s. A comparison of the mobility values with those obtained using organic field-effect transistors is also given. © 2009 Elsevier B.V. All r…

Operating Modes of Sandwiched Light-Emitting Electrochemical Cells

Light-emitting electrochemical cells (LECs) are promising lighting devices in which the redistribution of ionic charges allows for double electronic carrier injection from air-stable electrodes. Uncertainties about the mode of operation are limiting the progress of these devices. Using fast (with respect to the current growth time) but resolutive electrical measurement techniques, the electronic transport mechanism in state-of-the-art sandwiched devices can be monitored as a function of the operation time. The results indicate the formation of doped transport layers adjacent to the electrodes that reduces the extent of the central neutral light-emitting layer where electronic transport is l…

Modulation of the solubility of luminescent semiconductor nanocrystals through facile surface functionalization

The solubility of luminescent quantum dots in solvents from hexane to water can be finely tuned by the choice of the countercations associated with carboxylate residues present on the nanocrystal surface. The resulting nanocrystals exhibit long term colloidal and chemical stability and maintain their photophysical properties.

High voltage vacuum-processed perovskite solar cells with organic semiconducting interlayers

In perovskite solar cells, the choice of appropriate transport layers and electrodes is of great importance to guarantee efficient charge transport and collection, minimizing recombination losses. The possibility to sequentially process multiple layers by vacuum methods offers a tool to explore the effects of different materials and their combinations on the performance of optoelectronic devices. In this work, the effect of introducing interlayers and altering the electrode work function has been evaluated in fully vacuum-deposited perovskite solar cells. We compared the performance of solar cells employing common electron buffer layers such as bathocuproine (BCP), with other injection mate…

Solution processed organic light-emitting diodes using a triazatruxene crosslinkable hole transporting material.

A cross-linkable triazatruxene that leads to insoluble films upon thermal annealing at temperatures compatible with flexible substrates is presented. The films were used as the hole transporting and electron blocking layer in partially solution processed phosphorescent organic light-emitting diodes, reaching power conversion efficiencies of 24 lm W−1, an almost 50% improvement compared to the same OLEDs without the cross-linkable hole transporting layer.

Applications of vacuum vapor deposition for perovskite solar cells: A progress review

Metal halide perovskite solar cells (PSCs) have made substantial progress in power conversion efficiency (PCE) and stability in the past decade thanks to the advancements in perovskite deposition methodology, charge transport layer (CTL) optimization, and encapsulation technology. Solution-based methods have been intensively investigated and a 25.7% certified efficiency has been achieved. Vacuum vapor deposition protocols were less studied, but have nevertheless received increasing attention from industry and academia due to the great potential for large-area module fabrication, facile integration with tandem solar cell architectures, and compatibility with industrial manufacturing approach…

Vacuum-Deposited Cesium Tin Iodide Thin Films with Tunable Thermoelectric Properties

Most current thermoelectric materials have important drawbacks, such as toxicity, scarceness, and peak operating temperatures above 300 °C. Herein, we report the thermoelectric properties of different crystalline phases of Sn-based perovskite thin films. The 2D phase, Cs2SnI4, is obtained through vacuum thermal deposition and easily converted into the black β phase of CsSnI3(B-β CsSnI3) by annealing at 150 °C. B-β CsSnI3is a p-type semiconductor with a figure of merit (ZT) ranging from 0.021 to 0.033 for temperatures below 100 °C, which makes it a promising candidate to power small electronic devices such as wearable sensors which may be interconnected in the so-called Internet of Things. T…

Dynamically Doped White Light Emitting Tandem Devices

Solution-processed, salt-containing, blue and orange light-emitting layers lead to efficient white light-emitting devices when arranged in a tandem configuration separated by a thin metal layer.

Preface to Special Issue of ChemSusChem on Perovskite Optoelectronics

This Editorial introduces one of two companion Special Issues on "Halide Perovskites for Optoelectronics Applications" in ChemSusChem and Energy Technology following the ICMAT 2017 Conference in Singapore. More information on the other Special Issue can be found in the Editorial published in Energy Technology.

Regioisomerism in cationic sulfonyl-substituted [Ir(C^N)2(N^N)]+ complexes: its influence on photophysical properties and LEC performance

A series of regioisomeric cationic iridium complexes of the type [Ir(C^N)2(bpy)][PF6] (bpy = 2,2'-bipyridine) is reported. The complexes contain 2-phenylpyridine-based cyclometallating ligands with a methylsulfonyl group in either the 3-, 4- or 5-position of the phenyl ring. All the complexes have been fully characterized, including their crystal structures. In acetonitrile solution, all the compounds are green emitters with emission maxima between 493 and 517 nm. Whereas substitution meta to the Ir-C bond leads to vibrationally structured emission profiles and photoluminescence quantum yields of 74 and 77%, placing a sulfone substituent in a para position results in a broad, featureless em…

Impedance of space-charge-limited currents in organic light-emitting diodes with double injection and strong recombination

The impedance model for a one-carrier space-charge-limited (SCL) current has been applied to explain some experimental features of double carrier organic light-emitting diodes. We report the analytical model of impedance of bipolar drift transport in SCL regime in the limit of infinite recombination. In this limit the ac impedance function is identical to that of a single carrier device, with a transit time modified by the sum of mobilities for electrons and holes, μn+μp. The static capacitance C(ω→0) is a factor of ¾ lower than the geometric capacitance, as observed for single carrier devices, but it is shifted to higher frequencies. It follows that impedance measurements in the dual-carri…

Stable Light-Emitting Electrochemical Cells Using Hyperbranched Polymer Electrolyte

The choice of an adequate electrolyte is a fundamental aspect in polymer light-emitting electrochemical cells (PLECs) as it provides the in situ electrochemical doping and influences the performance of these devices. In this study, a hyperbranched polymer (Hybrane DEO750 8500) blended with a Li salt is used as a novel electrolyte in state-of-the-art Super Yellow (a polyphenylenevinylene) based LECs. Due to the desirable properties of the hyperbranched polymer and the homogeneous and smooth films that it forms with the emitting polymer, PLEC with excellent electroluminescent properties are obtained using a pulsed current bias scheme. The devices are very stable, with lifetimes in excess of 2…

Dynamic doping in planar ionic transition metal complex-based light-emitting electrochemical cells

Using a planar electrode geometry, the operational mechanism of iridium(III) ionic transition metal complex (iTMC)-based light-emitting electrochemical cells (LECs) is studied by a combination of fluorescence miscroscopy and scanning Kelvin probe microscopy (SKPM). Applying a bias to the LECs leads to the quenching of the photoluminescence (PL) in between the electrodes and to a sharp drop of the electrostatic potential in the middle of the device, far away from the contacts. The results shed light on the operational mechanism of iTMC-LECs and demonstrate that these devices work essentially the same as LECs based on conjugated polymers do, i.e., according to an electrochemical doping mechan…

Vacuum Deposited Triple-Cation Mixed-Halide Perovskite Solar Cells

Hybrid lead halide perovskites are promising materials for future photovoltaics applications. Their spectral response can be readily tuned by controlling the halide composition, while their stability is strongly dependent on the film morphology and on the type of organic cation used. Mixed cation and mixed halide systems have led to the most efficient and stable perovskite solar cells reported, so far they are prepared exclusively by solution-processing. This might be due to the technical difficulties associated with the vacuum deposition from multiple thermal sources, requiring a high level of control over the deposition rate of each precursor during the film formation. In this report, the…

Persistent photovoltage in methylammonium lead iodide perovskite solar cells

Open circuit voltage decay measurements are performed on methylammonium lead iodide (CH3NH3PbI3) perovskite solar cells to investigate the charge carrier recombination dynamics. The measurements are compared to the two reference polymer-fullerene bulk heterojunction solar cells based on P3HT:PC60BM and PTB7:PC70BM blends. In the perovskite devices, two very different time domains of the voltage decay are found, with a first drop on a short time scale that is similar to the organic solar cells. However, two major differences are also observed. 65-70% of the maximum photovoltage persists on much longer timescales, and the recombination dynamics are dependent on the illumination intensity.

Nontemplate Synthesis of CH3NH3PbBr3 Perovskite Nanoparticles

To date, there is no example in the literature of free, nanometer-sized, organolead halide CH3NH3PbBr3 perovskites. We report here the preparation of 6 nm-sized nanoparticles of this type by a simple and fast method based on the use of an ammonium bromide with a medium-sized chain that keeps the nanoparticles dispersed in a wide range of organic solvents. These nanoparticles can be maintained stable in the solid state as well as in concentrated solutions for more than three months, without requiring a mesoporous material. This makes it possible to prepare homogeneous thin films of these nanoparticles by spin-coating on a quartz substrate. Both the colloidal solution and the thin film emit l…

The shiny side of copper: bringing copper(i) light-emitting electrochemical cells closer to application

Heteroleptic [Cu(P^P)(N^N)][PF6] complexes, where N^N is 5,50-dimethyl-2,20-bipyridine (5,50-Me2bpy), 4,5,6-trimethyl-2,20-bipyridine (4,5,6-Me3bpy), 6-(tert-butyl)-2,20-bipyridine (6-tBubpy) and 2-ethyl-1,10- phenanthroline (2-Etphen) and P^P is either bis(2-(diphenylphosphino)phenyl)ether (POP, PIN [oxydi(2,1- phenylene)]bis(diphenylphosphane)) or 4,5-bis(diphenylphosphino)-9,9-dimethylxanthene (xantphos, PIN (9,9-dimethyl-9H-xanthene-4,5-diyl)bis(diphenylphosphane)) have been synthesized and their NMR spectroscopic, mass spectrometric, structural, electrochemical and photophysical properties were investigated. The single-crystal structures of [Cu(POP)(5,50-Me2bpy)][PF6], [Cu(xantphos)(5,…

Coating Evaporated MAPI Thin Films with Organic Molecules: Improved Stability at High Temperature and Implementation in High-Efficiency Solar Cells

Methylammonium lead iodide (MAPI) has proven to be an exceptional light-absorber for single-junction thin-film solar cells. Nonetheless, degradation induced by environmental agents (air, moisture, heat) limits the stability of this hybrid perovskite. Here, we demonstrate that coating evaporated MAPI thin films with different hydrophobic molecules leads to a significant improvement in their stability. We especially investigated the degradation of MAPI and the subsequent formation of PbI2 at 150 °C by in situ XRD analysis and showed that this transformation is remarkably slowed down in films coated with trioctyl phosphine oxide and tridodecyl methylammonium iodide. This enhances the processab…

Lumineszierende ionische Übergangsmetallkomplexe für leuchtende elektrochemische Zellen

Durch die Umsetzung neuer Beleuchtungskonzepte konnte die Verwertung von Energie deutlich effizienter gestaltet werden. Alle derzeit entwickelten Technologien beruhen auf elektrolumineszierenden Festkorpern und lassen sich allgemein als Festkorperbeleuchtung (solid-state lighting, SSL) einstufen. Die beiden wichtigsten Zweige der SSL-Technologie sind Leuchtdioden (LEDs) und organische Leuchtdioden (OLEDs), doch seit kurzem bilden auch leuchtende elektrochemische Zellen (LECs) eine Alternative, die als aktive Materialien entweder lumineszierende Polymere in Kombination mit ionischen Salzen oder lumineszierende ionische Spezies wie ionische Ubergangsmetallkomplexe (iTMCs) enthalten. Cyclometa…

Band unpinning and photovoltaic model for P3HT:PCBM organic bulk heterojunctions under illumination

Capacitance analysis of P3HT:PCBM bulk heterojunction solar cells, in dark and under illumination, shows a linear Mott-Schottky characteristic at moderate reverse bias, indicating p-doping of the organic blend. The flatband potential under illumination is displaced negatively about 0.6 V with respect to dark conditions. A basic photovoltaic model is developed to explain this, in terms of electron transfer via surface states at the metal/organic interface. Surface states with a slow exchange kinetics, become charged under illumination, unpinning the band and decreasing the depletion layer at the electron extraction contact. This becomes a major factor limiting the performance of bulk heteroj…

Radiative efficiency of lead iodide based perovskite solar cells

The maximum efficiency of any solar cell can be evaluated in terms of its corresponding ability to emit light. We herein determine the important figure of merit of radiative efficiency for Methylammonium Lead Iodide perovskite solar cells and, to put in context, relate it to an organic photovoltaic (OPV) model device. We evaluate the reciprocity relation between electroluminescence and photovoltaic quantum efficiency and conclude that the emission from the perovskite devices is dominated by a sharp band-to-band transition that has a radiative efficiency much higher than that of an average OPV device. As a consequence, the perovskite have the benefit of retaining an open circuit voltage ~0.1…

White-light phosphorescence emission from a single molecule: application to OLED.

A simple mononuclear cyclometallated iridium(III) complex exhibits white photo- and electro- luminescence in the wavelength range from 440 to 800 nm, which originates from a single emitting excited state of mixed character. Bolink Henk, Henk.Bolink@uv.es ; Coronado Miralles, Eugenio, Eugenio.Coronado@uv.es

Boosting inverted perovskite solar cell performance by using 9,9-bis(4-diphenylaminophenyl)fluorene functionalized with triphenylamine as a dopant-free hole transporting material

In this study, two newly developed small molecules based on 9,9-bis(4-diphenylaminophenyl)fluorene functionalized with triphenylamine moieties, namely TPA-2,7-FLTPA-TPA and TPA-3,6-FLTPA-TPA, are designed, synthesized and characterized. The electrochemical, optical and thermal properties of both materials are investigated using various techniques. Afterwards, these materials are employed as dopant-free hole transporting materials (HTMs) in planar inverted perovskite solar cell devices with the aim of determining the device performance and studying their stability in comparison with reference N4,N4,N4′′,N4′′-tetra([1,10-biphenyl]-4-yl)-[1,1′:4′,1′′-terphenyl]-4,4′′-diamine (TaTm)-based devic…

Photoluminescence quantum yield exceeding 80% in low dimensional perovskite thin-films via passivation control

Quasi-2D perovskites with the BA : MA molar ratio equal to 3 : 3 show a remarkable PLQY exceeding 80%, thanks to the use of an electron donor as the passivating agent. These films have been applied in LEDs that exhibit high brightness exceeding 1000 cd m−2 and current efficiencies >3 cd A−1.

Perovskites and Beyond: Dry Mechanochemical Synthesis of Multinary Metal Halides

Mechanochemical Synthesis of Sn(II) and Sn(IV) Iodide Perovskites and Study of Their Structural, Chemical, Thermal, Optical and Electrical Properties

Phase‐pure CsSnI3, FASnI3, Cs(PbSn)I3, FA(PbSn)I3 perovskites (FA = formamidinium = HC(NH2)2+) as well as the analogous so‐called vacancy‐ordered double perovskites Cs2SnI6 and FA2SnI6 are mechanochemically synthesized. The addition of SnF2 is found to be crucial for the synthesis of Cs‐containing perovskites but unnecessary for hybrid ones. All compounds show an absorption onset in the near‐infrared (NIR) region, which makes them especially relevant for photovoltaic applications. The addition of Pb(II) and SnF2 is crucial to improve the electronic properties in 3D Sn(II)‐based perovskites, in particular their charge carriers mobility (≈0.2 cm2 Vs−1) which is enhanced upon reduction of the …

Intrinsic Organic Semiconductors as Hole Transport Layers in p–i–n Perovskite Solar Cells

Thin polymeric and small-molecular-weight organic semiconductors are widely employed as hole transport layers (HTLs) in perovskite solar cells. To ensure ohmic contact with the electrodes, the use of doping or additional high work function (WF) interlayer is common. In some cases, however, intrinsic organic semiconductors can be used without any additive or buffer layers, although their thickness must be tuned to ensure selective and ohmic hole transport. Herein, the characteristics of thin HTLs in vacuum-deposited perovskite solar cells are studied, and it is found that only very thin (&lt;5 nm) HTLs readily result inhigh-performing devices, as the HTL acts as a WF enhancer while still ens…

Highly phosphorescent perfect green emitting iridium(iii) complex for application in OLEDs.

A novel iridium complex, [bis-(2-phenylpyridine)(2-carboxy-4-dimethylaminopyridine)iridium(III)] (N984), was synthesized and characterized using spectroscopic and electrochemical methods; a solution processable OLED device incorporating the N984 complex displays electroluminescence spectra with a narrow bandwidth of 70 nm at half of its intensity, with colour coordinates of x = 0.322; y = 0.529 that are very close to those suggested by the PAL standard for a green emitter. Bolink, Henk, Henk.Bolink@uv.es ; Coronado Miralles, Eugenio, Eugenio.Coronado@uv.es ; Garcia Santamaria, Sonsoles Amor, Sonsoles.Garcia@uv.es

Working mechanisms of vacuum-deposited perovskite solar cells

SiPMs coated with TPB: coating protocol and characterization for NEXT

[EN] Silicon photomultipliers (SiPM) are the photon detectors chosen for the tracking readout in NEXT, a neutrinoless \bb decay experiment which uses a high pressure gaseous xenon time projection chamber (TPC). The reconstruction of event track and topology in this gaseous detector is a key handle for background rejection. Among the commercially available sensors that can be used for tracking, SiPMs offer important advantages, mainly high gain, ruggedness, cost-effectiveness and radio-purity. Their main drawback, however, is their non sensitivity in the emission spectrum of the xenon scintillation (peak at 175 nm). This is overcome by coating these sensors with the organic wavelength shifte…

Iridium(III) Complexes with Phenyl-tetrazoles as Cyclometalating Ligands

Ir(II) cationic complexes with cyclometalating tetrazolate ligands were prepared for the first time, following a two-step strategy based on (i) a silver-assisted cyclometalation reaction of a tetrazole derivative with IrCl3 affording a bis-cyclometalated solvato-complex P ([Ir(ptrz)(2)(CH3CN)(2)](+), Hptrz = 2-methyl-5-phenyl-2H-tetrazole); (ii) a substitution reaction with five neutral ancillary ligands to get [Ir(ptrz)(2)L](+), with L = 2,2'-bypiridine (1), 4,4'-di-tert-butyl-2,2'-bipyridine (2), 1,10-phenanthroline (3), and 2-(1-phenyl-1H-1,2,3-triazol-4-yl)pyridine (4), and [Ir(ptrz)(2)L-2](+), with L = tertbutyl isocyanide (5). X-ray crystal structures of P, 2, and 3 were solved. Elect…

Wafer-scale pulsed laser deposition of ITO for solar cells: reduced damage vs. interfacial resistance

Transparent conducting oxides (TCOs) used in solar cells must be optimized to achieve minimum parasitic absorption losses while providing sufficient lateral conductivity. Low contact resistance with the adjacent device layers and low damage to the substrate during deposition of the TCO are also important requirements to ensure high solar cell efficiencies. Pulsed laser deposition (PLD) has been proposed as an alternative low-damage TCO deposition technique on top of sensitive layers and interfaces in organic and perovskite solar cells but is yet to be studied for the more mature silicon technology. Focusing on the PLD deposition pressure as the key parameter to reduce damage, we developed t…

Colour tuning by the ring roundabout: [Ir(C^N)2(N^N)]+ emitters with sulfonyl-substituted cyclometallating ligands

A series of cationic bis-cyclometallated iridium(III) complexes [Ir(C^N)2(N^N)]+ is reported. Cyclometallating C^N ligands are based on 2-phenylpyridine with electron-withdrawing sulfone substituents in the phenyl ring: 2-(4-methylsulfonylphenyl)pyridine (H1) and 2-(3-methylsulfonylphenyl)pyridine (H2). 2-(1H-Pyrazol-1-yl)pyridine (pzpy) and 2-(3,5-dimethyl-1H-pyrazol-1-yl)pyridine (dmpzpy) are used as electron-rich ancillary N^N ligands. The complexes have been fully characterized and the single crystal structure of [Ir(2)2(dmpzpy)][PF6]·MeCN has been determined. Depending on the position of the methylsulfonyl group, the complexes are green or blue emitters with vibrationally structured em…

Efficient orange light-emitting electrochemical cells

We report the first bis-cyclometalated cationic iridium(III) complex with N-aryl-substituted 1H-imidazo [4,5-f][1,10]phenanthroline. The complex emits yellow-orange phosphorescence with a maximum at 583 nm, a quantum yield of 43%, and an excited-state lifetime of 910 ns in argon-saturated dichloromethane. Optimized orange light-emitting electrochemical cells with the new Ir(III) complex exhibit fast turn-on, a peak luminance of 684 cd m(-2) and a peak efficacy of 6.5 cd A(-1); in 850 h of continuous operation their luminance and efficacy decrease only by 20%.

Efficient and Thermally Stable Wide Bandgap Perovskite Solar Cells by Dual‐Source Vacuum Deposition

Transparent Light‐Emitting Electrochemical Cells

Single layer light-emitting electrochemical cells (LECs) are amongst the simplest electroluminescent devices and operate with air-stable electrodes. Transparent light-emitting devices are of great interest as they can enable new applications in consumer electronics. In this work, a transparent ionic transition metal complex based LEC is fabricated by developing a transparent top contact based on tin (IV) oxide (SnO2) and indium-tin oxide, processed by low-temperature atomic layer deposition and pulsed laser deposition, respectively. The resulting devices present transparency in excess of 75% over the full visible spectrum (380-750 nm), with 82% transmission at the emission peak (563 nm). Th…

Molecular Passivation of MoO3: Band Alignment and Protection of Charge Transport Layers in Vacuum-Deposited Perovskite Solar Cells

Vacuum-deposition of perovskite solar cells can achieve efficiencies rivalling solution-based methods and it allows for more complex device stacks. MoO3 has been used to enhance carrier extraction to the transparent bottom electrode in a p-i-n configuration, here we show that by inserting an organic charge transport molecule it can also be used on the top of a perovskite absorber in a n-i-p configuration. This strategy enables the first vacuum-deposited perovskite solar cells with metal oxides as charge transporting layers for both electrons and holes leading to power conversion efficiency > 19 %.

Deep-Red-Emitting Electrochemical Cells Based on Heteroleptic Bis-chelated Ruthenium(II) Complexes

Two ruthenium(II)-based complexes were prepared that show intense deep-red light emission at room temperature. Solid-state electroluminescent devices were prepared using one of the ruthenium complexes as the only active component. These devices emit deep-red light at low voltages and exhibit extraordinary stabilities, demonstrating their potential for low-cost deep-red light sources.

Long-Lived Luminescence and Slow Carrier Diffusion in Metal Halide Perovskites as a result of Multiple Trapping and De-Trapping by Shallow Non-Quenching Traps

Dipole reorientation and local density of optical states influence the emission of light-emittingelectrochemical cells

Herein, we analyze the temporal evolution of the electroluminescence of light-emitting electrochemicalcells (LECs), a thin-film light-emitting device, in order to maximize the luminous power radiated bythese devices. A careful analysis of the spectral and angular distribution of the emission of LECsfabricated under the same experimental conditions allows describing the dynamics of the spatial regionfrom which LECs emit,i.e.the generation zone, as bias is applied. This effect is mediated by dipolereorientation within such an emissive region and its optical environment, since its spatial drift yields adifferent interplay between the intrinsic emission of the emitters and the local density of …

Efficient, 23%, Solution-Processed Perovskite Tandem Cells

In this issue of Joule, Palmstrom and coworkers present efficient solution-processed two-terminal solar cells employing two metal halide perovskite-based absorbers. The key to this achievement is 2-fold: the deposition of a thin yet robust transparent conductor in between the two sub-cells allows solution processing of the back-cell and enables efficient and local charge recombination. Furthermore, the insertion of large cations reduces halide segregation and enables a higher open-circuit voltage and stability for the high-band-gap sub-cell.

Extended liquid-crystalline oligofluorenes with photo- and electroluminescence

In this paper we report the synthesis and characterization of a series of low-molecular weight light-emitting molecules based on short oligofluorene cores, from one to three 9,9-dioctylfluorene units, elongated at the 2- and 7-positions by means of promesogenic units. The effect of this structural modification on the mesomorphic properties, as well as on the optical and electrochemical properties, is studied. The possibility of using these molecules as emitters in light-emitting diodes (LEDs) and polarized photoluminescent layers has been explored.

Improved stability of solid state light emitting electrochemical cells consisting of ruthenium and iridium complexes

ABSTRACTTwo charged organometallic complexes containing bulky hydrophobic ligands based on ruthenium (II) and iridium (III) were synthesized and their performance in solid state light emitting electrochemical cells is described. The complexes were chosen as due to their large ligands a diminished susceptibility towards the formation of destructive complexes during device operation is expected. The LEC device performances reveal the longest living devices reported so far under dc bias. Quantum chemical calculations confirm that the major effect of the bulky diphenylphenanthroline ligands is of steric origin and not related with changes in the molecular electronic structure of the complexes.

Sputtered transparent electrodes for optoelectronic devices

Summary Transparent electrodes and metal contacts deposited by magnetron sputtering find applications in numerous state-of-the-art optoelectronic devices, such as solar cells and light-emitting diodes. However, the deposition of such thin films may damage underlying sensitive device layers due to plasma emission and particle impact. Inserting a buffer layer to shield against such damage is a common mitigation approach. We start this review by describing how sputtered transparent top electrodes have become archetypal for a broad range of optoelectronic devices and then discuss the possible detrimental consequences of sputter damage on device performance. Next, we review common buffer-layer m…

Light-emitting electrochemical cells based on a supramolecularly-caged phenanthroline-based iridium complex.

The complex [Ir(ppy)(2)(pphen)][PF(6)] (Hppy = 2-phenylpyridine, pphen = 2-phenyl-1,10-phenanthroline) has been prepared and evaluated as an electroluminescent component for light-emitting electrochemical cells (LECs). Like in analogous LECs using bpy-based iridium(III) complexes a significant enhancement of the device stability is observed.

Highly Photoluminescent Blue Ionic Platinum-Based Emitters

New cycloplatinated N-heterocyclic carbene (NHC) compounds with chelate diphosphines (P^P) as ancillary ligands: [Pt(R-C^C*)(P^P)]PF6 (R = H, P^P = dppm (1A), dppe (2A), dppbz (3A); R = CN, P^P = dppm (1B), dppe (2B), dppbz (3B)) have been prepared from the corresponding starting material [{Pt(R-C^C*)(μ-Cl)}2] (R = H, A, R = CN, B) and fully characterized. The new compound A has been prepared by a stepwise protocol. The photophysical properties of 1A–3A and 1B–3B have been widely studied and supported by the time-dependent-density functional theory. These compounds show an efficient blue (dppe, dppbz) or cyan (dppm) emission in PMMA films (5 wt %), with photoluminescence quantum yield (PLQY…

Shine bright or live long: substituent effects in [Cu(N^N)(P^P)]+-based light-emitting electrochemical cells where N^N is a 6-substituted 2,2'-bipyridine

We report [Cu(P^P)(N^N)][PF6] complexes with P^P = bis(2-(diphenylphosphino)phenyl)ether (POP) or 4,5-bis(diphenylphosphino)-9,9-dimethylxanthene (xantphos) and N^N = 6-methyl-2,2′-bipyridine (Mebpy), 6-ethyl-2,2′-bipyridine (Etbpy), 6,6′-dimethyl-2,2′-bipyridine (Me2bpy) or 6-phenyl-2,2′-bipyridine (Phbpy). The crystal structures of [Cu(POP)(Phbpy)][PF6]·Et2O, [Cu(POP)(Etbpy)][PF6]·Et2O, [Cu(xantphos)(Me2bpy)][PF6], [Cu(xantphos)(Mebpy)][PF6]·CH2Cl2·0.4Et2O, [Cu(xantphos)(Etbpy)][PF6]·CH2Cl2·1.5H2O and [Cu(xantphos)(Phbpy)][PF6] are described; each copper(I) centre is distorted tetrahedral. In the crystallographically determined structures, the N^N domain in [Cu(xantphos)(Phbpy)]+ and [Cu(…

Lead acetate precursor based p-i-n perovskite solar cells with enhanced reproducibility and low hysteresis

A low temperature approach for the fabrication of p-i-n perovskite solar cells is presented. Using lead acetate-based precursors, flat and homogeneous CH3NH3PbI3 films, compatible with the use of thin organic charge transport layers, can be obtained. The corresponding solar cells showed power conversion efficiency up to 12.5%, with remarkable reproducibility and very low hysteresis.

Nucleant layer effect on nanocolumnar ZnO films grown by electrodeposition

Different ZnO nanostructured films were electrochemically grown, using an aqueous solution based on ZnCl2, on three types of transparent conductive oxides grow on commercial ITO (In2O3:Sn)-covered glass substrates: (1) ZnO prepared by spin coating, (2) ZnO prepared by direct current magnetron sputtering, and (3) commercial ITO-covered glass substrates. Although thin, these primary oxide layers play an important role on the properties of the nanostructured films grown on top of them. Additionally, these primary oxide layers prevent direct hole combination when used in optoelectronic devices. Structural and optical characterizations were carried out by scanning electron microscopy, atomic for…

Effect of free rotation in polypyridinic ligands of Ru(ii) complexes applied in light-emitting electrochemical cells

In the present work we report the synthesis and the electrochemical, photoluminescent and electroluminescent properties of two new Ru(II) complexes described by the general formula [Ru(phen)2X](2+), where phen is 1,10-phenanthroline. The X ligand consists of a 2,2'-bipyridine (bpy) unit substituted with two phenyl rings connected to the bpy core through a saturated (Lhydro = 4,4'-diphenylethyl-2,2'-bipyridine) or a conjugated (LH = 4,4'-bis(α-styrene)-2,2'-bipyridine) carbon-carbon bridge. The photoluminescent spectra indicate that, both in solution and solid state, the complex bearing the aliphatic substitution bridges exhibits a higher quantum yield and a longer excited state lifetime tha…

Low-dimensional iodide perovskite nanocrystals enable efficient red emission

We report herein a simple ligand-assisted reprecipitation method at room temperature to synthesize mixed-cation hybrid organic–inorganic perovskite nanocrystals with low structural dimensionality.

Improving Perovskite Solar Cells: Insights From a Validated Device Model

To improve the efficiency of existing perovskite solar cells (PSCs), a detailed understanding of the underlying device physics during their operation is essential. Here, a device model has been developed and validated that describes the operation of PSCs and quantitatively explains the role of contacts, the electron and hole transport layers, charge generation, drift and diffusion of charge carriers and recombination. The simulation to the experimental data of vacuum-deposited CH3NH3PbI3 solar cells over multiple thicknesses has been fit and the device behavior under different operating conditions has been studied to delineate the influence of the external bias, charge-carrier mobilities, e…

Vacuum-Deposited Multication Tin-Lead Perovskite Solar Cells

The use of a combination of tin and lead is the most promising approach to fabricate narrow bandgap metal halide perovskites. This work presents the development of reproducible tin and lead perovskites by vacuum co-deposition of the precursors, a solvent-free technique which can be easily implemented to form complex stacks. Crystallographic and optical characterization reveal the optimal film composition based on cesium and methylammonium monovalent cations. Device optimization makes use of the intrinsically additive nature of vacuum deposition, resulting in solar cells with 8.89% photovoltaic efficiency. The study of the devices by impedance spectroscopy identifies bulk recombination as on…

PEDOT:Poly(1-vinyl-3-ethylimidazolium) dispersions as alternative materials for optoelectronic devices

p–n Metallophosphor based on cationic iridium(iii) complex for solid-state light-emitting electrochemical cells

An ionic transition-metal complex for improved charge transporting properties was designed, containing both n-type dimesitylboryl (BMes2) and p-type carbazole groups. The complex, [Ir(Bpq)2(CzbpyCz)]PF6 (1) (Bpq = 2-[4-(dimesitylboryl)phenyl] quinoline, CzbpyCz = 5,5′-bis(9-hexyl-9H-carbazol-3-yl)-2,2′-bipyridine) and its equivalent in which the BMes2 groups were substituted with carbazole moieties were evaluated on the photoluminescence and excited state properties in detail. According to the photophysical and electrochemical properties, we concluded that the BMes2 groups can increase the conjugation length of the cyclometalated C^N ligands and greatly enhance the phosphorescence efficienc…

Vacuum-Deposited Microcavity Perovskite Photovoltaic Devices

The interaction between semiconductor materials and electromagnetic fields resonating in microcavities or the light-matter coupling is of both fundamental and practical significance for improving the performance of various photonic technologies. The demonstration of light-matter coupling effects in the emerging perovskite-based optoelectronic devices via optical pumping and electrical readout (e.g., photovoltaics) and vice versa (e.g., light-emitting diodes), however, is still scarce. Here, we demonstrate the microcavity formation in vacuum-deposited methylammonium lead iodide (CH3NH3PbI3, MAPI) p-i-n photovoltaic devices fabricated between two reflecting silver electrodes. We tune the posi…

Twisted hexaazatrianthrylene: synthesis, optoelectronic properties and near-infrared electroluminescent heterojunctions thereof

The synthesis, optoelectronic properties and near-infrared electroluminescent heterojunctions of a twisted and soluble 7,8,15,16,23,24-hexaazatrianthrylene derivative are reported.

Metal-Oxide-Free Methylammonium Lead Iodide Perovskite-Based Solar Cells: the Influence of Organic Charge Transport Layers

Metal-oxide-free methylammonium lead iodide perovskite-based solar cells are prepared using a dual-source thermal evaporation method. This method leads to high quality reproducible films with large crystal domain sizes allowing for an in depth study of the effect of perovskite film thickness and the nature of the electron and hole blocking layers on the device performance. The power conversion efficiency increases from 4.7% for a device with only an organic electron blocking layer to almost 15% when an organic hole blocking layer is also employed. In addition to the in depth study on small area cells, larger area cells (approx. 1 cm(-2)) are prepared and exhibit efficiencies in excess of 10…

Capacitance-voltage characteristics of organic light-emitting diodes varying the cathode metal: Implications for interfacial states

Capacitance-voltage $(C\text{\ensuremath{-}}V)$ characteristics of organic light-emitting diodes based on a polyphenylenevinylene have been measured by means of impedance spectroscopy. The effect of the metallic cathode (Au, Ag, Al, Mg, and Ba) was analyzed in the low-frequency region $(2\phantom{\rule{0.3em}{0ex}}\mathrm{Hz})$ of the capacitive response. The $C\text{\ensuremath{-}}V$ curves collapse into a single pattern in the low bias region, and exhibit a dependence on the cathode work function showing a crossover from positive to negative (inductive) values. The voltage corresponding to the onset of the inductive behavior shifts toward higher bias as the cathode work function increases…

Phosphomolybdic acid as an efficient hole injection material in perovskite optoelectronic devices.

Efficient perovskite devices consist in a perovskite film sandwiched in between charge selective layers, in order to avoid non-radiative recombination. A common metal oxide used as p-type or hole transport layer is molybdenum oxide. MoO3 is of particular interest for its very large work function, which allows it to be used both as an interfacial charge transfer material as well as a dopant for organic semiconductors. However, high quality and high work function MoO3 is typically thermally evaporated in vacuum. An alternative solution-processable high work function material is phosphomolybdic acid (PMA), which is stable, commercially available and environmentally friendly. In this communicat…

High efficiency single-junction semitransparent perovskite solar cells

Semitransparent perovskite solar cells with a high power conversion efficiency (PCE) above 6% and 30% full device transparency have been achieved by implementing a thin perovskite layer and a simple foil compatible layout.

Red-light-emitting electrochemical cell using a polypyridyl iridium(III) polymer.

A deep-red phosphorescent ionic iridium(III) complex is prepared and incorporated into a polymer. Both the complex (1) and the polymer (2) were used as the single active material in solid-state light-emitting electrochemical cells (LECs). The devices built up using 1 and 2 emit in the deep-red region of the visible spectrum with CIE coordinates x = 0.710; y = 0.283 and x = 0.691; y = 0.289, respectively, making them one of the deepest-red emitting LECs reported. It is the first example of a polymeric LEC incorporating an ionic iridium complex, which exhibits increased stabilities compared with the device based on the small molecular weight complex.

A deep-blue emitting charged bis-cyclometallated iridium(iii) complex for light-emitting electrochemical cells

We report here a new cationic bis-cyclometallated iridium(III) complex, 1, with deep-blue emission at 440 nm and its use in Light-emitting Electrochemical Cells (LECs). The design is based on the 2′,6′-difluoro-2,3′-bipyridine skeleton as the cyclometallating ligand and a bis-imidazolium carbene-type ancillary ligand. Furthermore, bulky tert-butyl substituents are used to limit the intermolecular interactions. LECs have been driven both at constant voltage (6 V) and constant current (2.5 mA cm−2). The performances are significantly improved with the latter method, resulting overall in one of the best reported greenish-blue LECs having fast response (17 s), light intensity over 100 cd m−2 an…

Influence of the cyanine counter anions on a bi-layer solar cell performance

ABSTRACTWe present normal and inverted solution processed bi-layer solar cells using cationic cyanine dyes as the electron donor and a fullerene as the electron acceptor. The cells exhibit high open circuit voltages up to 1 volt showing the optimal alignment of donor and acceptor energy levels. We demonstrate the large effect that cyanine dye counter ions can have on the energetics of the solar cells and how the S-shaped current density vs. voltage (J-V) curves can be avoided.

Efficient Wide-Bandgap Mixed-Cation and Mixed-Halide Perovskite Solar Cells by Vacuum Deposition

Vacuum deposition methods are increasingly applied to the preparation of perovskite films and devices, in view of the possibility to prepare multilayer structures at low temperature. Vacuum-deposited, wide-bandgap solar cells based on mixed-cation and mixed-anion perovskites have been scarcely reported, due to the challenges associated with the multiple-source processing of perovskite thin films. In this work, we describe a four-source vacuum deposition process to prepare wide-bandgap perovskites of the type FA1-n Cs n Pb(I1-x Br x )3 with a tunable bandgap and controlled morphology, using FAI, CsI, PbI2, and PbBr2 as the precursors. The simultaneous sublimation of PbI2 and PbBr2 allows the…

Dual-emitting Langmuir-Blodgett film-based organic light-emitting diodes.

Langmuir-Blodgett (LB) films containing alternating layers of the metallosurfactants bis(4,4'-tridecyl-2,2'-bipyridine)-(4,4'-dicarboxy-2,2'-bipyridine) ruthenium(II)-bis(chloride) (1) and bis[2-(2,4-difluorophenyl)pyridine](4,4'-dinonadecyl-2,2'-bipyridine)iridium(III) chloride (2) have been prepared. Langmuir monolayers at the air-water interface of 1 and 2 with different anions in the subphase have been characterized by pi-A compression isotherms and Brewster angle microscopy (BAM). The transferred LB films have been characterized by IR, UV-vis and emission spectroscopy, and atomic force microscopy (AFM). Electroluminescent devices formed by LB films containing alternating layers of thes…

Influence of the intermediate density-of-states occupancy on open-circuit voltage of bulk heterojunction solar cells with different fullerene acceptors

Electron density of states (DOS) and recombination kinetics of bulk heterojunction solar cells consisting of a poly(3-hexylthiophene) (P3HT) donor and two fullerene acceptors, either [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) or 4,4′-dihexyloxydiphenylmethano[60]fullerene (DPM6), have been determined by means of impedance spectroscopy. The observed difference of 125 mV in the output open-circuit voltage is attributed to significant differences of the occupancy of the DOS in both fullerenes. Whereas DPM6 exhibits a full occupation of the electronic band, occupancy is restricted to the tail of the DOS in the case of PCBM-based devices, implying a higher rise of the Fermi level in the D…

Preparation and Characterization of Mixed Halide MAPbI 3− x Cl x Perovskite Thin Films by Three‐Source Vacuum Deposition

Tuning the Emission of Cationic Iridium (III) Complexes Towards the Red Through Methoxy Substitution of the Cyclometalating Ligand

The synthesis, characterization and evaluation in solid-state devices of a series of 8 cationic iridium complexes bearing different numbers of methoxy groups on the cyclometallating ligands are reported. The optoelectronic characterization showed a dramatic red shift in the absorption and the emission and a reduction of the electrochemical gap of the complexes when a methoxy group was introduced para to the Ir-C bond. The addition of a second or third methoxy group did not lead to a significant further red shift in these spectra. Emission maxima over the series ranged from 595 to 730 nm. All complexes possessing a motif with a methoxy group at the 3-position of the cyclometalating ligands s…

Solution processable high band gap hosts based on carbazole functionalized cyclic phosphazene cores for application in organic light‐emitting diodes

A new class of solution processable dendrimers based on cyclic phosphazene (CP) cores have been prepared and used as host materials for blue and green organic light emitting diodes (OLEDs). The dendrimers are prepared in high yield from minimal step reactions, are soluble in common solvents for solution processing, are amorphous, and have excellent thermal properties necessary for application in OLEDs. OLED efficiencies of 10.3 cd/A (4.2 Im/W) and 35.3 cd/A (33.5 Im/W) were achieved using commercially available Flrpic and Ir(mppy) 3 as blue and green phosphorescent emitters, respectively. These efficiencies were 2x higher than control devices prepared using poly(N-vinylcarbazole), the most …

Origin of the large spectral shift in electroluminescence in a blue light emitting cationic iridium(III) complex

A new, but archetypal compound [ Ir( ppy- F-2) (2)Me(4)phen] PF6, where ppy- F2 is 2-(2',4'- fluorophenyl) pyridine and Me(4)phen is 3,4,7,8- tetramethyl- 1,10- phenanthroline, was synthesized and used to prepare a solid-state light-emitting electrochemical cell (LEEC). This complex emits blue light with a maximum at 476 nm when photoexcited in a thin film, with a photoluminescence quantum yield of 52%. It yields an efficient single-component solid-state electroluminescence device with a current efficiency reaching 5.5 cd A(-1) and a maximum power efficiency of 5.8 Lm Watt(-1). However, the electroluminescence spectrum is shifted with respect to the photoluminescence spectrum by 80 nm resul…

Wide-Bite-Angle Diphosphine Ligands in Thermally Activated Delayed Fluorescent Copper(I) Complexes: Impact on the Performance of Electroluminescence Applications.

We report a series of seven cationic heteroleptic copper(I) complexes of the form [Cu(P^P)(dmphen)]BF4, where dmphen is 2,9-dimethyl-1,10-phenanthroline and P^P is a diphosphine chelate, in which the effect of the bite angle of the diphosphine ligand on the photophysical properties of the complexes was studied. Several of the complexes exhibit moderately high photoluminescence quantum yields in the solid state, with ΦPL of up to 35%, and in solution, with ΦPL of up to 98%. We were able to correlate the powder photoluminescence quantum yields with the % Vbur of the P^P ligand. The most emissive complexes were used to fabricate both organic light-emitting diodes and light-emitting electrochem…

A new cross-linkable 9,10-diphenylanthracene derivative as a wide bandgap host for solution-processed organic light-emitting diodes

Efficient organic light-emitting diodes (OLEDs) can be obtained using multilayered architectures where the processes of charge injection, transport and recombination are separated and optimized in each layer. Processing these structures from solution requires strategies to avoid redissolution or damage of the previously deposited layers. Several reports have demonstrated the development of cross-linkable hole transport materials, while less literature describes the synthesis and applications of such wide bandgap host materials for multilayered OLEDs. In this work we introduce a cross-linkable derivative of 9-(4-(10-phenylanthracene-9-yl)phenyl)-9H-carbazole incorporating styrene moieties (S…

Pyrene-fused bisphenazinothiadiazoles with red to NIR electroluminescence

The synthesis and characterisation of two pyrene-fused phenazinothiadiazole derivatives with different substituents is described. Light-emitting diodes incorporating such derivatives display red to near-infrared electroluminescence with emission peaks at wavelengths as long as 721 nm, illustrating that pyrene-fused bisphenazinothiadiazoles can serve as deep red and NIR emitters.

Emission energy of azole-based ionic iridium(III) complexes: a theoretical study.

A theoretical density functional theory study has been performed on different families of cationic cyclometallated Ir(III) complexes with the general formula [Ir(C^N)2(N^N)](+) and azole-based ligands. The goal was to investigate the effect that the number and position of the nitrogen atoms of the azole ring have on the electronic structure and emission wavelength of the complex. The increase in the number of nitrogen atoms changes the relative energy of the HOMO and LUMO levels and leads to a gradual shift in the emission wavelength that can be larger than 100 nm. The direction of the shift however depends on the ligand in which the azole ring is introduced. The emission shifts to bluer wa…

Copper(i) complexes for sustainable light-emitting electrochemical cells

Four prototype heteroleptic copper(I) complexes [Cu(bpy)(pop)][PF6] (bpy = 2,2′-bipyridine, pop = bis(2-(diphenylphosphino)phenyl)ether), [Cu(phen)(pop)][PF6] (phen = 1,10-phenanthroline), [Cu(bpy)(pdpb)][PF6] (pdpb = 1,2-bis(diphenylphosphino)benzene) and [Cu(phen)(pdpb)][PF6] are presented. The synthesis, X-ray structures, solution and solid-state photophysical studies, and the performance in light-emitting electrochemical cells (LECs) of these complexes are described. Their photophysical properties are interpreted with the help of density functional theory (DFT) calculations. The photophysical studies in solution and in the solid-state indicate that these copper(I) complexes show good lu…

Recent advances in light-emitting electrochemical cells

Light-emitting electrochemical cells (LECs) are solution-processable thin-film electroluminescent devices consisting of a luminescent material in an ionic environment. The simplest type of LEC is based on only one material, ionic transition-metal complexes (iTMCs). These materials are of interest for different scientific fields such as chemistry, physics, and technology as selected chemical modifications of iTMCs resulted in crucial breakthroughs for the performance of LECs. This short review highlights the different strategies used to design these compounds with the aim to enhance the performances of LECs.

Improving the efficiency of light-emitting diode based on a thiophene polymer containing a cyano group

Abstract We report on the overall improvement of a single layer organic light-emitting diode device based on poly{[3-hethylthiophene]-co-3-[2-( p -cyano-phenoxy)ethyl]thiophene} or namely PTOPhCN. This polymer was recently developed by adding a cyano group as a side-chain substituent of the thiophenic backbone onto the main polymer chain and showed promising results for light-emitting diode devices. Using an improved device layout, bright red electroluminescence was obtained at 4 V and showed a luminance of about 400 cd/m 2 at 8 V with current densities in the order of 6000 A/m 2 .

Improving the Turn-On Time of Light-Emitting Electrochemical Cells without Sacrificing their Stability

The luminance, efficiency, and turn-on time of ionic iridium complex-based light-emitting electrochemical cells can be improved by inserting an ionic liquid with high intrinsic conductivity. This results in a device in which the decrease in turn-on time is achieved while maintaining the stability.

Perovskite solar cells prepared by flash evaporation

A simple vacuum deposition method for the preparation of high quality hybrid organic-inorganic methylammonium lead iodide perovskite thin films is reported. When sandwiched in between organic charge transporting layers, such films lead to solar cells with a power conversion efficiency of 12.2%.

Simple approach for an electron extraction layer in all-vacuum processed n-i-p perovskite solar cell

Vacuum processing is considered to be a promising method allowing the scalable fabrication of perovskite solar cells (PSCs). In vacuum processed PSCs, the n-i-p structure employing organic charge transport layers is less common than the p-i-n structure due to limited options to achieve an efficient electron extraction layer (EEL) on indium tin oxide (ITO) with vacuum thermal evaporation. There are a number of specific applications where an n-i-p structure is required and therefore, it is of interest to have alternative solutions for the n-type contact in vacuum processed PSCs. In this work, we report an efficient vacuum deposited EEL using a mixture of conventional organic small molecules, …

Strontium Insertion in Methylammonium Lead Iodide: Long Charge Carrier Lifetime and High Fill-Factor Solar Cells.

The addition of Sr2+ in CH3 NH3 PbI3 perovskite films enhances the charge carrier collection efficiency of solar cells leading to very high fill factors, up to 85%. The charge carrier lifetime of Sr2+ -containing perovskites is in excess of 40 μs, longer than those reported for perovskite single crystals.

Photovoltaic devices employing vacuum-deposited perovskite layers

Organic–inorganic perovskites have emerged as one of the most promising materials for future optoelectronics applications, most notably photovoltaics. The achievement of high-efficiency solar cells has been possible mainly through the understanding of the perovskite formation during the solution deposition of thin films. Vacuum deposition methods have also been developed and have intrinsic advantages over solution-based processing, including control over the film thickness and composition, low-temperature processing, and the possibility of preparing multilayer structures. This article summarizes the latest advances in the vacuum deposition of hybrid perovskites, with an emphasis on the appl…

Preface to Special Issue of Energy Technology on Perovskite Optoelectronics

This Editorial introduces one of two companion Special Issues on “Halide Perovskites for Optoelectronics Applications” in Energy Technology and ChemSusChem following the ICMAT 2017 Conference in Singapore. More information on the other Special Issue can be found in the Editorial published in ChemSusChem.

Spontaneous Self-Assembly of a 1,8-Naphthyridine into Diverse Crystalline 1D Nanostructures: Implications on the Stimuli-Responsive Luminescent Behaviour

The previously reported organic solid-state fluorophore 7-(3,4-dimethoxyphenyl)-2-ethoxy-4-phenyl-1,8-naphthyridine-3-carbonitrile 1 was found to spontaneously self-organize into diverse 1D crystalline nanostructures by choosing appropriate liquid phase self-assembly conditions. Experimental results, as well as DFT quantum calculations (at the M06-2X/6-31+G(d) level), shed light on the aggregation mechanism. This was found in good agreement with molecules being primarily joined together through intermolecular alignment caused by electrostatic interactions, as well as minimization of the steric repulsions. This alignment provokes the preferential growth of the crystalline materials into 1D a…

Incorporation of a tricationic subphthalocyanine in an organic photovoltaic device

A new tricationic subphthalocyanine was synthesized and employed as light-harvesting and donor material in an ionic solid state organic photovoltaic cell. The incorporation of ionic dyes in organic photovoltaics aims to take advantage of ionic movement in order to enhance the charge transport properties of these materials. In this preliminary study, we report the results obtained in the fabrication of a partially solution-processed device with a cationic dye, where an effiency of 0.5% was reached.

Interfacial engineering for single and multijunction vacuum-deposited perovskite solar cells

Fully Vacuum-Processed Wide Band Gap Mixed-Halide Perovskite Solar Cells

Methylammonium lead mixed-halide perovskites MAPb(BrxI1–x)3 are promising materials for the preparation of tandem devices. When exposed to light, MAPb(BrxI1–x)3 segregates in iodide- and bromide-rich phases, limiting the achievable photovoltage and hence the attainable device efficiency. To date only solution-processed mixed-halide perovskites have been demonstrated. We present fully vacuum-deposited mixed-halide perovskite thin films with band gap of 1.72 and 1.87 eV, prepared by controlling the deposition rates of the different halide precursors. When used in thin-film devices, these materials lead to power conversion efficiencies of 15.9 and 10.5%, respectively, which are among the highe…

Efficient photovoltaic and electroluminescent perovskite devices.

Planar diode structures employing hybrid organic–inorganic methylammonium lead iodide perovskites lead to multifunctional devices exhibiting both a high photovoltaic efficiency and good electroluminescence. The electroluminescence strongly improves at higher current density applied using a pulsed driving method.

Dynamic doping in bright and stable light emitting electrochemical cells.

By using fast current density and luminance versus voltage (JL-V) analysis the device operation of sandwiched light emitting electrochemical cells (LECs) during their normal voltage driving operation mode is studied. In LECs the application of a voltage results in the movement of ions changing the state of the device, as a result the JL-V scans need to be performed fast and meet certain conditions to be meaningful. Space-charge limited current behavior is observed once the injection barriers are overcome. The increase of the current density after this point imply that the effective thickness of the devices is reduced which indicates the formation of more conductive regions adjacent to the e…

Evidence of Band Bending Induced by Hole Trapping at MAPbI3 Perovskite / Metal Interface

International audience; Electron injection by tunneling from a gold electrode and hole transport properties in polycrystalline MAPbI3 has been investigated using variable temperature experiments and numerical simulations. The presence of a large and unexpected band bending at the Au/MAPbI3 interface is revealed and attributed to the trapping of holes, which enhances the injection of electrons via tunneling. These results elucidate the role of volume and interface defects in state-of-the-art hybrid perovskite semiconductors.

White hybrid organic-inorganic light-emitting diode using ZnO as the air-stable cathode

An efficient white light emitting hybrid organic−inorganic device utilizing air-stable metal oxides as anode and cathode and a polyfluorene mixed with a phosphorescent iridium complex as the emitting material is presented.

Solvent-Free Synthesis and Thin-Film Deposition of Cesium Copper Halides with Bright Blue Photoluminescence

Non-toxic alternatives to lead halide perovskites are highly sought after for applications in optoelectronics. Blue-luminescent materials are especially demanded as they could be used to prepare white light-emitting diodes, with important potential applications in lighting systems. However, wide bandgap blue emitters with high photoluminescence quantum yields (PLQY) are typically more difficult to obtain as compared to green- or red-emitting ones. Here, we prepared two series of inorganic cesium copper halides, with the general formulas Cs3Cu2X5 and CsCu2X3 (X = Cl, Br, I, and mixtures thereof) by dry mechanochemical synthesis at room temperature. X-ray diffraction demonstrates quantitative…

Radiative and non-radiative losses by voltage-dependent in-situ photoluminescence in perovskite solar cell current-voltage curves

Abstract The rapid development of perovskite solar cells has been based on improvements in materials and device architectures, yet further progress towards their theoretical limit will require a detailed study of the main physical processes determining the photovoltaic performance. Luminescence can be a key parameter for this purpose, as it directly assesses radiative recombination. We present steady-state absolute photoluminescence of an operating device at varying voltages as a tool to study the loss mechanisms in perovskite devices. The calibration to absolute photon numbers gives access to the variation of the relative radiative/non-radiative recombination weighted along the measured po…

Light-emitting electrochemical cells: recent progress and future prospects

We provide a short review on light-emitting electrochemical cells (LECs), one of the simplest kinds of electroluminescent devices. In their simplest form, they consist of just one active layer containing an emitter and a salt. They operate with low voltages, which allows for high power efficiencies, and air-stable electrodes, which simplifies the encapsulation requirements. The aim of this review is to highlight the recent advances and the main remaining challenges. We describe the current understanding of their peculiar operation mechanism and focus on the major concepts used to improve their performance.

Near-Quantitative Internal Quantum Efficiency in a Light-Emitting Electrochemical Cell

A green-light-emitting iridium(III) complex was prepared that has a photoluminescence quantum yield in a thin-film configuration of almost unity. When used in a simple solid-state single-layer light-emitting electrochemical cell, it yielded an external quantum efficiency of nearly 15% and a power efficiency of 38 Lm/W. We argue that these high external efficiencies are only possible if near-quantitative internal electron-to-photon conversion occurs. This shows that the limiting factor for the efficiency of these devices is the photoluminescence quantum yield in a solid film configuration. The observed efficiencies show the prospect of these simple electroluminescent devices for lighting and…

Tuning the Self-Assembly of Rectangular Amphiphilic Cruciforms

The self-assembly of a series of nonionic amphiphilic cruciforms based on the 1,2,4,5-tetrakis(phenylethynyl)benzene (TPEB) skeleton, in which the peripheral substituents have been modified to modulate the morphology of the supramolecular structures, is reported. The presence of linear paraffinic and hydrophilic chains in TPEBs 1 and 2 gives rise to two-dimensional structures of high aspect ratio. In contrast, the incorporation of dendronized hydrophilic chains results in the formation of twisted ribbons in amphiphile 3 and impedes the organized self-assembly of TPEB 4. Theoretical calculations show that the self-assembly of these amphiphiles might be initiated with the formation of π-stack…

Efficient Semitransparent Perovskite Solar Cells Based on Thin Compact Vacuum Deposited CH3NH3PbI3 Films

Lead halide perovskite materials are promising candidates for the application of semitransparent solar cells due to their bandgap tunability and high device efficiencies. The high absorption coefficient of these materials, however, makes it difficult to attain high average visible transmittance values without compromising the power conversion efficiencies (PCEs). In this work, a co-evaporation process is employed to fabricate thin (50 and 100 nm) methylammonium lead iodide (MAPI) perovskite films and integrate them in semitransparent perovskite solar cells (ST-PSCs). Due to the compact nature of the thin MAPI films, the resultant fully vacuum and room temperature-processed devices demonstra…

Efficient deep-red light-emitting electrochemical cells based on a perylenediimide-iridium-complex dyad

A two-layer light-emitting electrochemical cell device based on a new perylenediimide-iridium-complex dyad is presented emitting in the deep-red region with high external quantum efficiencies (3.27%). Costa Riquelme, Ruben Dario, Ruben.Costa@uv.es ; Orti Guillen, Enrique, Enrique.Orti@uv.es ; Bolink, Henk, Henk.Bolink@uv.es ; Gierschner, Johannes, Johannes.Gierschner@uv.es

Red emitting [Ir(C^N)2(N^N)]+ complexes employing bidentate 2,2':6,2''-terpyridine ligands for light-emitting electrochemical cells

2,2':6',2''-Terpyridine (tpy), 4'-(4-HOC6H4)-2,2':6',2''-terpyridine (1), 4'-(4-MeOC6H4)-2,2':6',2''-terpyridine (2), 4'-(4-MeSC6H4)-2,2':6',2''-terpyridine (3), 4'-(4-H2NC6H4)-2,2':6',2''-terpyridine (4) and 4'-(4-pyridyl)-2,2':6',2''-terpyridine (4) act as N^N chelates in complexes of the type [Ir(C^N)2(N^N)][PF6] in which the cyclometallating ligand, C^N, is derived from 2-phenylpyridine (Hppy) or 3,5-dimethyl-1-phenyl-1H-pyrazole (Hdmppz). The single crystal structures of eight complexes have been determined, and in each iridium(III) complex cation, the non-coordinated pyridine ring of the tpy unit is involved in a face-to-face π-stacking interaction with the cyclometallated ring of an …

Relaxation of photogenerated carriers in P3HT:PCBM organic blends.

Relaxing in the sunlight. Long time-transient decays of photogenerated carriers in P3HT:PCBM blends for organic solar cells are interpreted in terms of the relaxation of hole carriers in a broad density of states. The after-pulse time-resolved microwave conductivity (TRMC) decays observed in P3HT:PCBM blends display a dependence on time close to t−β, independent of excitation intensity, in the 10 ns–1 μs range. This is explained in terms of the relaxation of carriers in a Gaussian density of states (DOS). The model is based on a demarcation level that moves with time by thermal release and retrapping of initially trapped carriers. The model shows that when the disorder is large the after-pu…

Charge Transport Layers Limiting the Efficiency of Perovskite Solar Cells: How To Optimize Conductivity, Doping, and Thickness

Perovskite solar cells (PSCs) are one of the main research topics of the photovoltaic community; with efficiencies now reaching up to 24%, PSCs are on the way to catching up with classical inorganic solar cells. However, PSCs have not yet reached their full potential. In fact, their efficiency is still limited by nonradiative recombination, mainly via trap-states and by losses due to the poor transport properties of the commonly used transport layers (TLs). Indeed, state-of-the-art TLs (especially if organic) suffer from rather low mobilities, typically within 10(-5) and 10(-2) cm(-2) V-1 s(-1), when compared to the high mobilities, 1-10 cm(-2) V-1 s(-1), measured for perovskites. This work…

Effect of the precursor's stoichiometry on the optoelectronic properties of methylammonium lead bromide perovskites

International audience; Methylammonium lead bromide (MAPbBr 3) perovskites have been widely studied in applications such as lasers and light-emitting diodes, thanks to their favorable bandgap, efficient charge transport, and the possibility of processing by simple solution methods. The film morphology has a large impact on the optical and electronic properties of the material; hence the deposition methods and the type of precursors used are crucial in the preparation of efficient optoelectronic devices. Here we studied the effect of the precursor´s stoichiometry of solution processed MAPbBr 3 thin films on their optical and electronic properties. We found a drastic effect of the stoichiomet…

Highly Efficient Thermally Co-evaporated Perovskite Solar Cells and Mini-modules

The rapid improvement in the power conversion efficiency (PCE) of perovskite solar cells (PSCs) has prompted interest in bringing the technology toward commercialization. Capitalizing on existing industrial processes facilitates the transition from laboratory to production lines. In this work, we prove the scalability of thermally co-evaporated MAPbI3 layers in PSCs and mini-modules. With a combined strategy of active layer engineering, interfacial optimization, surface treatments, and light management, we demonstrate PSCs (0.16 cm2 active area) and mini-modules (21 cm2 active area) achieving record PCEs of 20.28% and 18.13%, respectively. Un-encapsulated PSCs retained ∼90% of their initial…

Low Current Density Driving Leads to Efficient, Bright and Stable Green Electroluminescence

Electroluminescent devices have the potential to reshape lighting and display technologies by providing low-energy consuming solutions with great aesthetic features, such as flexibility and transparency. In particular, light-emitting electrochemical cells (LECs) are among the simplest electro-luminescent devices. The device operates with air-stable materials and the active layer can be resumed to an ionic phosphorescent emitter. As a consequence, LECs can be assembled using solution-process technologies, which could allow for low-cost and large-area lighting applications in the future. High efficiencies have been reported at rather low luminances (<50 cd m(-2)) and at very low current densi…

Exploring the effect of the cyclometallating ligand in 2-(pyridine-2-yl)benzo[d]thiazole-containing iridium(III) complexes for stable light-emitting electrochemical cells

The preparation and characterization of a series of iridium(III) ionic transition-metal complexes for application in light-emitting electrochemical cells (LECs) are reported. The complexes are of the type [Ir(C^N)2(N^N)][PF6] in which C^N is one of the cyclometallating ligands 2-(3-(tert-butyl)phenyl)pyridine (tppy), 2-phenylbenzo[d]thiazole (pbtz), 1-phenyl-1H-pyrazole (ppz) and 1-phenylisoquninoline (piq), and N^N is 2-(pyridine-2-yl)benzo[d]thiazole (btzpy). The variation in the C^N ligands allows the HOMO energy level to be tuned, leading to HOMO–LUMO gaps in the range 2.76–3.01 eV and values of Eox1/2 of 0.81–1.11 V. In solution, the complexes are orange to deep-red emitters (λmax in t…

Phosphorescent hybrid organic-inorganic light-emitting diodes.

Quadruple-Cation Wide-Bandgap Perovskite Solar Cells with Enhanced Thermal Stability Enabled by Vacuum Deposition.

Vacuum processing of multicomponent perovskites is not straightforward, because the number of precursors is in principle limited by the number of available thermal sources. Herein, we present a process which allows increasing the complexity of the formulation of vacuum-deposited lead halide perovskite films by multisource deposition and premixing both inorganic and organic components. We apply it to the preparation of wide-bandgap CsMAFA triple-cation perovskite solar cells, which are found to be efficient but not thermally stable. With the aim of stabilizing the perovskite phase, we add guanidinium (GA+) to the material formulation and obtained CsMAFAGA quadruple-cation perovskite films wi…

Peripheral halo-functionalization in [Cu(N^N)(P^P)]+ emitters: influence on the performances of light-emitting electrochemical cells

A series of heteroleptic [Cu(N^N)(P^P)][PF6] complexes is described in which P^P = bis(2-(diphenylphosphino)phenyl)ether (POP) or 4,5-bis(diphenylphosphino)-9,9-dimethylxanthene (xantphos) and N^N = 4,4′-diphenyl-6,6′-dimethyl-2,2′-bipyridine substituted in the 4-position of the phenyl groups with atom X (N^N = 1 has X = F, 2 has X = Cl, 3 has X = Br, 4 has X = I; the benchmark N^N ligand with X = H is 5). These complexes have been characterized by multinuclear NMR spectroscopy, mass spectrometry, elemental analyses and cyclic voltammetry; representative single crystal structures are also reported. The solution absorption spectra are characterized by high energy bands (arising from ligand-c…

Combined thermal evaporated and solution processed organic light emitting diodes

Abstract Highly efficient, partly solution processed phosphorescent red, green and white organic light emitting diodes with small molecular weight host materials are prepared from commercially available starting compounds. Starting from an evaporated reference device, layers are stepwise replaced by solution processed layers. Replacing the evaporated hole transport layer by a solution processed polymer interlayer does not affect the performance and allows spincoating of the emissive layer after annealing of the polymer. Devices with, next to the spincoated hole injection and transport layer, a solution processed emission layer show similar characteristics and efficiencies as the reference d…

Deposition Kinetics and Compositional Control of Vacuum-Processed CH3NH3PbI3 Perovskite

Halide perovskites have generated considerable research interest due to their excellent optoelectronic properties in the past decade. To ensure the formation of high-quality semiconductors, the deposition process for the perovskite film is a critical issue. Vacuum-based processing is considered to be a promising method, allowing, in principle, for uniform deposition on a large area. One of the benefits of vacuum processing is the control over the film composition through the use of quartz crystal microbalances (QCMs) that monitor the rates of the components in situ. In metal halide perovskites, however, one frequently employed component or precursor, CH3NH3I, exhibits nonstandard sublimatio…

Interpretation of capacitance spectra and transit times of single carrier space-charge limited transport in organic layers with field-dependent mobility

The ac impedance characteristics of a single carrier with space-charge limited current (SCLC) transport in organic layers with field-dependent mobility is analyzed, indicating the similarities as well as the differences to the constant mobility case. The model provides capacitance spectra and transit times from different calculation methods, in relation to the electric field distribution in the SCLC regime. It is found that the low frequency capacitance lies in the range 3Cg/4 < Cif < Cg, with respect to the geometric capacitance Cg. An approximated expression for the variation of the transit time with applied bias is derived, in good agreement with exact calculations. Experimental results …

Narrowband Monolithic Perovskite-Perovskite Tandem Photodetectors

Narrowband photodetectors (PDs) are sought after for many applications requiring selective spectral response. The most common systems combine optical bandpass filters with broadband photodiodes. This work reports a method to obtain a narrowband response in a perovskite PD by the monolithic integration of a perovskite photoconductor and a perovskite photodiode. The spectral response of the tandem PD is determined by the bandgap energy difference of the two perovskites, and exhibits a full width at half maximum below 85 nm, an external quantum efficiency up to 68% and a high specific detectivity of ≈1012 Jones in reverse bias, enabling the device to detect weak light signals. The absorption p…

Increasing the efficiency of light-emitting electrochemical cells by limiting the exciton quenching

ABSTRACTLight-emitting electrochemical cells (LECs) are one of the simplest electroluminescent devices. The possibility to be processed from solution and to operate with air-stable materials makes them an attractive alternative to organic light emitting diodes (OLEDs). Still their efficiencies are below those obtained in OLEDs. Additionally the best efficiencies were reported at low luminances and sustained for a short period of time. Here we show that for a LEC employing an orange-emitting charged iridium complex that is driven using a pulsed driving scheme high efficiencies of up to 20.5 cd A-1 can be obtained at high luminance and sustained over the device lifetime. It is also shown that…

Zinc oxide nanocrystals as electron injecting building blocks for plastic light sources

Hybrid inorganic–organic light emitting devices (HyLEDs) employing ZnO nanocrystals as one of their metal oxide contacts lead to very bright devices on plastic substrates with performances superior to those obtained from the rigid counterparts employing planar films of bulk ZnO. The superior performance is related to the increase in the bandgap of the ZnO nanocrystals caused by quantum confinement effects. We demonstrate that this effect diminishes with increasing annealing temperature of the ZnO nanocrystal layer due to a gradual decrease of the bandgap towards the bulk ZnO value. Therefore, best performances were obtained with room temperature processing of the ZnO nanocrystals.

Long-Living Light-Emitting Electrochemical Cells - Control through Supramolecular Interactions

Light-emitting electrochemical cells with lifetimes surpassing 3000 hours at an average luminance of 200 cd m(-2) are obtained with an ionic iridium(III) complex conveniently designed to form a supramolecularly caged structure.

Mechanochemical synthesis of inorganic halide perovskites: evolution of phase-purity, morphology, and photoluminescence

Dry mechanochemical ball-milling of halide precursor salts is a promising route for the synthesis of high-purity halide perovskites in a fast and solvent-free manner. However, there is a lack of information on the process mechanisms, kinetics, and possible side-effects. Here, we investigated in detail the mechanochemical synthesis of fully-inorganic CsPbBr3 by ball-milling of stoichiometric CsBr and PbBr2. Detailed structural, morphological and optical analyses reveal several beneficial and detrimental effects of milling as a function of time. Three stages are identified during the process: (i) at short milling times (t < 5 min) different ternary compounds are formed, including stoichiometr…

Molecular Engineering of Iridium Blue Emitters Using Aryl N‐Heterocyclic Carbene Ligands

The synthesis of a new series of neutral bis[2-(2,4-difluorophen-2-yl)pyridine][1-(2-aryl)-3-methylimidazol-2-ylidene]iridium(III) complexes is reported. Each complex has been characterized by NMR spectroscopy, UV/Vis spectrophotometry, and cyclic voltammetry, and the photophysical properties examined in depth. Furthermore, two of the complexes have been characterized by single-crystal X-ray diffraction analysis. By systematically modifying the cyclometalating aryl group on the N-heterocyclic carbene (NHC) ligand from 2,4-dimethoxyphenyl to 6-methoxy-2-methyl-3-pyridyl, the energy levels of the Ir complexes were modified to produce new blue emitters with increased HOMO and triplet-state ene…

Polymorphism-Triggered Reversible Thermochromic Fluorescence of a simple 1,8-Naphthyridine

The fluorescent behavior in the solid state of a naphthyridine-based donor–acceptor heterocycle is presented. Synthesized as a crystalline blue-emissive solid (Pbca), the compound can easily be transformed in its P21/c polymorphic form by heating. The latter material shows blue to cyan emission switching triggered by a reversible thermally induced phase transformation. This fact, the reversible acidochromism, and the strong anisotropic fluorescence of the compound in the solid state, account for the potential of 1,8-naphthyridines as simple and highly tunable organic compounds in materials science.

A counterion study of a series of [Cu(P^P)(N^N)][A] compounds with bis(phosphane) and 6-methyl and 6,6′-dimethyl-substituted 2,2′-bipyridine ligands for light-emitting electrochemical cells†

The syntheses and characterisations of a series of heteroleptic copper(i) compounds [Cu(POP)(Mebpy)][A], [Cu(POP)(Me2bpy)][A], [Cu(xantphos)(Mebpy)][A] and [Cu(xantphos)(Me2bpy)][A] in which [A]− is [BF4]−, [PF6]−, [BPh4]− and [BArF4]− (Mebpy = 6-methyl-2,2′-bipyridine, Me2bpy = 6,6′-dimethyl-2,2′-bipyridine, POP = oxydi(2,1-phenylene)bis(diphenylphosphane), xantphos = (9,9-dimethyl-9H-xanthene-4,5-diyl)bis(diphenylphosphane), [BArF4]− = tetrakis(3,5-bis(trifluoromethyl)phenyl)borate) are reported. Nine of the compounds have been characterised by single crystal X-ray crystallography, and the consequences of the different anions on the packing interactions in the solid state are discussed. T…

ITO top-electrodes via industrial-scale PLD for efficient buffer-layer-free semitransparent perovskite solar cells

The deposition of transparent conductive oxides (TCO) usually employs harsh conditions that are frequently harmful to soft/organic underlayers. Herein, successful use of an industrial pulsed laser deposition (PLD) tool to directly deposit indium tin oxide (ITO) films on semitransparent vacuum-deposited perovskite solar cells without damage to the device stack is demonstrated. The morphological, electronic, and optical properties of the PLD deposited ITO films are optimized. A direct relation between the PLD chamber pressure and the solar cell performance is obtained. The semitransparent perovskite solar cells prepared exclusively by vacuum-assisted techniques had fill factors of 78% and exc…

Efficient wide band gap double cation – double halide perovskite solar cells

In this work we study the band gap variation and properties of the perovskite compound Cs0.15FA0.85Pb(BrxI1−x)3 as a function of the halide composition, with the aim of developing an efficient complementary absorber for MAPbI3 in all-perovskite tandem devices. We have found the perovskite stoichiometry Cs0.15FA0.85Pb(Br0.7I0.3)3 to be a promising candidate, thanks to its band gap of approximately 2 eV. Single junction devices using this perovskite absorber lead to a maximum PCE of 11.5%, among the highest reported for solar cells using perovskites with a band gap wider than 1.8 eV.

An inconvenient influence of iridium(III) isomer on OLED efficiency.

The recently reported heteroleptic cyclometallated iridium(III) complex [Ir(2-phenylpyridine)(2)(2-carboxy-4-dimethylaminopyridine)] N984 and its isomer N984b have been studied more in detail. While photo- and electrochemical properties are very similar, DFT/TDDFT calculations show that the two isomers have different HOMO orbital characteristics. As a consequence, solution processed OLEDs made using a mixture of N984 and isomer N984b similar to vacuum processed devices show that the isomer has a dramatic detrimental effect on the performances of the device. In addition, commonly used thermogravimetric analysis is not suitable for showing the isomerization process. The isomer could impact pe…

Unravelling steady-state bulk recombination dynamics in thick efficient vacuum-deposited perovskite solar cells by transient methods

Accurately identifying and understanding the dominant charge carrier recombination mechanism in perovskite solar cells are of crucial importance for further improvements of this already promising photovoltaic technology. Both optical and electrical transient methods have previously been employed to strive for this warranted goal. However, electrical techniques can be strongly influenced by the capacitive response of the device which hides the carrier recombination dynamics that are relevant under steady state conditions. To ascertain the identification of steady state relevant charge carrier dynamics, it is beneficial to evaluate thicker films to minimize the impact of device capacitance. H…

Recombination in Perovskite Solar Cells

Trap-assisted recombination, despite being lower as compared with traditional inorganic solar cells, is still the dominant recombination mechanism in perovskite solar cells (PSCs) and limits their efficiency. We investigate the attributes of the primary trap assisted recombination channels (grain boundaries and interfaces) and their correlation to defect ions in PSCs. We achieve this by using a validated device model to fit the simulations to the experimental data of efficient vacuum-deposited p-i-n and n-i-p CH3NH3PbI3 solar cells, including the light intensity dependence of the open circuit voltage and fill factor. We find that, despite the presence of traps at interfaces and grain bounda…

Vacuum-Deposited 2D/3D Perovskite Heterojunctions

Low-dimensional (quasi-) 2D perovskites are being extensively studied in order to enhance the stability and the open-circuit voltage of perovskite solar cells. Up to now, thin 2D perovskite layers on the surface and/or at the grain boundaries of 3D perovskites have been deposited solely by solution processing, leading to unavoidable intermixing between the two phases. In this work, we report the fabrication of 2D/3D/2D perovskite heterostructures by dual-source vacuum deposition, with the aim of studying the interaction between the 3D and 2D phases as well as the charge transport properties of 2D perovskites in neat 2D/3D interfaces. Unlike what is normally observed in solution-processed 3D…

Interface engineering in efficient vacuum deposited perovskite solar cells

Abstract We studied the effect of the charge transport layers in p-i-n perovskite solar cells using vacuum deposited methylammonium lead iodide thin-film absorbers. While solution-processed perovskite films are frequently deposited directly on PEDOT:PSS leading to good solar cell performances, in some cases even to very good Voc values, we show that in devices employing vacuum deposited MAPbI3 perovskites, the removal of the polyTPD electron blocker substantially reduces the photovoltaic behavior. This is indicative of rather different charge transport properties in the vacuum deposited MAPbI3 perovskites compared to those prepared from solution. On the other hand, we investigated the use o…

Highly Luminescent Transparent Cs 2 Ag x Na 1– x Bi y In 1– y Cl 6 Perovskite Films Produced by Single-Source Vacuum Deposition

Thermal deposition of halide perovskites as a universal and scalable route to transparent thin films becomes highly challenging in the case of lead-free double perovskites, requiring the evaporation dynamics of multiple metal halide sources to be balanced or a single-phase precursor preliminary synthesized to achieve a reliable control over the composition and the phase of the final films. In the present Letter, the feasibility of the single-source vacuum deposition of microcrystalline Cs2AgxNa1-xBiyIn1-yCl6 double perovskites into corresponding transparent nanocrystalline films while preserving the bulk spectral and structural properties is shown. The perovskite films produced from the mos…

White Light-Emitting Electrochemical Cells Based on the Langmuir–Blodgett Technique

Light-emitting electrochemical cells (LECs) showing a white emission have been prepared with Langmuir-Blodgett (LB) films of the metallosurfactant bis[2-(2,4-difluorophenyl)pyridine][2-(1-hexadecyl-1H-1,2,3-triazol-4-yl)pyridine]iridium(III) chloride (1), which work with an air-stable Al electrode. They were prepared by depositing a LB film of 1 on top of a layer of poly(N,N'-diphenyl-N,N'-bis(4-hexylphenyl)-[1,1'-biphenyl]-4,4'-diamine (pTPD) spin-coated on indium tin oxide (ITO). The white color of the electroluminescence of the device contrasts with the blue color of the photoluminescence of 1 in solution and within the LB films. Furthermore, the crystal structure of 1 is reported togeth…

Reduced Recombination Losses in Evaporated Perovskite Solar Cells by Postfabrication Treatment

The photovoltaic perovskite research community has now developed a large set of tools and techniques to improve the power conversion efficiency (PCE). One such arcane trick is to allow the finished devices to dwell in time, and the PCE often improves. Herein, a mild postannealing procedure is implemented on coevaporated perovskite solar cells confirming a substantial PCE improvement, mainly attributed to an increased open-circuit voltage (V\(_{OC}\)). From a V\(_{OC}\) of around 1.11 V directly after preparation, the voltage improves to more than 1.18 V by temporal and thermal annealing. To clarify the origin of this annealing effect, an in-depth device experimental and simulation character…

Fully Evaporated High Efficiency Single Junction and Tandem Perovskite based Solar Cells.

Flexible high efficiency perovskite solar cells

Flexible perovskite based solar cells with power conversion efficiencies of 7% have been prepared on PET based conductive substrates. Extended bending of the devices does not deteriorate their performance demonstrating their suitability for roll to roll processing.

Efficient Vacuum-Deposited Perovskite Solar Cells with Stable Cubic FA 1– x MA x PbI 3

Preparation of black formamidinium lead iodide (FAPbI3) requires high temperature annealing and the incorporation of smaller A-site cations, such as methylammonium (MA+), cesium or rubidium. A major advantage of vacuum processing is the possibility to deposit perovskite films at room temperature (RT), without any annealing step. Here we demonstrate stabilization of the cubic perovskite phase at RT, in a three-sources co-sublimation method. We found that the MA+ incorporation is a self-limiting process, where the amount of MA+ which is incorporated in the perovskite is essentially unvaried with increasing MAI deposition rate. In this way a phase-pure, cubic perovskite with a bandgap of 1.53 …

Dynamic doping and degradation in sandwich-type light-emitting electrochemical cells

Photoluminescence spectroscopy has been performed in situ during device operation and after switch-off on ionic transition metal complex (iTMC)-based sandwich-type light-emitting electrochemical cells (LECs). It is demonstrated that the photoluminescence of the LECs decreases with increasing operating time. For operating times up to three hours the decline in photoluminescence is fully recoverable after switching off the bias. These results imply that doping of the iTMC layer is responsible, not only, for the turn-on of LECs but also for their lifetimes.

Amplified spontaneous emission in thin films of quasi-2D BA3MA3Pb5Br16 lead halide perovskites

Quasi-2D (two-dimensional) hybrid perovskites are emerging as a new class of materials with high photoluminescence yield and improved stability compared to their three-dimensional (3D) counterparts. Nevertheless, despite their outstanding emission properties, few studies have been reported on amplified spontaneous emission (ASE) and a thorough understanding of the photophysics of these layered materials is still lacking. In this work, we investigate the ASE properties of multilayered quasi-2D BA3MA3Pb5Br16 films through the dependence of the photoluminescence on temperature and provide a novel insight into the emission processes of quasi-2D lead bromide perovskites. We demonstrate that the …

Tuning the photophysical properties of cationic iridium(iii) complexes containing cyclometallated 1-(2,4-difluorophenyl)-1H-pyrazole through functionalized 2,2′-bipyridineligands: blue but not blue enough

Four new heteroleptic iridium(III) complexes in the family [Ir(dfppz)(2)((NN)-N-boolean AND)](+), where Hdfppz = 1-(2,4-difluorophenyl)-1H-pyrazole and (NN)-N-boolean AND = 6-phenyl-2,2'-bipyridine (1), 4,4'-(di-tert-butyl)-6-phenyl-2,2'-bipyridine (2), 4,4'-(di-tert-butyl)-6,6'-diphenyl-2,2'-bipyridine (3) and 4,4'-bis(dimethylamino)-2,2'-bipyridine (4), have been synthesized as the hexafluoridophosphate salts and fully characterized. Single crystal structures of ligand 3 and the precursor [Ir-2(dfppz)(4)(mu-Cl)(2)] have been determined, along with the structures of the complexes 4{[Ir(dfppz)(2)(1)][PF6]}center dot 3CH(2)Cl(2), [Ir(dfppz)(2)(3)][PF6]center dot CH2Cl2 and [Ir(dfppz)(2)(4)][…

Efficient, Cyanine Dye Based Bilayer Solar Cells

Simple bilayer solar cells, using commercially available cationic cyanine dyes as donors and evaporated C60 layer as an acceptor are prepared. Cyanine dyes with absorption maxima of 578, 615 and 697 nm having either perchlorate or hexafluorophosphate counter-ions are evaluated. The perchlorate dye leads to cells with S-shape current-voltage curves; only the dyes with the hexafluorophosphate counter-ions lead to efficient solar cells. When the wide bandgap dyes are employed, S-shape current-voltage curves are obtained when the conductive polymer PEDOT:PSS is used as hole transport layer. Substitution of PEDOT:PSS with MoO3 leads to cells with more rectangular current–voltage curves and high …

Millisecond radiative recombination in poly(phenylene vinylene)-based light-emitting diodes from transient electroluminescence

The current and electroluminescence transient responses of standard poly phenylene vinylene -based light-emitting devices have been investigated. The electroluminescence time response is longer milliseconds scale than the current switch-off time by more than one order of magnitude, in the case of small area devices 0.1 cm2 . For large area devices 6 cm2 the electroluminescence decay time decreases from 1.45 ms to 100 s with increasing bias voltage. The fast current decay limits the electroluminescence decay at higher voltages. Several approaches are discussed to interpret the observed slow decrease of electroluminescence after turning off the bias. One relies upon the Langevin-type bimolecu…

Transient drift‐diffusion simulation of the open circuit voltage decay in ionic perovskite solar cells

Photovoltaic Devices Using Sublimed Methylammonium Lead Iodide Perovskites: Long‐Term Reproducible Processing

Incorporation of potassium halides in the mechanosynthesis of inorganic perovskites: feasibility and limitations of ion-replacement and trap passivation

Potassium halides (KX; X = I, Br, or Cl) were incorporated as partial replacements of CsBr in the mechanosynthesis of CsPbBr3. This led to partial substitution of both monovalent ions forming mixed Cs1−xKxPbBr3−yXy perovskites. Longer photoluminescence lifetimes were also observed, possibly linked to the formation of a non-perovskite KPb2X5 passivating layer.

Pulsed Laser Deposition of Cs 2 AgBiBr 6 : from Mechanochemically Synthesized Powders to Dry, Single-Step Deposition

Cs2AgBiBr6 has been proposed as a promising lead-free and stable double perovskite alternative to hybrid and lead-based perovskites. However, the low solubility of precursors during wet synthesis, or the distinct volatility of components during evaporation, results in complex multistep synthesis approaches, hampering the widespread employment of Cs2AgBiBr6 films. Here, we present pulsed laser deposition of Cs2AgBiBr6 films as a dry, single-step and single-source deposition approach for high-quality film formation. Cs2AgBiBr6 powders were prepared by mechanochemical synthesis and pressed into a solid target maintaining phase purity. Controlled laser ablation of the double perovskite target i…

Highly Luminescent Half-Lantern Cyclometalated Platinum(II) Complex: Synthesis, Structure, Luminescence Studies, and Reactivity.

The half-lantern compound [{Pt(bzq)(μ-C 7H 4NS 2-κN,S)} 2]•Me 2CO (1) was obtained by reaction of equimolar amounts of potassium 2-mercaptobenzothiazolate (KC 7H 4NS 2) and [Pt(bzq)(NCMe) 2]ClO 4. The Pt(II)•••Pt(II) separation in the neutral complex [{Pt(bzq)(μ-C 7H 4NS 2-κN,S)} 2] is 2.910 (2) Å, this being among the shortest observed in half-lantern divalent platinum complexes. Within the complex, the benzo[h]quinoline (bzq) groups lie in close proximity with most C•••C distances being between 3.3 and 3.7 Å, which is indicative of significant π-π interactions. The reaction of 1 with halogens X 2 (X 2 = Cl 2, Br 2, or I 2) proceeds with a two-electron oxidation to give the corresponding d…

Anionic Cyclometalated Iridium(III) Complexes with a Bis-Tetrazolate Ancillary Ligand for Light-Emitting Electrochemical Cells

none 10 si A series of monoanionic Ir(III) complexes (2-4) of general formula [Ir(C^N)2(b-trz)](TBA) are presented, where C^N indicates three different cyclometallating ligands (Hppy = 2-phenylpyridine; Hdfppy = 2-(2,4-difluoro-phenyl)pyridine; Hpqu = 2-methyl-3-phenylquinoxaline), b-trz is a bis-tetrazolate anionic N^N chelator (H2b-trz = di(1H-tetrazol-5-yl)methane), and TBA = tetrabutylammonium. 2-4 are prepared in good yields by means of the reaction of the suitable b-trz bidentate ligand with the desired iridium(III) precursor. The chelating nature of the ancillary ligand, thanks to an optimized structure and geometry, improves the stability of the complexes, which have been fully char…

Phosphane tuning in heteroleptic [Cu(N^N)(P^P)]+ complexes for light-emitting electrochemical cells

The synthesis and characterization of five [Cu(P^P)(N^N)][PF 6 ] complexes in which P^P = 2,7-bis( tert -butyl)-4,5-bis(diphenylphosphino)-9,9-dimethylxanthene ( t Bu 2 xantphos) or the chiral 4,5-bis(mesitylphenylphosphino)-9,9-dimethylxanthene (xantphosMes 2 ) and N^N = 2,2'-bipyridine (bpy), 6-methyl-2,2'-bipyridine (6-Mebpy) or 6,6'-dimethyl-2,2'-bipyridine (6,6'-Me 2 bpy) are reported. Single crystal structures of four of the compounds confirm that the copper(I) centre is in a distorted tetrahedral environment. In [Cu(xantphosMes 2 )(6-Mebpy)][PF 6 ], the 6-Mebpy unit is disordered over two equally populated orientations and this disorder parallels a combination of two dynamic processe…

Tunable luminescent lead bromide complexes

Lead halides are used extensively to prepare perovskite-based devices but it is less known that lead halides can also form luminescent complexes in solvents. Using polyethylene glycol as a solvent, a lead bromide complex with a photoluminescence quantum yield over 20% is obtained and the photoluminescence peak can be shifted around 50 nm with different alkylammonium bromides.

Fine‐Tuning of Photophysical and Electronic Properties of Materials for Photonic Devices Through Remote Functionalization

We report four new iridium(III) complexes of the type [Ir(ppy)2(N?N)][PF6] in which N?N is a 4,6-diphenyl-2,2`-bipyridine and the 4-phenyl ring is substituted at either the para or meta positions [4-Me, N?N = 1; 4-Br, N?N = 2; 3,5-Br2, N?N = 3; 3,5-(C6H4-4-NPh2)2, N?N = 4]. The complexes have been fully characterized, and single-crystal diffraction analyses of [Ir(ppy)2(N?N)][PF6] (N?N = 13) confirmed that each [Ir(ppy)2(N?N)]+ cation exhibits face-to-face p-stacking between the pendant phenyl substituent of the N?N ligand and the cyclometallated phenyl ring of an adjacent [ppy] ligand. In solution, the complexes are short-lived emitters; the emission maxima for [Ir(ppy)2(1)][PF6], [Ir(ppy)…

Negative capacitance caused by electron injection through interfacial states in organic light-emitting diodes

The negative capacitance frequently observed at low frequencies in organic light-emitting diodes (LEDs) is explained as a signature of sequential electron injection at the organic/metal interface first to states in the bandgap in the dipole layer and then to bulk states. The negative capacitance occurs when the interfacial states depart from equilibrium with the metal Fermi level due to an increasing rate of hopping to the bulk states. A simple kinetic model compares well with the experimental results and provides a new tool to investigate interfacial properties for improving the performance of organic LEDs.

Stable and Efficient Solid-State Light-Emitting Electrochemical Cells Based on a Series of Hydrophobic Iridium Complexes

Light-emitting electrochemical cells (LECs) based on ionic transition-metal complexes (iTMCs) exhibiting high efficiency, short turn-on time, and long stability have recently been presented. Furthermore, LECs emitting in the full range of the visible spectrum including white light have been reported. However, all these achievements were obtained individually, not simultaneously, using in each case a different iTMC. In this work, device stability is maintained by employing intrinsically stable ionic iridium complexes, while increasing the complex and the device quantum yields for exciton-to-photon conversion. This is done by sequentially modifying the archetype ionic iridium complex [Ir(ppy)…

Light-Emitting Electrochemical Cells Using Cyanine Dyes as the Active Components

Light-emitting electrochemical cells (LECs) based on cyanine molecules were prepared. High photoluminescence quantum yields were obtained for host-guest films using two cyanine dyes, reaching 27%. Sandwiching these films in between two electrodes allows for very stable near-infrared emission with a maximum radiant flux of 1.7 W m(-2) at an external quantum efficiency of 0.44%.

Luminescent copper(i) complexes with bisphosphane and halogen-substituted 2,2′-bipyridine ligands

Heteroleptic [Cu(P^P)(N^N)][PF6] complexes, where N^N is a halo-substituted 2,2'-bipyridine (bpy) and P^P is either bis(2-(diphenylphosphino)phenyl)ether (POP) or 4,5-bis(diphenylphosphino)-9,9- dimethylxanthene (xantphos) have been synthesized and investigated. To stabilize the tetrahedral geometry of the copper(I) complexes, the steric demands of the bpy ligands have been increased by introducing 6- or 6,6'-halo-substituents in 6,6'-dichloro-2,2'-bipyridine (6,6'-Cl2bpy), 6-bromo-2,2'- bipyridine (6-Brbpy) and 6,6'-dibromo-2,2'-bipyridine (6,6'-Br2bpy). The solid-state structures of [Cu(POP)(6,6'-Cl2bpy)][PF6], [Cu(xantphos)(6,6'-Cl2bpy)][PF6].CH2Cl2, [Cu(POP)(6-Brbpy)][PF6] and [Cu(xantp…

Ester-functionalized poly(3-alkylthiophene) copolymers : synthesis, physicochemical characterization and performance in bulk heterojunction organic solar cells

Abstract The introduction of functional moieties in the donor polymer (side chains) offers a potential pathway toward selective modification of the nanomorphology of conjugated polymer:fullerene active layer blends applied in bulk heterojunction organic photovoltaics, pursuing morphology control and solar cell stability. For this purpose, two types of poly(3-alkylthiophene) random copolymers, incorporating different amounts (10/30/50%) of ester-functionalized side chains, were efficiently synthesized using the Rieke method. The solar cell performance of the functionalized copolymers was evaluated and compared to the pristine P3HT:PCBM system. It was observed that the physicochemical and opt…

Advances in Perovskite Solar Cells.

Organolead halide perovskite materials possess a combination of remarkable optoelectronic properties, such as steep optical absorption edge and high absorption coefficients, long charge carrier diffusion lengths and lifetimes. Taken together with the ability for low temperature preparation, also from solution, perovskite-based devices, especially photovoltaic (PV) cells have been studied intensively, with remarkable progress in performance, over the past few years. The combination of high efficiency, low cost and additional (non-PV) applications provides great potential for commercialization. Performance and applications of perovskite solar cells often correlate with their device structures…

Electrothermal Feedback and Absorption-Induced Open-Circuit-Voltage Turnover in Solar Cells

A solar panel gets hot as it works up on the roof, yet photoinduced self-heating is often ignored when characterizing lab-sized samples. The authors present their understanding of the turnover effect in measurements of open-circuit voltage versus light intensity (Suns-${V}_{O\phantom{\rule{0}{0ex}}C}$ curves), which is identified as a unique feature of all semiconductor-based solar cells. This effect is explained in terms of electrothermal feedback arising when the incident irradiation heats up the device. The authors' model fully explains the experimental data, and allows one to determine key device parameters such as the ideality factor and the band gap from a single measurement.

Dry Mechanochemical Synthesis of Highly Luminescent, Blue and Green Hybrid Perovskite Solids

A simple method to obtain bright photoluminescent wide bandgap mixed‐halide 3D perovskites is reported. The materials are prepared by dry mechanochemical synthesis (ball‐milling) starting from neat binary precursors, and show enhanced photoluminescence upon the addition of an adamantane derivative in the precursors' mixture. The structural characterization suggests that the additive does not participate in the crystal structure of the perovskite, which remains unvaried even with high loading of amantadine hydrochloride. By simple stoichiometric control of the halide precursors, the photoluminescence can be finely tuned from the UV to the green part of the visible spectrum. Photoluminescence…

Vapor Phase Deposited Single Junction and Tandem Perovskite Solar Cells.

Correlating the Lifetime and Fluorine Content of Iridium(III) Emitters in Green Light-Emitting Electrochemical Cells

In light-emitting electrochemical cells, the lifetime of the device is intrinsically linked to the stability of the phosphorescent emitter. In this study, we present a series of ionic iridium(III) emitters based on cyclometalating phenylpyridine ligands whose fluorine substituents are varied in terms of position and number. Importantly, despite these structural modifications, the emitters exhibit virtually identical electrochemical and spectroscopic properties, which allows for proper comparison in functional devices. Quantum chemical calculations support the properties measured in solution and suggest great similarities regarding the electronic structures of the emitters. In electrolumines…

Efficient Photo- and Electroluminescence by Trap States Passivation in Vacuum-Deposited Hybrid Perovskite Thin Films

Methylammonium lead iodide (MAPI) has excellent properties for photovoltaic applications, although it typically shows low photoluminescence quantum yield. Here, we report on vacuum-deposited MAPI perovskites obtained by modifying the methylammonium iodide (MAI) to PbI2 ratio during vacuum deposition. By studying the excitation density dependence of the photoluminescence lifetime, a large concentration of trap states was deduced for the stoichiometric MAPI films. The use of excess MAI during vacuum processing is capable of passivating these traps, resulting in luminescent films which can be used to fabricate planar light-emitting diodes with quantum efficiency approaching 2%.

Can we use time-resolved measurements to get Steady-State Transport data for Halide perovskites?

Time-resolved, pulsed excitation methods are widely used to deduce optoelectronic properties of semiconductors, including now also Halide Perovskites (HaPs), especially transport properties. However, as yet, no evaluation of their amenability and justification for the use of the results for the above-noted purposes has been reported. To check if we can learn from pulsed measurement results about steady-state phototransport properties, we show here that, although pulsed measurements can be useful to extract information on the recombination kinetics of HaPs, great care should be taken. One issue is that no changes in the material are induced during or as a result of the excitation, and anothe…

Efficient Perovskite Light-Emitting Diodes: Effect of Composition, Morphology, and Transport Layers

Organic-inorganic metal halide perovskites are emerging as novel materials for light-emitting applications due to their high color purity, band gap tunability, straightforward synthesis, and inexpensive precursors. In this work, we improve the performance of three-dimensional perovskite light-emitting diodes (PeLEDs) by tuning the emissive layer composition and thickness and by using small-molecule transport layers. Additionally, we correlate PeLED efficiencies to the perovskite structure and morphology. The results show that the PeLEDs containing perovskites with an excess of methylammonium bromide (MABr) to lead bromide (PbBr2) in a 2:1 ratio and a layer thickness of 80 nm have the highes…

Semitransparent near-infrared Sn–Pb hybrid perovskite photodetectors

We report semitransparent NIR perovskite photodetectors based on tin–lead hybrid perovskites, by using very thin film perovskite layers and transparent indium tin oxide electrodes.

Single-Source Vacuum Deposition of Mechanosynthesized Inorganic Halide Perovskites

Fully inorganic cesium lead halide perovskite thin films were prepared by an easy, fast and dry process based on single-source vacuum deposition. We investigated the structural and optical characteristics of the so-formed films as a function of chemical composition (chloride, bromide and iodide films were formed), post-deposition thermal annealing, as well as previous mechanosynthesis of perovskite powders. We found out that the CsPbX3 perovskite was preferentially formed for the smaller halides and favored by previous ball-milling of CsX and PbX2 precursors. When bigger halides were used and/or CsX and PbX2 precursors were simply mixed without previous mechanosynthesis, PbX2-rich compounds…

Effects of Masking on Open-Circuit Voltage and Fill Factor in Solar Cells

Guidelines for the correct measurement protocol of novel photovoltaic technologies such as perovskites are becoming more frequent in literature. This because, as will be confirmed in this perspective, it is not straightforward to correctly measure the efficiency parameters of these and many other novel solar cells. This is particularly the case for small area research devices which are prone to overestimate the short circuit current density, due to edge effects of various types. To reduce the inaccuracy of current density determination, the common recommended practice is to utilize masks with well‐defined apertures, often smaller than the device active area. Herein we show both experimental…

Ionic iridium complex and conjugated polymer used to solution-process a bilayer white light-emitting diode.

Bilayer white light-emitting devices are prepared from solution, using an ionic orange phosphorescent organometallic complex and a neutral fluorescent conjugated polymer. Because of the very different polarity of the two components, they dissolve in orthogonal solvents, allowing for the direct deposition of the blue emitter on top of the orange emitter without the need of cross-linking or special coating methodology. Fine tuning of the layer thickness of both light-emitting layers allows for the color tuning of different types of white light.

Ionic Space-Charge Effects in Solid State Organic Photovoltaics

The effect of mobile ions on the operation of donor-acceptor bilayer solar cells is studied. We demonstrate the large effect ions can have on the energetics of the solar cells, illustrated by (for instance) changing the output voltage of a cell in situ from 0.35 to 0.74 V. More importantly, it is shown ionic species do not obstruct the charge generating properties of the photovoltaic devices and ionic space charge can be used in situ to improve their efficiencies. The results obtained are explained by taking into account energetic changes at the donor-acceptor interface as well as built-in potentials, giving clear guidelines on how ionic species can offer many new and exciting functionaliti…

Hybrid Vapor-Solution Sequentially Deposited Mixed-Halide Perovskite Solar Cells

The recent sky-rocketing performance of perovskite solar cells has triggered a strong interest in further upgrading the fabrication techniques to meet the scalability requirements of the photovoltaic industry. The integration of vapor-deposition into the solution process in a sequential fashion can boost the uniformity and reproducibility of the perovskite solar cells. Besides, mixed-halide perovskites have exhibited outstanding crystallinity as well as higher stability compared with iodide-only perovskite. An extensive study was carried out to identify a reproducible process leading to highly crystalline perovskite films that when integrated into solar cells exhibited high power conversion…

Effect of conductivity of hole injection layer on the performance of a blue light emitting solution processable OLED

The performance of blue emitting OLED devices, using a polyspiro as blue light emitting polymer, were studied as a function of the conductivity of a novel hybrid hole injection material. The hole injection material is based on a polyarylamine using a molecular magnet as oxidant. The charge density and the luminance of the devices changed considerably with increasing conductivity of the hole injection layer. The change in device performance can be attributed to a change from a hole limited device to a balanced charge carrier device and eventually to an electron limited device. The performance of the optimized device configuration is significantly improved with respect to a device making use …

Advances in solution-processed near-infrared light-emitting diodes

A summary of recent advances in the near-infrared light-emitting diodes that are fabricated by solution-processed means, with coverage of devices based on organic semiconductors, halide perovskites and colloidal quantum dots.

Perovskite solar cells join the major league

Just six years after their discovery, organolead halide perovskite solar cells have taken the lead among emergent photovoltaic (PV) technologies, thanks to the demonstration of power conversion efficiencies (PCEs) of up to 20% ( 1 , 2 ). The perovskite precursor compounds are abundant and inexpensive and can easily be converted into thin films. Perovskite photovoltaics can therefore, in principle, generate electricity at a very low cost. However, high efficiencies have been limited to very small devices. On page 944 of this issue, Chen et al. ( 3 ) report perovskite solar cells of 1 cm2 with a certified efficiency of 15%.

Low-dimensional non-toxic A 3 Bi 2 X 9 compounds synthesized by a dry mechanochemical route with tunable visible photoluminescence at room temperature

We have synthesized fifteen inorganic and hybrid organic-inorganic non-toxic A3Bi2X9 compounds (A = K+, Rb+, Cs+, CH3NH3+ and HC(NH2)2+; X = I−, Br−, Cl−) through dry mechanochemistry. We demonstrate that this synthetic method is very well suited to prepare compounds from poorly soluble precursors, allowing thus the preparation of so far unreported compounds. X-ray diffraction analysis demonstrates the high crystallinity of the so-formed ternary bismuth halides. Furthermore, we show that, through substitution of the A-cation and X-anion, the bandgap of these compounds can be tuned to absorb throughout the whole visible spectrum. As-prepared powders of Cs3Bi2Br9 and Cs3Bi2I9 without any pass…

Segregation of lipid in Ir-dye/DMPA mixed monolayers as strategy to fabricate 2D supramolecular nanostructures at the air–water interface

A novel pseudospherical fluorinated iridium(III) derivative, Ir-dye/PF6, [Ir(F2-ppy)2(bpy)]PF6 (F2-ppy = 2-(2,4-difluoro)phenylpyridine, bpy = 2,2′-bipyridine), has been organized by using a lipid matrix, DMPA (dimyristoyl-phosphatidic acid), in several molar ratios at the air–water interface. The molecular organization of both components and the degree of miscibility in the different mixed films have been inferred by surface techniques such as π–A isotherms, ellipsometry, reflection spectroscopy, Brewster angle microscopy (BAM), and IR spectroscopy for the LB films, additionally the results have been discussed according to the additivity rule. The equimolecular Ir-dye/DMPA mixture leads to…

Pulsed-current versus constant-voltage light-emitting electrochemical cells with trifluoromethyl-substituted cationic iridium(iii) complexes

We report on five cationic iridium(III) complexes with cyclometalating 2-(3′-trifluoromethylphenyl)pyridine and a diimine, [(C⁁N)2Ir(N⁁N)](PF6), N⁁N = 4,4′-R2-2,2′-dipyridyl or 4,7-R2-1,10-phenanthroline (R = H, Me, tert-Bu, Ph), and characterize three of them by crystal structure analysis. The complexes undergo oxidation of the Ir–aryl fragment at 1.13–1.16 V (against ferrocene couple) and reduction of the N⁁N ligand at −1.66 V to −1.86 V, and have a redox gap of 2.84–2.99 V. The complexes exhibit bluish-green to green-yellow phosphorescence in an argon-saturated dichloromethane solution at room temperature with a maximum at 486–520 nm, quantum yield of 61–67%, and an excited-state lifetim…

Impact of the use of sterically congested Ir(III) complexes on the performance of light-emitting electrochemical cells

International audience; The synthesis, structural and optoelectronic characterization of a family of sterically congested cyclometalated cationic Ir(iii) complexes of the form [Ir(C^N)2(dtBubpy)]PF6 (with dtBubpy = 4,4′-di-tert-butyl-2,2′-bipyridine and C^N = a cyclometalating ligand decorated at the 4-position of the pyridine ring and/or the 3-position of the phenyl ring with a range of sterically bulky substituents) are reported. This family of complexes is compared to the unsubstituted analogue complex R1 bearing 2-phenylpyridinato as cyclometalating ligand. The impact of sterically bulky substituents on the C^N ligands on both the solid state photophysics and light-emitting electrochemi…

Archetype Cationic Iridium Complexes and Their Use in Solid-State Light-Emitting Electrochemical Cells

The archetype ionic transition-metal complexes (iTMCs) [Ir(ppy)2(bpy)][PF6] and [Ir(ppy)2(phen)][PF6], where Hppy = 2-phenylpyridine, bpy = 2,2'-bipyridine, and phen = 1,10-phenanthroline, are used as the primary active components in light-emitting electrochemical cells (LECs). Solution and solid-state photophysical properties are reported for both complexes and are interpreted with the help of density functional theory calculations. LEC devices based on these archetype complexes exhibit long turn-on times (70 and 160 h, respectively) and low external quantum efficiencies (~ 2%) when the complex is used as a pure film. The long turn-on times are attributed to the low mobility of the counter…

Combinatorial Vacuum-Deposition of Wide Bandgap Perovskite Films and Solar Cells

The development of vacuum-deposited perovskite materials and devices is partially slowed down by the minor research effort in this direction, due to the high cost of the required research tools. But there is also another factor, thermal co-deposition in high vacuum involves the simultaneous sublimation of several precursors with an overall deposition rate in the range of few Å s−1 . This leads to a deposition time of hours with only a single set of process parameters per batch, hence to a long timeframe to optimize even a single perovskite composition. Here we report the combinatorial vacuum deposition of wide bandgap perovskites using 4 sources and a non-rotating sample holder. By using sm…

Two are not always better than one: ligand optimisation for long-living light-emitting electrochemical cells

The complex [Ir(ppy)2(dpbpy)][PF6] (Hppy = 2-phenylpyridine, dpbpy = 6,6'-diphenyl-2,2'-bipyridine) has been prepared and evaluated as an electroluminescent component for light-emitting electrochemical cells (LECs); the complex exhibits two intramolecular face-to-face π-stacking interactions and long-lived LECs have been constructed; the device characteristics are not significantly improved in comparison to analogous LECs with 6-phenyl-2,2'-bipyridine. Costa Riquelme, Ruben Dario, Ruben.Costa@uv.es ; Orti Guillen, Enrique, Enrique.Orti@uv.es ; Bolink, Henk, Henk.Bolink@uv.es

Trap-Assisted Non-Radiative Recombination in Organic-Inorganic Perovskite Solar Cells

Molecular Iodine for a General Synthesis of Binary and Ternary Inorganic and Hybrid Organic-inorganic Iodide Nanocrystals

We report the synthesis of various binary and ternary inorganic and hybrid organic–inorganic iodide nanocrystals (NCs) starting from molecular iodine (I2). The synthesis described herein utilizes a reaction between I2 and oleylamine, which results in oleylammonium iodide, an iodide precursor that can be directly used in the preparation of iodide-based NCs. The generality of the synthesis was demonstrated by synthesizing KI, RbI, CsI, AgI, CsPbI3, FAPbI3, Cs4PbI6, Cs3Bi2I9, FA3Bi2I9, and RbAg4I5 NCs. Furthermore, the syntheses are facile and are carried out in vials heated on a hot plate in air. They exhibit not only narrow size distributions, but also, in the case of lead-based perovskites …

Conductive Hybrid Films of Polyarylamine Electrochemically Oxidized with the Molecular Nanomagnet [Mn12O12(H2O)4-(C6F5COO)16]

Simple, Fast, Bright, and Stable Light Sources

In this work we show that solution-processed light-emitting electrochemical cells (LECs) based on only an ionic iridium complex and a small amount of ionic liquid exhibit exceptionally good performances when applying a pulsed current: sub-second turn-on times and almost constant high luminances (>600 cd m(-2) ) and power efficiencies over the first 600 h. This demonstrates the potential of LECs for applications in solid-state signage and lighting.

Fullerene imposed high open-circuit voltage in efficient perovskite based solar cells

Five different commercially available fullerenes are evaluated as hole blocking/electron transporting materials in p–i–n methylammonium lead iodide perovskite solar cells using a vacuum deposited perovskite absorber layer. A significant enhancement of the solar cell performance can be obtained by selecting a suitable fullerene derivative. Open-circuit voltages as high as 1.11 volts are obtained leading to a power conversion efficiency of 14.6%.

Polymer solar cells based on diphenylmethanofullerenes with reduced sidechain length

Diphenylmethanofullerenes (DPMs) show interesting properties as acceptors in polymer bulk heterojunction solar cells due to the high open circuit voltages they generate compared to their energy levels. Here we investigate the effect of reducing the alkane sidechain length of the DPMs from C12 to C6 in the properties of the solar cell. This change leads to an increase in the electron mobility, thus allowing for a lower fullerene content, which in turn results in an increase in the short circuit current and, finally, in an increase in the efficiency of the device (from 2.3 to 2.6%) due to the higher concentration of the more absorbing polymer in the film. Atomic force microscopy images and ex…

Bis-Sulfone- and Bis-Sulfoxide-Spirobifluorenes: Polar Acceptor Hosts with Tunable Solubilities for Blue-Phosphorescent Light-Emitting Devices

Bis-sulfone- and bis-sulfoxide-spirobifluorenes are a promising class of high-triplet-energy electron-acceptor hosts for blue phosphorescent light-emitting devices. The molecular design and synthetic route are simple and facilitate tailoring of the solubilities of the host materials without lowering the high-energy triplet state. The syntheses and characterization (including single-crystal structures) of four electron-accepting hosts are reported; the trend in their reduction potentials is consistent with the electron-withdrawing nature of the sulfone or sulfoxide substituents. Emission maxima of 421–432 nm overlap with the MLCT absorption of the sky-blue emitter bis(4,6-difluorophenyl-pyri…

Light-emitting electrochemical cells and solution-processed organic light-emitting diodes using small molecule organic thermally activated delayed fluorescence emitters

EZ-C thanks the University of St Andrews for support. The authors are grateful to the EPSRC for financial support (grants EP/J01771X and EP/J00916). IDWS is a Royal Society Wolfson Research Merit Award Holder. Two novel charged organic thermally activated delayed fluorescence (TADF) emitters, 1 and 2, have been synthesized. Their TADF behavior is well-supported by the multiexponential decay of their emission (nanosecond and microsecond components) and the oxygen dependence of the photoluminescence quantum yields. Spin-coated electroluminescent devices have been fabricated to make light-emitting electrochemical cells (LEECs) and organic light-emitting diodes (OLEDs). The first example of a n…

CF3 Substitution of [Cu(P^P)(bpy)][PF6 ] Complexes: Effects on Photophysical Properties and Light-Emitting Electrochemical Cell Performance

Herein, [Cu(P^P)(N^N)][PF6 ] complexes (P^P=bis[2-(diphenylphosphino)phenyl]ether (POP) or 4,5-bis(diphenylphosphino)-9,9-dimethylxanthene (xantphos); N^N=CF3 -substituted 2,2'-bipyridines (6,6'-(CF3 )2 bpy, 6-CF3 bpy, 5,5'-(CF3 )2 bpy, 4,4'-(CF3 )2 bpy, 6,6'-Me2 -4,4'-(CF3 )2 bpy)) are reported. The effects of CF3 substitution on their structure as well as their electrochemical and photophysical properties are also presented. The HOMO-LUMO gap was tuned by the N^N ligand; the largest redshift in the metal-to-ligand charge transfer (MLCT) band was for [Cu(P^P){5,5'-(CF3 )2 bpy}][PF6 ]. In solution, the compounds are weak yellow to red emitters. The emission properties depend on the substitu…

Trap-limited mobility in space-charge limited current in organic layers

Space-charge limited current transport in organic devices, relevant to the operation of a range of organic optoelectronic devices, is analyzed in the frequency domain. The classical multiple trapping picture with one transport state and one trap level is used as the basis for the descriptions. By varying the energetic and kinetic properties of the traps, we show that the admittance and the capacitance spectra are considerably modified depending on the interplay between the trap-limited mobility and the trap kinetics. We point out that capacitance steps at low-frequency, usually found in experiments, are observed only for slow traps. © 2008 Elsevier B.V. All rights reserved.

Engineering Charge Injection Interfaces in Hybrid Light-Emitting Electrochemical Cells

Light-emitting electrochemical cells (LECs) consists of a thin film of an ionic organic semiconductor sandwiched between two electrodes. Because of the large density of ions, LECs are often reported to perform independently on the electrodes work function. Here we use metal oxides as charge injection layers and demonstrate that, although electroluminescence is observed independently of the electrodes used, the device performances are strongly dependent on the choice of the interface materials. Relying on metal oxide charge injection layers, such hybrid devices are of interest for real lighting applications and could pave the way for new efficient, stable, low-cost lighting sources.

Light-emitting fabrics

Light-emitting fibres that suit integration with textiles are prepared by dip-coating a steel wire with an electroluminescent material and then cleverly wrapping the structure with a carbon nanotube sheet that functions as a transparent electrode.

Intramolecular pi-stacking in a phenylpyrazole-based iridium complex and its use in light-emitting electrochemical cells.

A novel iridium(III) complex, [Ir(dmppz)(2)pbpy][PF(6)] (Hdmppz = 3,5-dimethyl-1-phenylpyrazole and pbpy = 6-phenyl-(2,2'-bipyridine)), is reported. The complex shows an intramolecular face-to-face pi-stacking between the phenyl ring of the dmppz ligand and the pendant phenyl of the pbpy ligand. This interaction provides a supramolecular cage formation that holds also in the excited states. Light-emitting electrochemical cells (LECs) using the novel complex show extraordinary lifetimes of approximately 2000 h. The high stability is favored by the presence of pendant methyl groups on the dmppz ligands that hinder the entrance of water molecules rendering the degradation of the complex more d…

Tuning the Optical Absorption of Sn-, Ge-, and Zn-Substituted Cs2AgBiBr6 Double Perovskites: Structural and Electronic Effects

Lead-free halide double perovskites (DPs) are highly tunable materials in terms of chemical composition and optical properties. One of the most widely reported DPs is Cs2AgBiBr6, which is envisaged as a promising absorber for photovoltaics. Nevertheless, its bandgap (around 1.9−2.3 eV) remains too large for common tandem solar cells. In this work, we report the mechanochemical synthesis of Sn-, Ge-, and Zn-substituted Cs2AgBiBr6 in powder form; their bandgaps reach 1.55, 1.80, and 2.02 eV, respectively. These differences are rationalized through density functional theory calculations, demonstrating combined electronic and structural (disorder) effects introduced by the divalent metal-cation…

Solid-State Lighting: Simple, Fast, Bright, and Stable Light Sources (Adv. Mater. 7/2012)

Soret emission from water-soluble porphyrin thin films: effect on the electroluminescence response

The emission properties of TSPP [tetrakis(4-sulfonatophenyl) porphyrin] and TMPyP [tetrakis(4-methylpyridyl) porphyrin] in thin films, prepared both by the Langmuir–Blodgett technique and the spin-coating method, have been investigated. Surprisingly, in most of the samples analyzed, the emission spectra do not show the usual two bands typical of porphyrins (in the region 650–750 nm), and depend strongly on the excitation energy. The origin of a new emission band detected at ∼480–500 nm is discussed in terms of the nature of the porphyrin aggregates. Moreover, we demonstrate that the presence or absence of this band in the fluorescence spectrum is directly related to the generation of electr…

Chloride ion impact on materials for light-emitting electrochemical cells

Small quantities of Cl(-) ions result in dramatic reductions in the performance of ionic transition metal complexes in light-emitting electrochemical cells. Strong ion-pairing between aromatic protons and chloride has been established in both the solid state and solution. X-ray structural determination of 2{[Ir(ppy)2(bpy)][Cl]}·2CH2Cl2·[H3O]·Cl reveals the unusual nature of an impurity encountered in the preparation of [Ir(ppy)2(bpy)][PF6].

[Cu(P^P)(N^N)][PF6] compounds with bis(phosphane) and 6-alkoxy, 6-alkylthio, 6-phenyloxy and 6-phenylthio-substituted 2,2'-bipyridine ligands for light-emitting electrochemical cells

We report a series of [Cu(P^P)(N^N)][PF6] complexes with P^P = bis(2-(diphenylphosphino)phenyl)ether (POP) or 4,5-bis(diphenylphosphino)-9,9-dimethylxanthene (xantphos) and N^N = 6-methoxy-2,2′-bipyridine (MeObpy), 6-ethoxy-2,2′-bipyridine (EtObpy), 6-phenyloxy-2,2′-bipyridine (PhObpy), 6-methylthio-2,2′-bipyridine (MeSbpy), 6-ethylthio-2,2′-bipyridine (EtSbpy) and 6-phenylthio-2,2′-bipyridine (PhSbpy). The single crystal structures of all twelve compounds have been determined and confirm chelating modes for each N^N and P^P ligand, and a distorted tetrahedral geometry for copper(I). For the xantphos-containing complexes, the asymmetrical bpy ligand is arranged with the 6-substituent lying …

Degradation mechanisms in organic lead halide perovskite light-emitting diodes

Organic–inorganic metal halide perovskites have attracted significant attention for low-cost, high-efficiency, color-pure light-emitting applications. However, as seen in many reports so-far, perovskite light-emitting diodes (PeLED) suffer from poor operational lifetime, limiting their practical use. The underlying degradation mechanism is a topic of crucial importance. Here, the degradation mechanisms of methylammonium lead bromide based PeLED are investigated. When the PeLED is electrically biased, there is an initial raise in the luminance followed by a rapid reduction in luminance and current density. Microscopic studies reveal the formation of micrometer-sized spots that are photolumin…

Single Molecule Solid State Light Emitting Electrochemical Cells with Lifetimes Superior to 3000 Hours

Air stable hybrid organic-inorganic light emitting diodes using ZnO as the cathode

An air stable hybrid organic-inorganic light emitting device is presented. This architecture makes use of metal oxides as charge injecting materials into the light emitting polymer, avoiding the use of air sensitive cathodes commonly employed in organic light emitting diode manufacturing. We report the application of zinc oxide as a cathode in an organic light emitting device. This electroluminescent device shows high brightness levels reaching 6500 cd/m2 at voltages as low as 8 V. Compared to a conventional device using low workfunction metal cathodes, our device shows a lower turn-on voltage and it can operate in air.

Exceptionally long-lived light-emitting electrochemical cells: multiple intra-cation π-stacking interactions in [Ir(C^N)2(N^N)][PF6] emitters

A series of cyclometalated iridium(iii) complexes [Ir(C^N)2(N^N)][PF6] (N^N = 2,2′-bipyridine (1), 6-phenyl-2,2′-bipyridine (2), 4,4′-di-tert-butyl-2,2′-bipyridine (3), 4,4′-di-tert-butyl-6-phenyl-2,2′-bipyridine (4); HC^N = 2-(3-phenyl)phenylpyridine (HPhppy) or 2-(3,5-diphenyl)phenylpyridine (HPh2ppy)) are reported. They have been synthesized using solvento precursors so as to avoid the use of chlorido-dimer intermediates, chloride ion contaminant being detrimental to the performance of [Ir(C^N)2(N^N)][PF6] emitters in light-electrochemical cell (LEC) devices. Single crystal structure determinations and variable temperature solution 1H NMR spectroscopic data confirm that the pendant pheny…

Temperature Effect of Ionic Transition Metal Complex Light-Emitting Electrochemical Cells

ABSTRACTLight-Emitting Electrochemical Cells (LECs) consist of solution processable ionic light-emitting materials and use air stable electrodes. Their operational mechanism relies on both ionic and electronic conduction. The dynamic behavior is primarily determined by the ionic conductivity. Here, we demonstrate that with increasing temperature the LECs turn-on faster yet without decreasing the efficiency. This is due to the activation energy of ionic transport and the temperature independent photoluminescence quantum yields.

Perovskite Solar Cells: Stable under Space Conditions

Metal halide perovskite solar cells (PSCs) are of interest for high altitude and space applications due to their lightweight and versatile form factor. However, their resilience toward the particle spectrum encountered in space is still of concern. For space cells, the effect of these particles is condensed into an equivalent 1 MeV electron fluence. The effect of high doses of 1 MeV e-beam radiation up to an accumulated fluence to 10^16 e-cm-2 on methylammonium lead iodide perovskite thin films and solar cells is probed. By using substrate and encapsulation materials that are stable under the high energy e-beam radiation, its net effect on the perovskite film and solar cells can be studied.…

High voltage vacuum-deposited CH3NH3PbI3-CH3NH3PbI3 tandem solar cells

The recent success of perovskite solar cells is based on two solid pillars: the rapid progress of their power conversion efficiency and their flexibility in terms of optoelectrical properties and processing methods. That versatility makes these devices ideal candidates for multi-junction photovoltaics. We report an optically optimized double junction CH3NH3PbI3–CH3NH3PbI3 tandem solar cell where the matched short-circuit current is maximized while parasitic absorption is minimized. The use of an additive vacuum-deposition protocol allows us to reproduce calculated stack designs, which comprise several charge selective materials that ensure appropriate band alignment and charge recombination…

Perovskite-Perovskite Homojunctions via Compositional Doping.

One of the most important properties of semiconductors is the possibility of controlling their electronic behavior via intentional doping. Despite the unprecedented progress in the understanding of hybrid metal halide perovskites, extrinsic doping of perovskite remains nearly unexplored and perovskite–perovskite homojunctions have not been reported. Here we present a perovskite–perovskite homojunction obtained by vacuum deposition of stoichiometrically tuned methylammonium lead iodide (MAPI) films. Doping is realized by adjusting the relative deposition rates of MAI and PbI2, obtaining p-type (MAI excess) and n-type (MAI defect) MAPI. The successful stoichiometry change in the thin films is…

Room temperature vacuum-deposition of CsPbI2Br perovskite films from multiple-sources and mixed halide precursors

Fully inorganic cesium lead halide perovskites, such as CsPbI2Br, show enhanced thermal stability compared to hybrid ones and are being widely investigated as wide bandgap absorbers for tandem applications. Despite their simple stoichiometry, the preparation of highly crystalline and stable cesium lead halide thin films is not trivial. In general, high-efficiency solar cells based on solution-processed CsPbI2Br thin films are prepared by hightemperature annealing or the use of chemical additives. In this work, we use solvent-free synthesis to investigate the formation of CsPbI2Br in bulk or in thin films via mechanochemical synthesis and multiple-source vacuum deposition, respectively. We d…

Hovering solar cells

Ultrathin, flexible and lightweight perovskite solar cells with improved stability in air can now power model airplanes for several hours.

High Photoluminescence Quantum Yields in Organic Semiconductor-Perovskite Composite Thin Films.

One of the obstacles towards efficient radiative recombination in hybrid perovskites is a low exciton binding energy, typically in the orders of tens of meV. It has been shown that the use of electron-donor additives can lead to a substantial reduction of the non-radiative recombination in perovskite films. Herein, the approach using small molecules with semiconducting properties, which are candidates to be implemented in future optoelectronic devices, is presented. In particular, highly luminescent perovskite-organic semiconductor composite thin films have been developed, which can be processed from solution in a simple coating step. By tuning the relative concentration of methylammonium l…

Molecular organization of a water-insoluble iridium(III) complex in mixed monolayers.

Abstract In this work, organized mixed monolayers containing a cationic water-insoluble iridium(III) complex, Ir-dye, [Ir(ppy)2(tmphen)]PF6, (tmphen = 3,4,7,8-tetramethyl-1,10-phenanthroline, and ppy = 2-phenylpyridine), and an anionic lipid matrix, DMPA, dimyristoyl-phosphatidic acid, with different molar proportions, were formed by the co-spreading method at the air–water interface. The presence of the dye at the interface, as well as the molecular organization of the mixed films, is deduced from surface techniques such as π – A isotherms, Brewster angle microscopy (BAM) and reflection spectroscopy. The results obtained remark the formation of an equimolar mixed film, Ir-dye/DMPA = 1:1. B…

Meniscus coated high open-circuit voltage bi-layer solar cells

Neat bi-layer solar cells of a fullerene acceptor and a cyanine dye donor were prepared using meniscus coating. Meniscus coating is very material efficient and leads to high quality pinhole-free films. The cells exhibit high open circuit voltages of 1 volt, only 0.8 eV below the band gap of the cyanine dye. This is one of the smallest differences reported for organic solar cells and illustrates an almost optimal donor-acceptor energy level alignment.

Mixed Iodide-Bromide Methylammonium Lead Perovskite-based Diodes for Light Emission and Photovoltaics.

Vacuum deposition techniques are used to prepare mixed iodide–bromide methylammonium lead perovskite diodes via an intermediate double layer of the pure iodide and bromide perovskites. The diodes lead to bright electroluminescence, whose emission spectra maxima shift from the infrared toward the visible with increasing bromide content. When illuminated with AM1.5 simulated sunlight the devices function as efficient solar cells with power conversion efficiencies as high as 12.9%.

Hybrid organic-inorganic light emitting diodes: effect of the metal oxide

Hybrid organic-inorganic light emitting diodes (HyLEDs), employing metal oxides as the electron injecting contacts, are interesting as an alternative to OLEDs. Until recently, the metal oxide of choice was either titanium dioxide or zinc oxide. In this work two wide bandgap metal oxides, HfO2 and MgO, are employed as electron injecting layer in HyLEDs. It is demonstrated that both the current density and the luminance values obtained are directly related to the barriers for electron injection (from the ITO to the metal oxide) and for hole transfer to the same metal oxide, outlining a new design rule for the optimization of HyLEDs. Record device efficacies (3.3 cd/A, >10000 cd/m2) using the …

Efficient vacuum deposited p-i-n and n-i-p perovskite solar cells employing doped charge transport layers

Methylammonium lead halide perovskites have emerged as high performance photovoltaic materials. Most of these solar cells are prepared via solution-processing and record efficiencies (>20%) have been obtained employing perovskites with mixed halides and organic cations on (mesoscopic) metal oxides. Here, we demonstrate fully vacuum deposited planar perovskite solar cells by depositing methylammonium lead iodide in between intrinsic and doped organic charge transport molecules. Two configurations, one inverted with respect to the other, p-i-n and n-i-p, are prepared and optimized leading to planar solar cells without hysteresis and very high efficiencies, 16.5% and 20%, respectively. It is t…

Influence of doped charge transport layers on efficient perovskite solar cells

Planar vacuum deposited p–i–n methyl ammonium lead tri-iodide perovskite solar cells are prepared with different electron and hole transporting layers, either doped or undoped. The effect of these layers on the solar cells performance (efficiency and stability) is studied. The main benefit of using doped layers lies in the formation of barrier free charge extraction contacts to the electrodes. However, this comes at the cost of increased residual absorption (reducing the current density and efficiency of the cells) and a decreased stability. A generic solar cell structure using undoped charge extraction layers is presented, containing a thin layer of a strong electron acceptor in between th…

Phosphine Oxide Derivative as a Passivating Agent to Enhance the Performance of Perovskite Solar Cells

Defects of metal-halide perovskites detrimentally influence the optoelectronic properties of the thin film and, ultimately, the photovoltaic performance of perovskite solar cells (PSCs). Especially, defect-mediated nonradiative recombination that occurs at the perovskite interface significantly limits the power conversion efficiency (PCE) of PSCs. In this regard, interfacial engineering or surface treatment of perovskites has become a viable strategy for reducing the density of surface defects, thereby improving the PCE of PSCs. Here, an organic molecule, tris(5-((tetrahydro-2H-pyran-2-yl)oxy)pentyl) phosphine oxide (THPPO), is synthesized and introduced as a defect passivation agent in PSC…

Delayed Luminescence in Lead Halide Perovskite Nanocrystals

The mechanism responsible for the extremely long photoluminescence (PL) lifetimes observed in many lead halide perovskites is still under debate. While the presence of trap states is widely accepted, the process of electron detrapping back to the emissive state has been mostly ignored, especially from deep traps as these are typically associated with nonradiative recombination. Here, we study the photophysics of methylammonium lead bromide perovskite nanocrystals (PNCs) with a photoluminescence quantum yield close to unity. We show that the lifetime of the spontaneous radiative recombination in PNCs is as short as 2 ns, which is expected considering the direct bandgap character of perovskit…

[Cu(bpy)(P^P)]+ containing light-emitting electrochemical cells: improving performance through simple substitution

Light-emitting electrochemical cells (LECs) containing [Cu(POP)(N^N)][PF6] (POP = bis(2-diphenylphosphinophenyl)ether, N^N = 6-methyl- or 6,6′-dimethyl-2,2′-bipyridine) exhibit luminance and efficiency surpassing previous copper(i)-containing LECs.

Zero-Dimensional Hybrid Organic−Inorganic Lead Halides and Their Post-Synthesis Reversible Transformation into Three-Dimensional Perovskites

Zero-dimensional (0D) mixed-halide hybrid organic-inorganic MA4PbX6·2H2O (MA = CH3NH3+; X = Br1 - xIx with 0 < x < 1) has been synthesized by a solvent-free mechanochemical approach. It has been shown that this 0D phase with sharp absorption features in the near-UV is a hydrated structure, which can be reversibly transformed into the three-dimensional perovskite phase MAPbX3 by simple thermal annealing (dehydration) in air. This work reveals a new approach to hybrid organic-inorganic perovskites and related 0D structures, which have so far only been thoroughly studied for the inorganic Cs4PbX6 compounds. Hetero-structures for Efficient Luminescent Devices (HELD) REFERENCIA: 834431 PCIN-2019…

FAPb0.5Sn0.5I3: A Narrow Bandgap Perovskite Synthesized through Evaporation Methods for Solar Cell Applications

The tunability of the optoelectrical properties upon compositional modification is a key characteristic of metal halide perovskites. In particular, bandgaps narrower than those in conventional lead‐based perovskites are essential to achieve the theoretical efficiency limit of single‐absorber solar cells, as well as develop multijunction tandem devices. Herein, the solvent‐free vacuum deposition of a narrow bandgap perovskite based on tin-lead metal and formamidinium cation is reported. Pinhole‐free films with 1.28 eV bandgap are obtained by thermal codeposition of precursors. The optoelectrical quality of these films is demonstrated by their use in solar cells with a power conversion effici…

Enhancing the photoluminescence quantum yields of blue-emitting cationic iridium(iii) complexes bearing bisphosphine ligands

EZ-C acknowledges the University of St Andrews for financial support. We thank Johnson Matthey and Umicore AG for the gift of materials and Cihang Yu for the preparation of isopropxantphos. We thank Dr. Nail Shaveleev for the synthesis of NMS25. IDWS and AKB acknowledge support from EPSRC (EP/J01771X). This work has been supported by the Spanish Ministry of Economy and Competitiveness (MINECO) MAT2014-55200. Herein we present a structure-property relationship study of thirteen cationic iridium (III) complexes of the form of [Ir(C^N)2(P^P)]PF6 in both solution and the solid state through systematic evaluation of six bisphosphine (P^P) ligands (xantphos, dpephos, dppe, Dppe, nixantphos and is…

Fluorine-free blue-green emitters for light-emitting electrochemical cells

Date of Acceptance: 29/05/2014 There is presently a lack of efficient and stable blue emitters for light-emitting electrochemical cells (LEECs), which limits the development of white light emitting systems for lighting. Cyclometalated iridium complexes as blue emitters tend to show low photoluminescence efficiency due to significant ligand-centred character of the radiative transition. The most common strategy to blue-shift the emission is to use fluorine substituents on the cyclometalating ligand, such as 2,4-difluorophenylpyridine, dFppy, which has been shown to decrease the stability of the emitter in operating devices. Herein we report a series of four new charged cyclometalated iridium…

Assigning ionic properties in perovskite solar cells; a unifying transient simulation/experimental study

Kinetic modelling has proven to be essential to understand the time and spatial dependence of charge carriers in solar cells. Traditional drift–diffusion simulations have generally been employed to describe static steady-state conditions, whereas recently the transient counterpart has been able to reveal more detailed information regarding carrier kinetics. In addition to customary electron and hole dynamics, perovskite materials are known to also be strongly affected by the displacement of lattice vacancies, charged atoms or even entire molecules. Such ionic motion transpires on vastly different time scales compared to free charges and are generally not straightforward to simultaneously ac…

Ruthenium pentamethylcyclopentadienyl mesitylene dimer: a sublimable n-dopant and electron buffer layer for efficient n-i-p perovskite solar cells

Electron-transport materials such as fullerenes are widely used in perovskite solar cells to selectively transfer the photogenerated electrons to the electrodes. In order to minimize losses at the interface between the fullerene and the electrode, it is important to reduce the energy difference between the transport level of the two materials. A common approach to reduce such energy mismatch is to increase the charge carrier density in the semiconductor through doping. A variety of molecular dopants have been reported to reduce (n-dope) fullerenes. However, most of them are either difficult to process or extremely air sensitive, with most n-dopants leading to the formation of undesirable si…

An Ester-Substituted Iridium Complex for Efficient Vacuum-Processed Organic Light-Emitting Diodes

An orange-red-emitting iridium complex (N958) was prepared, and its photophysical and device-based characteristics were investigated. Despite N958 displaying quite poor photophysical properties in solution (acetonitrile), organic light-emitting diode (OLED) devices based on the complex exhibit an efficiency close to 10%.

Origin of the Enhanced Photoluminescence Quantum Yield in MAPbBr 3 Perovskite with Reduced Crystal Size

Methylammonium lead bromide perovskite (MAPbBr3) has been widely investigated for applications in visible perovskite light-emitting diodes (LEDs). Fine-tuning of the morphology and of the crystal size, from the microscale down to the quantum confinement regime, has been used to increase the photoluminescence quantum yield (PLQY). However, the physical processes underlying the PL emission of this perovskite remain unclear. Here, we elucidate the origin of the PL emission of polycrystalline MAPbBr3 thin films by different spectroscopic techniques. We estimate the exciton binding energy, the reduced exciton effective mass, and the trap density. Moreover, we confirm the coexistence of free carr…

Determination of electron and hole energy levels in mesoporous nanocrystalline TiO2 solid-state dye solar cell

A study of a hybrid heterojunction solar cell based on nanocrystalline mesoporous TiO2 and the hole conductor spiro-OMeTAD (2,2′7,7′-tetrakis(N,N′-di-p-methoxyphenyl-amine)-9,9′-spiro-bifluorene) has been realized. Impedance and cyclic voltammetry techniques were used to measure the interfacial properties of the hybrid heterojunction and establish the energy levels of the solid-state electrolyte. It was observed that the energy levels of the organic hole transport material are changed when it forms a film deposited onto indium-doped tin oxide (ITO). Moreover, the HOMO level of the mono oxidized spiro-OMeTAD is well coupled with the HOMO level of the dye N719 (Ru(4,4′-dicarboxy-2,2′-bipyridy…

Efficient Monolithic Perovskite/Perovskite Tandem Solar Cells

Thin-film solar cells suffer from various types of recombination, of which leakage current usually dominates at lower voltages. Herein, we demonstrate first a three-order reduction of the shunt loss mechanism in planar methylammonium lead iodide perovskite solar cells by replacing the commonly used hole transport layer poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) with a better hole-selective polyarylamine. As a result, these cells exhibit superior operation under reduced light conditions, which we demonstrate for the extreme case of moonlight irradiance, at which open-circuit voltages of 530 mV can still be obtained. By the shunt removal we also observe the VOC to dro…

Bis(arylimidazole) Iridium Picolinate Emitters and Preferential Dipole Orientation in Films

The straightforward synthesis and photophysical properties of a new series of heteroleptic iridium(III) bis(2-arylimidazole) picolinate complexes are reported. Each complex has been characterized by nuclear magnetic resonance, UV-vis, cyclic voltammetry, and photoluminescent angle dependency, and the emissive properties of each are described. The preferred orientation of transition dipoles in emitter/host thin films indicated more preferred orientation than homoleptic complex Ir(ppy)3.

Enamine-based hole transporting materials for vacuum-deposited perovskite solar cells

In a short period of time, the rapid development of perovskite solar cells attracted a lot of attention in the science community with the record for power conversion efficiency being broken every year. Despite the fast progress in power conversion efficiency there are still many issues that need to be solved before starting large scale commercial applications, such as, among others, the difficult and costly synthesis and usage of toxic solvents for the deposition of hole transport materials (HTMs). We herein report new enamine-based charge transport materials obtained via a simple one step synthesis procedure, from commercially available precursors and without the use of expensive organomet…

Guideline for Optical Optimization of Planar Perovskite Solar Cells

Organometallic halide perovskite solar cells have emerged as a versatile photovoltaic technology with soaring efficiencies. Planar configuration in particular, has been a structure of choice thanks to its lower temperature processing, compatibility with tandem solar cells and potential in commercialization. Despite all the breakthroughs in the field, the optical mechanisms leading to highly efficient perovskite solar cells lack profound insight. In this paper, a comprehensive guideline is introduced involving semi-analytical equations for thickness optimization of the front and rear transport layers, perovskite, and transparent conductive oxides to improve the antireflection and light trapp…

Front Cover: CF3 Substitution of [Cu(P^P)(bpy)][PF6 ] Complexes: Effects on Photophysical Properties and Light-Emitting Electrochemical Cell Performance (ChemPlusChem 4/2018)

Deep-blue thermally activated delayed fluorescence (TADF) emitters for light-emitting electrochemical cells (LEECs)

The authors acknowledge the University of St Andrews for financial support. The authors also acknowledge financial support from the European Union H2020 project INFORM (grant 675867), the Spanish Ministry of Economy and Competitiveness (MINECO) via the Unidad de Excelencia María de Maeztu MDM-2015-0538, MAT2014-55200 and the Generalitat Valenciana (Prometeo/2016/135). MLP acknowledges support from a Grisolia grant (GRISOLIA/2015/A/146). Two deep blue thermally activated delayed fluorescence (TADF) emitters ( imCzDPS and imDPADPS ) that contain charged imidazolium groups tethered to the central luminophore were designed and synthesized as small molecule organic emitters for light-emitting e…

Highly luminescent perovskite–aluminum oxide composites

In this communication we report on the preparation of CH3NH3PbBr3 perovskite/Al2O3 nanoparticle composites in a thin film configuration and demonstrate their high photoluminescence quantum yield. The composite material is solution-processed at low temperature, using stable alumina nanoparticle dispersions. There is a large influence of the alumina nanoparticle concentration on the perovskite morphology and on its photoluminescence.

Hansen theory applied to the identification of nonhazardous solvents for hybrid perovskite thin-films processing

Abstract Metal-halide perovskites have become the most studied material for efficient next-generation solar cells, in part because of the possibility of depositing high quality semiconducting perovskites by simple solution-based methods. However, the majority of solvent systems implemented in literature for deposition of lead halide perovskites are hazardous to handle. Investigation of alternatives perovskite processing methods are hence key to safely upscale the perovskite photovoltaic manufacturing. In this manuscript we use the Hansen theory to find suitable nonhazardous solvents to solubilize two lead salts, PbBr2 and PbI2, used to fabricate the corresponding methylammonium (MA) lead ha…

Influence of mobile ions on the electroluminescence characteristics of methylammonium lead iodide perovskite diodes

In this work, we study the effect of voltage bias on the optoelectronic behavior of methylammonium lead iodide planar diodes. Upon biasing the diodes with a positive voltage, the turn-on voltage of the electroluminescence diminishes and its intensity substantially increases. This behavior is reminiscent of that observed in light-emitting electrochemical cells (LECs), single-layer electroluminescent devices in which the charge injection is assisted by the accumulation of ions at the electrode interface. Because of this mechanism, performances are largely independent from the work function of the electrodes. The similarities observed between planar perovskite diodes and LECs suggest that mobi…

Efficient light-emitting electrochemical cells using small molecular weight, ionic, host-guest systems

This work has been supported by the Spanish Ministry of Economy and Competitiveness (MAT2014-55200). Light-emitting electrochemical cells (LECs) based on fluorescent host-guest small molecules system are reported. The LECs show electroluminescence coming solely from the guest, with an external quantum efficiency (EQE) of 2.0%, which is very close to the theoretical maximum EQE (2.2%) for this particular system. This work demonstrates the possibility to obtain high efficiency devices employing low-cost materials, making host-guest systems a real alternative to more traditional semiconducting polymer or transition metal compounds. Postprint Peer reviewed

Efficient electroluminescence from a perylenediimide fluorophore obtained from a simple solution processed OLED

Simple solution processed organic light emitting diodes are used to screen the performance of two types of highly efficient, narrow band red emitting fluorescent perylenediimides (PDIs). PDIs substituted at the diimide positions seem to form aggregates in the thin film architecture as evidenced by the shifted electroluminescent spectrum. When substituted on the bay position and when used both as the emitting and the electron transporting specie, bright electroluminescence with a narrow width around 610 nm reaching 500 cd m−2 at moderate voltages was observed, demonstrating the usefulness of these fluorophores for OLED applications.

Luminescent Ionic Transition-Metal Complexes for Light-Emitting Electrochemical Cells

Higher efficiency in the end-use of energy requires substantial progress in lighting concepts. All the technologies under development are based on solid-state electroluminescent materials and belong to the general area of solid-state lighting (SSL). The two main technologies being developed in SSL are light-emitting diodes (LEDs) and organic light-emitting diodes (OLEDs), but in recent years, light-emitting electrochemical cells (LECs) have emerged as an alternative option. The luminescent materials in LECs are either luminescent polymers together with ionic salts or ionic species, such as ionic transition-metal complexes (iTMCs). Cyclometalated complexes of Ir(III) are by far the most util…

Dimensionality Controls Anion Intermixing in Electroluminescent Perovskite Heterojunctions.

Metal halide perovskites have emerged as a promising group of materials for optoelectronic applications such as photovoltaics, light emission, and photodetectors. So-far, in particular, the stability of light-emitting devices is limited, which is in part attributed to the intrinsic ionic conductivity of these materials. High-performance devices inevitably contain heterojunctions similar to other optoelectronic devices based on oxide perovskites, II-VI, or III-V group semiconductors. To enable efficient heterojunctions, ion exchange at the interface between different layers should be controlled. Herein, we report a method that enables to control and monitor the extent of anion intermixing be…

Low Temperature, Vacuum-Processed Bismuth Triiodide Solar Cells with Organic Small-Molecule Hole Transport Bilayer

Herein, the preparation of fully vacuum-processed bismuth triiodide solar cells with low annealing temperature is reported. Planar n-i-p devices are prepared using a thin compact SnO2 layer as the electron extraction layer and an electron blocking/hole extraction bilayer consisting of an intrinsic and doped organic hole-transport molecule. Using this configuration, herein, higher fill-factors and overall power conversion efficiencies than with conventional solution-processed hole transport materials are achieved.

Pyridine-Incorporated Dihexylquaterthiophene: A Novel Blue Emitter for Organic Light Emitting Diodes (OLEDs)

The synthesis and characterisation of 2,5-bis(5′-hexyl-[2,2′-bithiophen]-5-yl)pyridine (Th4PY) and its use as a blue emitter in organic light emitting diodes (OLEDs) is reported. Th4PY was synthesised in high yield using a straightforward Suzuki coupling route with commercially available starting materials. As Th4PY is both soluble and has low molecular weight, blue OLEDs were fabricated using both spin-coating and vacuum deposition thin film processing techniques to study the effect of processing on device performance. OLED devices using a spin-coated layer consisting of 4′,4′′-tris(N-carbazolyl)triphenylamine (TCTA) and 2-(4-biphenylyl)-5-(4-tert-butylphenyl)-1,3,4-oxadiazole (PBD) as a …

Solution processable phosphorescent dendrimers based on cyclic phosphazenes for use in organic light emitting diodes (OLEDs)

A novel solution processable phosphorescent dendrimer based on cyclic phosphazene (CP) cores has been prepared and used as emissive layers in simple OLED architectures, providing efficiencies of 24.0 cd A^-1 and 16.7 lm W^-1. Bolink, Henk, Henk.Bolink@uv.es ; Garcia Santamaria, Sonsoles Amor, Sonsoles.Garcia@uv.es

Highly Stable and Efficient Light-Emitting Electrochemical Cells Based on Cationic Iridium Complexes Bearing Arylazole Ancillary Ligands.

A series of bis-cyclometalated iridium(III) complexes of general formula [Ir(ppy)2(N∧N)][PF6] (ppy− = 2-phenylpyridinate; N∧N = 2-(1H-imidazol-2-yl)pyridine (1), 2-(2-pyridyl)benzimidazole (2), 1-methyl-2-pyridin-2-yl- 1H-benzimidazole (3), 2-(4′-thiazolyl)benzimidazole (4), 1- methyl-2-(4′-thiazolyl)benzimidazole (5)) is reported, and their use as electroluminescent materials in light-emitting electrochemical cell (LEC) devices is investigated. [2][PF6] and [3][PF6] are orange emitters with intense unstructured emission around 590 nm in acetonitrile solution. [1][PF6], [4][PF6], and [5][PF6] are green weak emitters with structured emission bands peaking around 500 nm. The different photoph…

Quantification of spatial inhomogeneity in perovskite solar cells by hyperspectral luminescence imaging

Vacuum evaporated perovskite solar cells with a power conversion efficiency of 15% have been characterized using hyperspectral luminescence imaging. Hyperspectral luminescence imaging is a novel technique that offers spectrally resolved photoluminescence and electroluminescence maps (spatial resolution is 2 micrometer) on an absolute scale. This allows, using the generalized Planck’s law, the construction of absolute maps of the depth-averaged quasi-Fermi level splitting (Δμ), which determines the maximum achievable open circuit voltage (Voc) of the solar cells. In a similar way, using the generalized reciprocity relations the charge transfer efficiency of the cells can be obtained from the…

Solution-processed bi-layer polythiophene–fullerene organic solar cells

An ionic polymer based on a polythiophene backbone with appended imidazolium moieties was successfully implemented as a donor material in fully solution-processed efficient bi-layer solar cells prepared by the low impact meniscus coating technique. High fill factors and device reproducibility were obtained, even for ultrathin polymer layers, indicating excellent film formation properties and good compatibility with solution processing techniques. The possibility of smooth counter ion exchange, allowing solubility modification and efficiency tuning, enables exploration of new functionalities and other device architectures.

Efficient photoluminescent thin films consisting of anchored hybrid perovskite nanoparticles

Methylammonium lead bromide nanoparticles are synthetized with a new ligand (11-aminoundecanoic acid hydrobromide) by a non-template method. Upon dispersion in toluene they show a remarkable photoluminescence quantum yield of 80%. In addition, the bifunctional ligand allows anchoring of the nanoparticles on a variety of conducting and semiconducting surfaces, showing bright photoluminescence with a quantum yield exceeding 50%. This opens a path for the simple and inexpensive preparation of multilayer light-emitting devices. NRF (Natl Research Foundation, S’pore) ASTAR (Agency for Sci., Tech. and Research, S’pore) Accepted version

CCDC 2081388: Experimental Crystal Structure Determination

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CCDC 968510: Experimental Crystal Structure Determination

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CCDC 1490702: Experimental Crystal Structure Determination

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CCDC 1562407: Experimental Crystal Structure Determination

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CCDC 1562410: Experimental Crystal Structure Determination

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CCDC 1423252: Experimental Crystal Structure Determination

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CCDC 987700: Experimental Crystal Structure Determination

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CCDC 2081386: Experimental Crystal Structure Determination

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Ionic Multi-Resonant Thermally Activated Delayed Fluorescence Emitters for Light Emitting Electrochemical Cells (dataset)

CCDC 1546695: Experimental Crystal Structure Determination

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CCDC 1422375: Experimental Crystal Structure Determination

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Enhancing the photoluminescence quantum yields of blue-emitting cationic iridium(III) complexes bearing bisphosphine ligands (dataset)

CCDC 1490703: Experimental Crystal Structure Determination

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CCDC 1423251: Experimental Crystal Structure Determination

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CCDC 2061123: Experimental Crystal Structure Determination

Related Article: Chenfei Li, Campbell F. R. Mackenzie, Said A. Said, Amlan K. Pal, Mohammad A. Haghighatbin, Azin Babaei, Michele Sessolo, David B. Cordes, Alexandra M. Z. Slawin, Paul C. J. Kamer, Henk J. Bolink, Conor F. Hogan, Eli Zysman-Colman|2021|Inorg.Chem.|60|10323|doi:10.1021/acs.inorgchem.1c00804

CCDC 974016: Experimental Crystal Structure Determination

Related Article: Edwin C. Constable, Catherine E. Housecroft, Gabriel E. Schneider, Jennifer A. Zampese, Henk J. Bolink, Antonio Pertegás, Cristina Roldan-Carmona|2014|Dalton Trans.|43|4653|doi:10.1039/C3DT53477D

CCDC 974019: Experimental Crystal Structure Determination

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CCDC 1515402: Experimental Crystal Structure Determination

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CCDC 1944543: Experimental Crystal Structure Determination

Related Article: Violeta Sicilia, Lorenzo Arnal, Andrés J. Chueca, Sara Fuertes, Azin Babaei, Ana María Igual Muñoz, Michele Sessolo, Henk J. Bolink|2020|Inorg.Chem.|59|1145|doi:10.1021/acs.inorgchem.9b02782

CCDC 1044762: Experimental Crystal Structure Determination

Related Article: Iván González, Paulina Dreyse, Diego Cortés-Arriagada, Mahesh Sundararajan, Claudio Morgado, Iván Brito, Cristina Roldán-Carmona, Henk J. Bolink, Bárbara Loeb|2015|Dalton Trans.|44|14771|doi:10.1039/C5DT01385B

CCDC 1490707: Experimental Crystal Structure Determination

Related Article: Diego Rota Martir, Cristina Momblona, Antonio Pertegás, David B. Cordes, Alexandra M. Z. Slawin, Henk J. Bolink, and Eli Zysman-Colman|2016|ACS Applied Materials and Interfaces|8|33907|doi:10.1021/acsami.6b14050

CCDC 1486906: Experimental Crystal Structure Determination

Related Article: Fabian Brunner, Laura Martínez-Sarti, Sarah Keller, Antonio Pertegás, Alessandro Prescimone, Edwin C. Constable, Henk J. Bolink, Catherine E. Housecroft|2016|Dalton Trans.|45|15180|doi:10.1039/C6DT02665F

CCDC 1422372: Experimental Crystal Structure Determination

Related Article: Sarah Keller, Antonio Pertegás, Giulia Longo, Laura Martínez, Jesús Cerdá, José M. Junquera-Hernández, Alessandro Prescimone, Edwin C. Constable, Catherine E. Housecroft, Enrique Ortí, Henk J. Bolink|2016|J.Mater.Chem.C|4|3857|doi:10.1039/C5TC03725E

CCDC 1546696: Experimental Crystal Structure Determination

Related Article: Adam F. Henwood, Amlan K. Pal, David B. Cordes, Alexandra M. Z. Slawin, Thomas W. Rees, Cristina Momblona, Azin Babaei, Antonio Pertegás, Enrique Ortí, Henk J. Bolink, Etienne Baranoff, Eli Zysman-Colman|2017|J.Mater.Chem.C|5|9638|doi:10.1039/C7TC03110F

CCDC 1486907: Experimental Crystal Structure Determination

Related Article: Fabian Brunner, Laura Martínez-Sarti, Sarah Keller, Antonio Pertegás, Alessandro Prescimone, Edwin C. Constable, Henk J. Bolink, Catherine E. Housecroft|2016|Dalton Trans.|45|15180|doi:10.1039/C6DT02665F

CCDC 1486908: Experimental Crystal Structure Determination

Related Article: Fabian Brunner, Laura Martínez-Sarti, Sarah Keller, Antonio Pertegás, Alessandro Prescimone, Edwin C. Constable, Henk J. Bolink, Catherine E. Housecroft|2016|Dalton Trans.|45|15180|doi:10.1039/C6DT02665F

CCDC 1844060: Experimental Crystal Structure Determination

Related Article: Fabian Brunner, Azin Babaei, Antonio Pertegás, José M. Junquera-Hernández, Alessandro Prescimone, Edwin C. Constable, Henk J. Bolink, Michele Sessolo, Enrique Ortí, Catherine E. Housecroft|2019|Dalton Trans.|48|446|doi:10.1039/C8DT03827A

CCDC 1555727: Experimental Crystal Structure Determination

Related Article: Elia Matteucci, Andrea Baschieri, Andrea Mazzanti, Letizia Sambri, Jorge Ávila, Antonio Pertegás, Henk J. Bolink, Filippo Monti, Enrico Leoni, and Nicola Armaroli|2017|Inorg.Chem.|56|10584|doi:10.1021/acs.inorgchem.7b01544

CCDC 1562409: Experimental Crystal Structure Determination

Related Article: Murat Alkan-Zambada, Sarah Keller, Laura Martínez-Sarti, Alessandro Prescimone, José M. Junquera-Hernández, Edwin C. Constable, Henk J. Bolink, Michele Sessolo, Enrique Ortí, Catherine E. Housecroft|2018|J.Mater.Chem.C|6|8460|doi:10.1039/C8TC02882F

CCDC 1978436: Experimental Crystal Structure Determination

Related Article: Sarah Keller, Alessandro Prescimone, Maria-Grazia La Placa, José M. Junquera-Hernández, Henk J. Bolink, Edwin C. Constable, Michele Sessolo, Enrique Ortí, Catherine E. Housecroft|2020|RSC Advances|10|22631|doi:10.1039/D0RA03824E

CCDC 972526: Experimental Crystal Structure Determination

Related Article: Gabriel E. Schneider, Antonio Pertegás, Edwin C. Constable, Catherine E. Housecroft, Nik Hostettler, Collin D. Morris, Jennifer A. Zampese, Henk J. Bolink, José M. Junquera-Hernández, Enrique Ortí, Michele Sessolo|2014|J.Mater.Chem.C|2|7047|doi:10.1039/C4TC01171F

CCDC 1423253: Experimental Crystal Structure Determination

Related Article: Diego Rota Martir, Ashu K. Bansal, Vincent Di Mascio, David B. Cordes, Adam F. Henwood, Alexandra M. Z. Slawin, Paul C. J. Kamer, Laura Martínez-Sarti, Antonio Pertegás, Henk J. Bolink, Ifor D. W. Samuel, Eli Zysman-Colman|2016|Inorg.Chem.Front.|3|218|doi:10.1039/C5QI00177C

CCDC 2061124: Experimental Crystal Structure Determination

Related Article: Chenfei Li, Campbell F. R. Mackenzie, Said A. Said, Amlan K. Pal, Mohammad A. Haghighatbin, Azin Babaei, Michele Sessolo, David B. Cordes, Alexandra M. Z. Slawin, Paul C. J. Kamer, Henk J. Bolink, Conor F. Hogan, Eli Zysman-Colman|2021|Inorg.Chem.|60|10323|doi:10.1021/acs.inorgchem.1c00804

CCDC 1019228: Experimental Crystal Structure Determination

Related Article: Andreas M. Bünzli, Edwin C. Constable, Catherine E. Housecroft, Alessandro Prescimone, Jennifer A. Zampese, Giulia Longo, Lidón Gil-Escrig, Antonio Pertegás, Enrique Ortí, Henk J. Bolink|2015|Chemical Science|6|2843|doi:10.1039/C4SC03942D

CCDC 968508: Experimental Crystal Structure Determination

Related Article: Filippo Monti, Florian Kessler, Manuel Delgado, Julien Frey, Federico Bazzanini, Gianluca Accorsi, Nicola Armaroli, Henk J. Bolink, Enrique Ortí, Rosario Scopelliti, Md. Khaja Nazeeruddin, and Etienne Baranoff|2013|Inorg.Chem.|52|10292|doi:10.1021/ic400600d

CCDC 1581155: Experimental Crystal Structure Determination

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CCDC 1844063: Experimental Crystal Structure Determination

Related Article: Fabian Brunner, Azin Babaei, Antonio Pertegás, José M. Junquera-Hernández, Alessandro Prescimone, Edwin C. Constable, Henk J. Bolink, Michele Sessolo, Enrique Ortí, Catherine E. Housecroft|2019|Dalton Trans.|48|446|doi:10.1039/C8DT03827A

CCDC 2081394: Experimental Crystal Structure Determination

Related Article: Marco Meyer, Lorenzo Mardegan, Daniel Tordera, Alessandro Prescimone, Michele Sessolo, Henk J. Bolink, Edwin C. Constable, Catherine E. Housecroft|2021|Dalton Trans.|50|17920|doi:10.1039/D1DT03239A

CCDC 1907394: Experimental Crystal Structure Determination

Related Article: Nina Arnosti, Fabian Brunner, Isidora Susic, Sarah Keller, José M. Junquera‐Hernández, Alessandro Prescimone, Henk J. Bolink, Michele Sessolo, Enrique Ortí, Catherine E. Housecroft, Edwin C. Constable|2020|Adv.Opt.Mater.|8|1901689|doi:10.1002/adom.201901689

CCDC 2061121: Experimental Crystal Structure Determination

Related Article: Chenfei Li, Campbell F. R. Mackenzie, Said A. Said, Amlan K. Pal, Mohammad A. Haghighatbin, Azin Babaei, Michele Sessolo, David B. Cordes, Alexandra M. Z. Slawin, Paul C. J. Kamer, Henk J. Bolink, Conor F. Hogan, Eli Zysman-Colman|2021|Inorg.Chem.|60|10323|doi:10.1021/acs.inorgchem.1c00804

CCDC 2081387: Experimental Crystal Structure Determination

Related Article: Marco Meyer, Lorenzo Mardegan, Daniel Tordera, Alessandro Prescimone, Michele Sessolo, Henk J. Bolink, Edwin C. Constable, Catherine E. Housecroft|2021|Dalton Trans.|50|17920|doi:10.1039/D1DT03239A

CCDC 1053872: Experimental Crystal Structure Determination

Related Article: Nail M. Shavaleev, Guohua Xie, Shinto Varghese, David B. Cordes, Alexandra M. Z. Slawin, Cristina Momblona, Enrique Ortí, Henk J. Bolink, Ifor D. W. Samuel, Eli Zysman-Colman|2015|Inorg.Chem.|54|5907|doi:10.1021/acs.inorgchem.5b00717

CCDC 1053870: Experimental Crystal Structure Determination

Related Article: Nail M. Shavaleev, Guohua Xie, Shinto Varghese, David B. Cordes, Alexandra M. Z. Slawin, Cristina Momblona, Enrique Ortí, Henk J. Bolink, Ifor D. W. Samuel, Eli Zysman-Colman|2015|Inorg.Chem.|54|5907|doi:10.1021/acs.inorgchem.5b00717

CCDC 2061118: Experimental Crystal Structure Determination

Related Article: Chenfei Li, Campbell F. R. Mackenzie, Said A. Said, Amlan K. Pal, Mohammad A. Haghighatbin, Azin Babaei, Michele Sessolo, David B. Cordes, Alexandra M. Z. Slawin, Paul C. J. Kamer, Henk J. Bolink, Conor F. Hogan, Eli Zysman-Colman|2021|Inorg.Chem.|60|10323|doi:10.1021/acs.inorgchem.1c00804

Blue-Emitting Cationic Iridium(III) Complexes Featuring Pyridylpyrimidine Cyclometalating Ligands and their Use in Sky-Blue and Blue-Green Light-Emitting Electrochemical Cells (LEECs) and Organic Light-Emitting Diodes (OLEDs) (dataset)

CCDC 1562458: Experimental Crystal Structure Determination

Related Article: Murat Alkan-Zambada, Sarah Keller, Laura Martínez-Sarti, Alessandro Prescimone, José M. Junquera-Hernández, Edwin C. Constable, Henk J. Bolink, Michele Sessolo, Enrique Ortí, Catherine E. Housecroft|2018|J.Mater.Chem.C|6|8460|doi:10.1039/C8TC02882F

CCDC 974020: Experimental Crystal Structure Determination

Related Article: Edwin C. Constable, Catherine E. Housecroft, Gabriel E. Schneider, Jennifer A. Zampese, Henk J. Bolink, Antonio Pertegás, Cristina Roldan-Carmona|2014|Dalton Trans.|43|4653|doi:10.1039/C3DT53477D

CCDC 2151291: Experimental Crystal Structure Determination

Related Article: Sara Fuertes, Lorenzo Mardegan, Ignacio Martínez, Silvia Ventura, Irene Ara, Daniel Tordera, Henk J. Bolink, Violeta Sicilia|2022|J.Mater.Chem.C|10|15491|doi:10.1039/D2TC02539F

CCDC 949190: Experimental Crystal Structure Determination

Related Article: Andreas M. Bünzli, Henk J. Bolink, Edwin C. Constable, Catherine E. Housecroft, José M. Junquera-Hernández, Markus Neuburger, Enrique Ortí, Antonio Pertegás, Juan J. Serrano-Pérez, Daniel Tordera, Jennifer A. Zampese|2014|Dalton Trans.|43|738|doi:10.1039/C3DT52622D

CCDC 910854: Experimental Crystal Structure Determination

Related Article: Daniel Tordera, Andreas M. Bünzli, Antonio Pertegás, José M. Junquera-Hernández, Edwin C. Constable, Jennifer A. Zampese, Catherine E. Housecroft, Enrique Ortí, Henk J. Bolink|2013|Chem.-Eur.J.|19|8597|doi:10.1002/chem.201300457

CCDC 1423259: Experimental Crystal Structure Determination

Related Article: Diego Rota Martir, Ashu K. Bansal, Vincent Di Mascio, David B. Cordes, Adam F. Henwood, Alexandra M. Z. Slawin, Paul C. J. Kamer, Laura Martínez-Sarti, Antonio Pertegás, Henk J. Bolink, Ifor D. W. Samuel, Eli Zysman-Colman|2016|Inorg.Chem.Front.|3|218|doi:10.1039/C5QI00177C

CCDC 968506: Experimental Crystal Structure Determination

Related Article: Filippo Monti, Florian Kessler, Manuel Delgado, Julien Frey, Federico Bazzanini, Gianluca Accorsi, Nicola Armaroli, Henk J. Bolink, Enrique Ortí, Rosario Scopelliti, Md. Khaja Nazeeruddin, and Etienne Baranoff|2013|Inorg.Chem.|52|10292|doi:10.1021/ic400600d

CCDC 959828: Experimental Crystal Structure Determination

Related Article: Gabriel E. Schneider, Henk J. Bolink, Edwin C. Constable, Cathrin D. Ertl, Catherine E. Housecroft, Antonio Pertegàs, Jennifer A. Zampese, Andreas Kanitz, Florian Kessler, Sebastian B. Meier|2014|Dalton Trans.|43|1961|doi:10.1039/C3DT53229A

CCDC 2061119: Experimental Crystal Structure Determination

Related Article: Chenfei Li, Campbell F. R. Mackenzie, Said A. Said, Amlan K. Pal, Mohammad A. Haghighatbin, Azin Babaei, Michele Sessolo, David B. Cordes, Alexandra M. Z. Slawin, Paul C. J. Kamer, Henk J. Bolink, Conor F. Hogan, Eli Zysman-Colman|2021|Inorg.Chem.|60|10323|doi:10.1021/acs.inorgchem.1c00804

CCDC 1978440: Experimental Crystal Structure Determination

Related Article: Sarah Keller, Alessandro Prescimone, Maria-Grazia La Placa, José M. Junquera-Hernández, Henk J. Bolink, Edwin C. Constable, Michele Sessolo, Enrique Ortí, Catherine E. Housecroft|2020|RSC Advances|10|22631|doi:10.1039/D0RA03824E

CCDC 1978441: Experimental Crystal Structure Determination

Related Article: Sarah Keller, Alessandro Prescimone, Maria-Grazia La Placa, José M. Junquera-Hernández, Henk J. Bolink, Edwin C. Constable, Michele Sessolo, Enrique Ortí, Catherine E. Housecroft|2020|RSC Advances|10|22631|doi:10.1039/D0RA03824E

CCDC 1490708: Experimental Crystal Structure Determination

Related Article: Diego Rota Martir, Cristina Momblona, Antonio Pertegás, David B. Cordes, Alexandra M. Z. Slawin, Henk J. Bolink, and Eli Zysman-Colman|2016|ACS Applied Materials and Interfaces|8|33907|doi:10.1021/acsami.6b14050

CCDC 1490705: Experimental Crystal Structure Determination

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CCDC 1562460: Experimental Crystal Structure Determination

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CCDC 1944542: Experimental Crystal Structure Determination

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CCDC 1562411: Experimental Crystal Structure Determination

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CCDC 1429456: Experimental Crystal Structure Determination

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CCDC 2151293: Experimental Crystal Structure Determination

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CCDC 1583689: Experimental Crystal Structure Determination

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CCDC 1546698: Experimental Crystal Structure Determination

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CCDC 1490429: Experimental Crystal Structure Determination

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CCDC 1486911: Experimental Crystal Structure Determination

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CCDC 1019229: Experimental Crystal Structure Determination

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CCDC 1562408: Experimental Crystal Structure Determination

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CCDC 1423255: Experimental Crystal Structure Determination

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CCDC 974892: Experimental Crystal Structure Determination

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CCDC 1515401: Experimental Crystal Structure Determination

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CCDC 1581154: Experimental Crystal Structure Determination

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CCDC 1538393: Experimental Crystal Structure Determination

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CCDC 1422374: Experimental Crystal Structure Determination

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CCDC 2151294: Experimental Crystal Structure Determination

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CCDC 1538394: Experimental Crystal Structure Determination

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CCDC 2081391: Experimental Crystal Structure Determination

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CCDC 1421913: Experimental Crystal Structure Determination

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CCDC 1581156: Experimental Crystal Structure Determination

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Impact of the Use of Sterically Congested Cyclometalated Ligands on the Optoelectronic Properties and Device Performances In Light-Emitting Electrochemical Cells of Cationic Iridium(III) Complexes (dataset)

CCDC 1944541: Experimental Crystal Structure Determination

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CCDC 2081389: Experimental Crystal Structure Determination

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CCDC 1562448: Experimental Crystal Structure Determination

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CCDC 1421914: Experimental Crystal Structure Determination

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CCDC 949192: Experimental Crystal Structure Determination

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CCDC 2081393: Experimental Crystal Structure Determination

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CCDC 1562457: Experimental Crystal Structure Determination

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CCDC 1019226: Experimental Crystal Structure Determination

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CCDC 1423254: Experimental Crystal Structure Determination

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CCDC 2061120: Experimental Crystal Structure Determination

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CCDC 1583690: Experimental Crystal Structure Determination

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CCDC 1581157: Experimental Crystal Structure Determination

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CCDC 974017: Experimental Crystal Structure Determination

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CCDC 974022: Experimental Crystal Structure Determination

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CCDC 1490428: Experimental Crystal Structure Determination

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CCDC 974021: Experimental Crystal Structure Determination

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CCDC 1009455: Experimental Crystal Structure Determination

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CCDC 2081390: Experimental Crystal Structure Determination

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CCDC 1055780: Experimental Crystal Structure Determination

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CCDC 1844062: Experimental Crystal Structure Determination

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CCDC 1562453: Experimental Crystal Structure Determination

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Data underpinning - Chiral Iridium(III) Complexes in Light-Emitting Electrochemical Cells: Exploring The Impact of Stereochemistry on The Photophysical Properties and Device Performances

CCDC 974023: Experimental Crystal Structure Determination

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CCDC 1486909: Experimental Crystal Structure Determination

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CCDC 1421915: Experimental Crystal Structure Determination

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CCDC 949191: Experimental Crystal Structure Determination

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CCDC 914725: Experimental Crystal Structure Determination

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CCDC 987698: Experimental Crystal Structure Determination

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CCDC 1978437: Experimental Crystal Structure Determination

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CCDC 1027525: Experimental Crystal Structure Determination

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CCDC 971737: Experimental Crystal Structure Determination

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CCDC 914726: Experimental Crystal Structure Determination

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CCDC 974018: Experimental Crystal Structure Determination

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CCDC 1546697: Experimental Crystal Structure Determination

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CCDC 1844061: Experimental Crystal Structure Determination

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CCDC 2061122: Experimental Crystal Structure Determination

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CCDC 996509: Experimental Crystal Structure Determination

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CCDC 1581158: Experimental Crystal Structure Determination

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CCDC 968507: Experimental Crystal Structure Determination

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CCDC 987699: Experimental Crystal Structure Determination

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CCDC 1486910: Experimental Crystal Structure Determination

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CCDC 1562412: Experimental Crystal Structure Determination

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CCDC 1860879: Experimental Crystal Structure Determination

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CCDC 1978438: Experimental Crystal Structure Determination

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CCDC 1423258: Experimental Crystal Structure Determination

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CCDC 1581159: Experimental Crystal Structure Determination

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CCDC 1422373: Experimental Crystal Structure Determination

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CCDC 914724: Experimental Crystal Structure Determination

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CCDC 1062206: Experimental Crystal Structure Determination

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CCDC 1562449: Experimental Crystal Structure Determination

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CCDC 968505: Experimental Crystal Structure Determination

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CCDC 2081392: Experimental Crystal Structure Determination

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CCDC 993287: Experimental Crystal Structure Determination

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