Perovskite Light-Emitting Devices - Fundamentals and Working Principles

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…

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.

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)

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…

Structural control of mixed ionic and electronic transport in conducting polymers

Poly(3,4-ethylenedioxythiophene) doped with poly(styrenesulfonate), PEDOT:PSS, has been utilized for over two decades as a stable, solution-processable hole conductor. While its hole transport properties have been the subject of intense investigation, recent work has turned to PEDOT:PSS as a mixed ionic/electronic conductor in applications including bioelectronics, energy storage and management, and soft robotics. Conducting polymers can efficiently transport both holes and ions when sufficiently hydrated, however, little is known about the role of morphology on mixed conduction. Here, we show that bulk ionic and electronic mobilities are simultaneously affected by processing-induced change…

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…

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…

Vacuum deposition of perovskite films and solar cells

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…

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…

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…

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.

Colloids of naked CH 3 NH 3 PbBr 3 Perovskite Nanoparticles: Synthesis, Ssability, and thin solid film deposition

A novel preparation of lead halide, CH3NH3PbBr3, perovskite nanoparticle solid films from colloidal "naked" nanoparticles, that is, dispersible nanoparticles without any surfactant, is reported. The colloids are obtained by simply adding potassium ions, whose counterions are both more lipophilic and less coordinating than bromide ions, to the perovskite precursor solutions (CH3NH3Br/PbBr2 in dimethylformamide) following the reprecipitation strategy. The naked nanoparticles exhibit a low tendency to aggregate in solution, and they effectively self-assembled on a substrate by centrifugation of the colloid, leading to homogeneous nanoparticle solid films with arbitrary thickness. These results…

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…

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…

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…

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…

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…

Quantifying the Composition of Methylammonium Lead Iodide Perovskite Thin Films with Infrared Spectroscopy

Lead halide perovskites (ABX3) are generally formed from a reaction of the lead halide salt (BX2) with the halide salt of the A cation (AX). The effects of varying film compositions as result of non-stoichiometric precursor ratios on electronic properties of halide perovskites are currently under debate. It is imperative, but experimentally challenging, to determine the chemical composition of thin films as a function of precursor ratio for a full understanding of the effect. Herein we report a precise quantification of the methylammonium (MA) content in differently fabricated films of MAPbI3 via infrared (IR) spectroscopy. We compare the thin film data to the first high quality dielectric …

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.

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…

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…

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…

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…

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

Highly photoluminescent, dense solid films from organic-capped CH3NH3PbBr3 perovskite colloids

The preparation of densely-packed films from hybrid lead halide perovskite nanocrystals is not trivial, as during assembly into the solid state both the charge transport and photoluminescence can be substantially altered. The objective of the present study was to retain the pre-engineered confined morphologies of hybrid lead halide perovskite nanocrystals in densely-packed solid films by using short organic ligands. Therefore, the roles of the organic ligands would be to provide stable colloids and a good passivation of the nanoparticle surface, as well as to enable the efficient assembly of the nanoparticles in the solid state. We report here an effective and reproducible process to deposi…

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

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

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 %.

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…

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.

Influence of device geometry on sensor characteristics of planar organic electrochemical transistors.

The response of PEDOT:PSS planar electrochemical transistors to H2O2 can be tuned by varying the ratio between the areas of the channel and the gate electrode. Devices with small gates show lower background signal and higher sensitivity. The detection range, on the other hand, is found to be rather independent of the gate/channel area ratio.

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.

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…

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…

Controlling the mode of operation of organic transistors through side chain engineering

Electrolyte-gated organic transistors offer low bias operation facilitated by direct contact of the transistor channel with an electrolyte. Their operation mode is generally defined by the dimensionality of charge transport, where a field-effect transistor allows for electrostatic charge accumulation at the electrolyte/semiconductor interface, whereas an organic electrochemical transistor (OECT) facilitates penetration of ions into the bulk of the channel, considered a slow process, leading to volumetric doping and electronic transport. Conducting polymer OECTs allow for fast switching and high currents through incorporation of excess, hygroscopic ionic phases, but operate in depletion mode…

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…

Reinforced Room-Temperature Spin Filtering in Chiral Paramagnetic Metallopeptides

Chirality-induced spin selectivity (CISS), whereby helical molecules polarize the spin of electrical current, is an intriguing effect with potential applications in nanospintronics. In this nascent field, the study of the CISS effect using paramagnetic chiral molecules, which could introduce another degree of freedom in controlling the spin transport, remains so far unexplored. To address this challenge, herein we propose the use of self-assembled monolayers (SAMs) of helical lanthanide-binding peptides. To elucidate the effect of the paramagnetic nuclei, monolayers of the peptide coordinating paramagnetic or diamagnetic ions are prepared. By means of spin-dependent electrochemistry, the CI…

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

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…

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…

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.

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…

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…

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…

Remote modification of bidentate phosphane ligands controlling the photonic properties in their complexes: Enhanced performance of [Cu(RN-xantphos)(N^N)][PF6] 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 BnNxantphos = 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 BnNxantphos- containing compounds (for which the highest-occupied molecular orbital is located on the phenoxazine moiety) are repor…

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…

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…

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.

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…

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.

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…

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

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 …

Preparation and Characterization of Mixed Halide MAPbI3−xClx Perovskite Thin Films by Three‐Source Vacuum Deposition

Chloride has been extensively used in the preparation of metal halide perovskites such as methylammonium lead iodide (MAPbI3-xClx), but its persistence and role in solution-processed materials has not yet been rationalized. Multiple-source vacuum deposition of perovskites enables a fine control over the thin-film stoichiometry, and allows to incorporate chemical species irrespectively of their solubility. In this communication, we present the first example of mixed MAPbI3-xClx thin films prepared by three-source vacuum deposition using MAI, PbI2 and PbCl2 as precursors. The optoelectronic properties of the material are evaluated through photovoltaic and electro-/photo-luminescent characteri…

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.

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.

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…

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…

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%.

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…

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.

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…

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…

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%.

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.

Origin of the Chemiresistive Response of Ultrathin Films of Conductive Metal–Organic Frameworks

Conductive metal-organic frameworks are opening new perspectives for the use of these porous materials for applications traditionally limited to more classical inorganic materials, such as their integration into electronic devices. This has enabled the development of chemiresistive sensors capable of transducing the presence of specific guests into an electrical response with good selectivity and sensitivity. By combining experimental data with computational modelling, a possible origin for the underlying mechanism of this phenomenon in ultrathin films (ca. 30 nm) of Cu-CAT-1 is described. ispartof: ANGEWANDTE CHEMIE-INTERNATIONAL EDITION vol:57 issue:46 pages:15086-15090 ispartof: location…

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…

[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 …

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.

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…

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…

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.

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…

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…

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…

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…

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

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.

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…

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

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 1562407: 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 1562410: 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 2081386: 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 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 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 1584756: Experimental Crystal Structure Determination

Related Article: Sarah Keller, Alessandro Prescimone, Henk Bolink, Michele Sessolo, Giulia Longo, Laura Martínez-Sarti, José M. Junquera-Hernández, Edwin C. Constable, Enrique Ortí, Catherine E. Housecroft|2018|Dalton Trans.|47|14263|doi:10.1039/C8DT01338A

CCDC 1584755: Experimental Crystal Structure Determination

Related Article: Sarah Keller, Alessandro Prescimone, Henk Bolink, Michele Sessolo, Giulia Longo, Laura Martínez-Sarti, José M. Junquera-Hernández, Edwin C. Constable, Enrique Ortí, Catherine E. Housecroft|2018|Dalton Trans.|47|14263|doi:10.1039/C8DT01338A

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 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 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 1535142: Experimental Crystal Structure Determination

Related Article: Sarah Keller, Alessandro Prescimone, Henk Bolink, Michele Sessolo, Giulia Longo, Laura Martínez-Sarti, José M. Junquera-Hernández, Edwin C. Constable, Enrique Ortí, Catherine E. Housecroft|2018|Dalton Trans.|47|14263|doi:10.1039/C8DT01338A

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 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

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 1583875: Experimental Crystal Structure Determination

Related Article: Sarah Keller, Alessandro Prescimone, Henk Bolink, Michele Sessolo, Giulia Longo, Laura Martínez-Sarti, José M. Junquera-Hernández, Edwin C. Constable, Enrique Ortí, Catherine E. Housecroft|2018|Dalton Trans.|47|14263|doi:10.1039/C8DT01338A

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 1584757: Experimental Crystal Structure Determination

Related Article: Sarah Keller, Alessandro Prescimone, Henk Bolink, Michele Sessolo, Giulia Longo, Laura Martínez-Sarti, José M. Junquera-Hernández, Edwin C. Constable, Enrique Ortí, Catherine E. Housecroft|2018|Dalton Trans.|47|14263|doi:10.1039/C8DT01338A

CCDC 1562460: 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 1944542: 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 1562411: 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 1535141: Experimental Crystal Structure Determination

Related Article: Sarah Keller, Alessandro Prescimone, Henk Bolink, Michele Sessolo, Giulia Longo, Laura Martínez-Sarti, José M. Junquera-Hernández, Edwin C. Constable, Enrique Ortí, Catherine E. Housecroft|2018|Dalton Trans.|47|14263|doi:10.1039/C8DT01338A

CCDC 1584754: Experimental Crystal Structure Determination

Related Article: Sarah Keller, Alessandro Prescimone, Henk Bolink, Michele Sessolo, Giulia Longo, Laura Martínez-Sarti, José M. Junquera-Hernández, Edwin C. Constable, Enrique Ortí, Catherine E. Housecroft|2018|Dalton Trans.|47|14263|doi:10.1039/C8DT01338A

CCDC 1562408: 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 2081391: 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 1944541: 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 2081389: 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 1562448: 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 2081393: Experimental Crystal Structure Determination

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CCDC 1562457: Experimental Crystal Structure Determination

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CCDC 2061120: 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 1844062: Experimental Crystal Structure Determination

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CCDC 1562453: Experimental Crystal Structure Determination

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CCDC 1978437: Experimental Crystal Structure Determination

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CCDC 1978438: Experimental Crystal Structure Determination

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CCDC 1584752: Experimental Crystal Structure Determination

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CCDC 1562449: Experimental Crystal Structure Determination

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CCDC 1584753: Experimental Crystal Structure Determination

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