0000000000082144
AUTHOR
Iván Mora-seró
Polymer Halide Perovskites-Waveguides Integrated in Nanocellulose as a Wearable Amplifier-Photodetector System
Semiconductor organometallic halide (CH 3 NH 3 PbX 3 , X=Cl, Br, I) perovskites (MHP) have emerged as a very high promising material for optoelectronics. Their large absorption coefficients, high electronic mobilities, excellent quantum yield of emission at room temperature and tunable band-gap with the composition resulted in a new generation of photovoltaics and electronic devices. In this work, HPVK materials are successfully incorporated on a nanocellulose (NC) substrate with the intention to exploit the interesting properties of HPVK materials to construct wearable devices. In particular, a bilayer Poly(methyl methacrylate) /HPVK deposited on NC resulted in a suitable waveguide to demo…
Preferred Growth Direction by PbS Nanoplatelets Preserves Perovskite Infrared Light Harvesting for Stable, Reproducible, and Efficient Solar Cells
Formamidinium-based perovskite solar cells (PSCs) present the maximum theoretical efficiency of the lead perovskite family. However, formamidinium perovskite exhibits significant degradation in air. The surface chemistry of PbS has been used to improve the formamidinium black phase stability. Here, the use of PbS nanoplatelets with (100) preferential crystal orientation is reported, to potentiate the repercussion on the crystal growth of perovskite grains and to improve the stability of the material and consequently of the solar cells. As a result, a vertical growth of perovskite grains, a stable current density of 23 mA cm(-2), and a stable incident photon to current efficiency in the infr…
Manipulating spontaneous emission of the CsPbI3 Perovskite NCs using hybrid (HMM-Mie resonator) structures
Vapor growth of Hg1−xCdxI2 on glass using CdTe buffer
Abstract Vapor phase epitaxy (VPE) of Hg1−xCdxI2 layers on glass substrates covered by a CdTe buffer layer has been studied. The buffer layers of 2–4 μm thickness were formed by VPE using polycrystalline CdTe and Cd metal sources. The Hg1−xCdxI2 layers were grown using a (Hg1−yCdy)1−z(I2)z polycrystalline source, with a composition in the range of y=0.1–0.5 and z=0.5–0.8. Scanning electron microscopy and X-ray diffraction studies have shown that the composition and structure of Hg1−xCdxI2 layers depend strongly on the VPE conditions. Varying the growth time and source composition, it has been possible to obtain Hg1−xCdxI2 layers with the composition x in the range from approximately 0 (HgI2…
Boosting Long-Term Stability of Pure Formamidinium Perovskite Solar Cells by Ambient Air Additive Assisted Fabrication
Due to the high industrial interest for perovskite-based photovoltaic devices, there is an urgent need to fabricate them under ambient atmosphere, not limited to low relative humidity (RH) conditions. The formamidinium lead iodide (FAPI) perovskite α-black phase is not stable at room temperature and is challenging to stabilize in an ambient environment. In this work, we show that pure FAPI perovskite solar cells (PSCs) have a dramatic increase of device long-term stability when prepared under ambient air compared to FAPI PSCs made under nitrogen, both fabricated with N-methylpyrrolidone (NMP). The T80 parameter, the time in which the efficiency drops to 80% of the initial value, increases f…
Outstanding nonlinear optical properties of methylammonium- and Cs-PbX3 (X = Br, I, and Br–I) perovskites: Polycrystalline thin films and nanoparticles
Metal Halide Perovskites (MHPs) have arisen as promising materials to construct cost-effective photovoltaic and light emission devices. The study of nonlinear optical properties of MHPs is necessary to get similar success in nonlinear photonic devices, which is practically absent in the literature. The determination of the third order nonlinear coefficients is typically done by the Z-scan technique, which is limited by the scattering of polycrystalline thin films. In this work, we have studied nonlinear optical properties of polycrystalline CH3NH3PbX3 (MAPbX3) thin films and colloidal CsPbX3 nanoparticles with three different bandgaps (X3 = I3, Br3, and Br1.5I1.5). Their bright generation o…
Tuning optical/electrical properties of 2D/3D perovskite by the inclusion of aromatic cation
The employment of bulky aliphatic cations in the manufacture of moisture-stable materials has triggered the development and application of 2D/3D perovskites as sensitizers in moisture-stable solar cells. Although it is true that the moisture stability increases, it is also true that the photovoltaic performance of 2D/3D PVK materials is severely limited owing to quantum and dielectric confinement effects. Accordingly, it is necessary the synthesis and deep optical characterization of materials with an adequate management of dielectric contrast between the layers. Here, we demonstrate the successful tuning of dielectric confinement by the inclusion of a conjugated molecule, as a bulky cation…
The role of surface chemical states on the photocatalytic behavior of all-inorganic mixed halide perovskite nanocrystals
Enhanced nanoscopy of individual CsPbBr3 perovskite nanocrystals using dielectric sub-micrometric antennas
We demonstrate an efficient, simple, and low-cost approach for enhanced nanoscopy in individual green emitting perovskite (CsPbBr3) nanocrystals via TiO2 dielectric nanoantenna. The observed three- to five-fold emission enhancement is attributed to near-field effects and emission steering promoted by the coupling between the perovskite nanocrystals and the dielectric sub-micrometric antennas. The dark-field scattering configuration is then exploited for surface-enhanced absorption measurements, showing a large increase in detection sensitivity, leading to the detection of individual nanocrystals. Due to the broadband spectral response of the Mie sub-micrometric antennas, the method can be e…
Role of Self-Absorption in the Photoluminescence Waveguided along CsPbBr3 Perovskite Nanocrystals Thin Films
During the last years, perovskite nanocrystals (PNCs) have been intensively studied as nanomaterials with excellent light absorption/emission properties. For example, PNCs have been successfully applied in solar cells, where the high absorption coefficient above the band gap increases the conversion efficiencies; or in optical sources, where the high quantum yield of emission at room temperature allows a low threshold of stimulated emission. In this scenario, an optical waveguide represents a suitable platform to enhance their electrooptical properties and to integrate different photonic functionalities. However, propagation of light along close packed films of PNCs is usually restricted to…
Amplified Spontaneous Emission in Thin Films of CsPbX3 Perovskite Nanocrystals
During the last years, Metal Halide Perovskites (MHPs) have attracted special attention as an efficient conversion films for photovoltaics, or excellent gain media to construct optical sources. In spite of the fact that most of the works have been focussed on CH 3 NH 3 PbX 3 (X=Cl, Br, I) polycrystalline thin films, MHP can be also synthesized as colloidal nanocrystals. In particular, caesium lead halide perovskite CsPbX 3 nanocrystals (NCs) revealed extraordinary properties for optoelectronics. With a high quantum yield of emission (>90%) at room temperature and linewidths less than 100 meV, CsPbX 3 NCs have demonstrated favourable characteristics for active photonics. Indeed, thin films o…
Influence of twinned structure on the morphology of CdTe(111) layers grown by MOCVD on GaAs(100) substrates
Abstract The morphology and structure of CdTe(1 1 1) layers grown on GaAs(1 0 0) by MOCVD have been studied by atomic force microscopy (AFM) and X-ray texture analysis. Growth conditions have been chosen so that mirror-like CdTe layers are obtained. Layers whose growth times vary between 10 s and 2 h have been investigated. The X-ray texture analysis shows that the CdTe layers grown on GaAs substrates that were thermally treated at 580°C for 30 min in a H 2 atmosphere exhibit a (1 1 1) preferential orientation and are twinned. This twinned structure of the (1 1 1)CdTe layer which is observed as 60° rotated triangular crystallites in the AFM images strongly influences the surface morphology.…
Study of the Partial Substitution of Pb by Sn in Cs-Pb-Sn-Br Nanocrystals Owing to Obtaining Stable Nanoparticles with Excellent Optical Properties.
Halide perovskites are revolutionizing the photovoltaic and optoelectronic fields with outstanding performances obtained in a remarkably short time. However, two major challenges remain: the long-term stability and the Pb content, due to its toxicity. Despite the great effort carried out to substitute the Pb by a less hazardous element, lead-free perovskite still remains more unstable than lead-containing perovskites and presents lower performance as well. In this work, we demonstrate the colloidal preparation of Cs–Pb–Sn–Br nanoparticles (NPs) where Sn is incorporated up to 18.8%. Significantly, we have demonstrated that the partial substitution of Pb by Sn does not produce a deleterious e…
Homogeneous and inhomogeneous broadening in single perovskite nanocrystals investigated by micro-photoluminescence
Abstract Metal halides with perovskite crystalline structure have given rise to efficient optoelectronic and photonic devices. In the present work, we have studied the light emission properties of single CsPbBr3 and CsPbI3 semiconductor perovskite nanocrystals (PNCs), as the basis for a statistical analysis of micro-photoluminescence (micro-PL) spectra measured on tens of them. At room temperature, the linewidth extracted from PL spectra acquired in dense films of these nanocrystals is not very different from that of micro-PL measured in single nanocrystals. This means that the homogeneous linewidth due to exciton-phonon interaction is comparable or larger than the inhomogeneous effect asso…
Integration of a perovskite-based amplifier and photodetector system in rigid and solid substrates
During the last years, organometallic lead halide perovskites (LHP) have been widely studied as outstanding materials for photovoltaics and photonics applications [1] . These emerging semiconductors are fabricated by cheap and straightforward solution process techniques on polycrystalline film of the compound CH 3 NH 3 PbX 3 (X=Cl, Br, I). Their outstanding properties of these films include large absorption coefficients above the bandgap, high electronic mobilities, high quantum yield of emission at room temperature or tunable band-gap with the composition [1] . In this work, we exploit the excellent light emitting and photodetection properties of CH 3 NH 3 PbI 3 thin films to integrate a w…
High Optical Performance of Cyan‐Emissive CsPbBr3 Perovskite Quantum Dots Embedded in Molecular Organogels
This is the pre-peer reviewed version of the following article: High Optical Performance of Cyan‐Emissive CsPbBr3 Perovskite Quantum Dots Embedded in Molecular Organogels, which has been published in final form at https://doi.org/10.1002/adom.202001786. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions." Perovskite quantum dots (PQDs) have fascinating optoelectronic properties, such as high photoluminescence quantum yield (PLQY) for a broad range of materials, and the possibility to obtain different bandgaps with the same material or halide combinations. Nevertheless, blue‐emissive materials generally present…
Optimization of semiconductor halide perovskite layers to implement waveguide amplifiers
Semiconductor organometallic halide (CH 3 NH 3 PbX 3 , X=Cl, Br, I) perovskites (HPVK) have been emerged as a potential gain media to construct a new generation of active photonic devices. Indeed, during the last three years a significant effort has been carried out to implement HPVK-based optical amplifiers or lasers with improved quality factors. In particular, minimization of the threshold of stimulated emission has been an important concern to decrease the power consumption, and hence to enhance the performances of the device. For this purpose strategies include a suitable integration of the semiconductor in a photonic structure, or the optimization of the material. Here we propose a no…
Flash infrared annealing as a cost-effective and low environmental impact processing method for planar perovskite solar cells
Abstract For successful commercialization of perovskite solar cells, straightforward solutions in terms of environmental impact and economic feasibility are still required. Flash Infrared Annealing (FIRA) is a rapid method to fabricate perovskite solar cells with efficiencies >18% on simple, planar architecture, which allows a film synthesis in only 1.2 s, faster than the previous report based in a meso architecture and all of them without the usage of antisolvent. In this work, through a comparative study with the common lab-scale method, the so-called antisolvent (AS), the main photovoltaic parameters and working mechanisms obtained from impedance spectroscopy (IS) measurements show simil…
Inhomogeneous Broadening of Photoluminescence Spectra and Kinetics of Nanometer-Thick (Phenethylammonium)2PbI4 Perovskite Thin Films: Implications for Optoelectronics
An outstanding potentiality of layered two-dimensional (2D) organic–inorganic hybrid perovskites (2DHPs) is in the development of solar cells, photodetectors, and light-emitting diodes. In 2DHPs, an exciton is localized in an atomically thin lead(II) halide inorganic layer of sub-nanometer thickness as in a quantum well sandwiched between organic layers as energetic and dielectric barriers. In previous years, versatile optical characterization of 2DHPs has been carried out mainly for thin flakes of single crystals and ultrathin (of the order of 20 nm) polycrystalline films, whereas there is a lack of optical characterization of thick (hundreds of nanometers) polycrystalline films, fundament…
Halide perovskite amplifiers integrated in polymer waveguides
Semiconductor organometallic halide perovskites (CH 3 NH 3 PbX 3 , X=Cl, Br, I) (HPVK) have emerged as a new promising material able to improve the optoelectronic technology performance. Although this material has mostly been applied to improve the efficiency of photovoltaic devices, it also shows amazing properties for photonic applications. In particular, HPVK exhibits high photoluminescence (PL) quantum yield (up to 70%) at room temperature together with a tunable band-gap controlled by its chemical composition. In addition, since HPVKs is deposited in solution at room conditions, it can be easily incorporated in different photonic structures to efficiently exploit its emission propertie…
Tunable light emission by exciplex state formation between hybrid halide perovskite and core/shell quantum dots: Implications in advanced LEDs and photovoltaics
A perovskite–quantum dot exciplex has been detected, opening a broad range of possibilities for advanced optoelectronic devices.
Integrated Optical Amplifier-Photodetector on a Wearable Nanocellulose Substrate
Flexible optoelectronics has emerged as an outstanding platform to pave the road toward vanguard technology advancements. As compared to conventional rigid substrates, a flexible technology enables mechanical deformation while maintaining stable performance. The advantages include not only the development to novel applications, but also the implementation of a wearable technology directly in contact with a curved surface. Here the monolithic integration of a perovskite‐based optical waveguide amplifier together with a photodetector on a nanocellulose substrate is shown to demonstrate the feasibility of a stretchable signal manipulation and receptor system fabricated on a biodegradable mater…
State of the art and prospects for halide perovskite nanocrystals
Financiado para publicación en acceso aberto: Universidade de Vigo/CISUG Metal-halide perovskites have rapidly emerged as one of the most promising materials of the 21st century, with many exciting properties and great potential for a broad range of applications, from photovoltaics to optoelectronics and photocatalysis. The ease with which metal-halide perovskites can be synthesized in the form of brightly luminescent colloidal nanocrystals, as well as their tunable and intriguing optical and electronic properties, has attracted researchers from different disciplines of science and technology. In the last few years, there has been a significant progress in the shape-controlled synthesis of …
Single step deposition of an interacting layer of a perovskite matrix with embedded quantum dots
Hybrid lead halide perovskite (PS) derivatives have emerged as very promising materials for the development of optoelectronic devices in the last few years. At the same time, inorganic nanocrystals with quantum confinement (QDs) possess unique properties that make them suitable materials for the development of photovoltaics, imaging and lighting applications, among others. In this work, we report on a new methodology for the deposition of high quality, large grain size and pinhole free PS films (CH3NH3PbI3) with embedded PbS and PbS/CdS core/shell Quantum Dots (QDs). The strong interaction between both semiconductors is revealed by the formation of an exciplex state, which is monitored by p…
Recycled Photons Traveling Several Millimeters in Waveguides Based on CsPbBr 3 Perovskite Nanocrystals
Reabsorption and reemission of photons, or photon recycling (PR) effect, represents an outstanding mechanism to enhance the carrier and photon densities in semiconductor thin films. This work demonstrates the propagation of recycled photons over several mm by integrating a thin film of CsPbBr3 nanocrystals into a planar waveguide. An experimental set-up based on a frequency modulation spectroscopy allows to characterize the PR effect and the determination of the effective decay time of outcoupled photons. A correlation between the observed photoluminescence redshift and the increase of the effective decay time is demonstrated, which grows from 3.5 to near 9 ns in the best device. A stochast…
Impedance analysis of perovskite solar cells: a case study
Metal halide perovskites are mixed electronic-ionic semiconductors with an extraordinary rich optoelectronic behavior and the capability to function very efficiently as active layers in solar cells, with a record efficiency surpassing 23% nowadays. In this work, we carry out an impedance spectroscopy analysis of two perovskite solar cells with quite distinct optical and electrical characteristics, i.e. MAPbI3 and CsPbBr3-based devices. The main aim of the analysis is to establish how, regardless the inherent complexity of the impedance spectrum due to ionic effects, information like ideality factors, recombination losses and the collection efficiency can be qualitative and quantitatively as…
Enabling long-term stable FAPb1-xSrxI3 quantum dots with high optical performance: the effect of Sr2+ doping
Numerical study of the growth conditions in an MOCVD reactor: application to the epitaxial growth of HgTe
Abstract In order to analyse the epitaxial growth by metalorganic chemical vapour deposition (MOCVD) of mercury telluride, HgTe, a 2D numerical model has been developed to simulate the gas flow in a horizontal MOCVD reactor. This model takes into account the Navier–Stokes equations coupled with the heat transfer and mass transport of chemical species. For the mathematical resolution of the governing equations a commercial solver, which can be run in a conventional personal computer, has been used. The study carried out presents a discussion about the dominant growth regime in a MOCVD growth as a function of different parameters: substrate temperature, total flow, partial pressure of precurs…
Structural quality of CH3NH3PbI3 perovskites for photovoltaic applications analyzed by electron microscopy techniques
Continuous-Flow Synthesis of Orange Emitting Sn(II)-Doped CsBr Materials
An ongoing demand toward lead-free all-inorganic cesium metal halide perovskites has presented Sn(II) as an ideal substitute of Pb(II) for applications in optoelectronic devices. The major concern regarding Sn(II) is the instability due to the ambient oxidation to Sn(IV). To expand the scope of traditional perovskite and analogues, herein the synthesis and optical performance of Sn(II)-doped CsBr, a new material formed by interstitial doping of Sn(II) into the CsBr matrix, are reported for the first time. This material is prepared following an antisolvent mediated recrystallization method using a continuous flow reactor, which is beneficial for scaling up the production compared to traditio…
Enhancement of the Performance of Perovskite Solar Cells, LEDs, and Optical Amplifiers by Anti-Solvent Additive Deposition
The efficiency of perovskite optoelectronic devices is increased by a novel method; its suitability for perovskite solar cells, light-emitting diodes, and optical amplifiers is demonstrated. The method is based on the introduction of organic additives during the anti-solvent step in the perovskite thin-film deposition process. Additives passivate grain boundaries reducing non-radiative recombination. The method can be easily extended to other additives.
Twin coarsening in CdTe(111) films grown on GaAs(100)
Abstract We present a scanning force microscopy study of twin coarsening in CdTe(1 1 1) films grown on GaAs(1 0 0). Two types of CdTe(1 1 1) twins grow epitaxially and with equal probability on the long-range wavy surface structure developed by previous in situ annealing of the GaAs(1 0 0) substrate. Due to this initial substrate wavy structure, the grain coarsening during film growth leads to a quasi-one-dimensional rippled pattern. We propose a coarsening mechanism between twins driven by the formation of stacking faults.
Optical Amplification in Hollow-Core Negative-Curvature Fibers Doped with Perovskite CsPbBr3 Nanocrystals
| openaire: EC/H2020/820423/EU//S2QUIP We report a hollow-core negative-curvature fiber (HC-NCF) optical signal amplifier fabricated by the filling of the air microchannels of the fiber with all-inorganic CsPbBr3 perovskite nanocrystals (PNCs). The optimum fabrication conditions were found to enhance the optical gain, up to +3 dB in the best device. Experimental results were approximately reproduced by a gain assisted mechanism based on the nonlinear optical properties of the PNCs, indicating that signal regeneration can be achieved under low pump powers, much below the threshold of stimulated emission. The results can pave the road of new functionalities of the HC-NCF with PNCs, such as op…
Signal Amplification in CsPbBr3 Nanoparticle-Doped Photonic Crystal Fibers
Nanoparticles (NPs) have been proved for various photonic and optoelectronic applications with superior performance. Doping holey-fibers with colloidal NPs is an idea with precedents in the optical literature. For example, CdZnS/ZnS core-shell quantum dots (QDs) based lasers at visible wavelengths [1, 2]; and PbS QDs doped fiber amplifiers operating at telecommunication wavelengths [3]. In this paper we harness the potential of photonic crystal fibers (PCFs) doped with chemically synthesized CsPbBr 3 Colloidal-NPs [4] to demonstrate gain functionalities in all-fiber optical microdevices.
Improving Long Term Stability of Pure Formamidinium Perovskite Solar Cells by Ambient Air Additive Assisted Fabrication
Some fundamentals of the vapor and solution growth of ZnSe and ZnO
Abstract Some fundamentals of ZnSe and ZnO vapor and solution growth are investigated. Residual water present in gases or gaseous mixtures such as H 2 , Ar or H 2 +H 2 O is shown to act as a sublimation activator in the vapor-phase transport of both compounds. The processes involved in the growth by chemically activated sublimation with such gases and gas mixtures have been studied by close-spaced vapor transport (CSVT). The ZnSe growth rate is found to be constant, while in the ZnO case a high initial growth rate is followed by slower growth subsequently. Using a theoretical model, the thermodynamic constants of the transport – energies of activation, sublimation and condensation and entha…
Optical Optimization of the TiO2 Mesoporous Layer in Perovskite Solar Cells by the Addition of SiO2 Nanoparticles
In this work, SiO2 nanoparticles (NPs) were integrated into the mesoporous TiO2 layer of a perovskite solar cell to investigate their effect on cell performance. Different concentrations of SiO2/ethanol have been combined in TiO2/ethanol to prepare pastes for the fabrication of the mesoporous layer with which perovskite solar cells have been fabricated. Addition of SiO2 NPs of 50 and 100 nm sizes produces an enhancement of cell performance mainly because of an improvement of the photocurrent. This increment is in good agreement with the theoretical predictions based on light scattering induced by dielectric SiO2 NPs. The samples using modified scaffolds with NPs also present a significant l…
Purcell Enhancement and Wavelength Shift of Emitted Light by CsPbI3 Perovskite Nanocrystals Coupled to Hyperbolic Metamaterials
Manipulation of the exciton emission rate in nanocrystals of lead halide perovskites (LHPs) was demonstrated by means of coupling of excitons with a hyperbolic metamaterial (HMM) consisting of alternating thin metal (Ag) and dielectric (LiF) layers. Such a coupling is found to induce an increase of the exciton radiative recombination rate by more than a factor of three due to the Purcell effect when the distance between the quantum emitter and HMM is nominally as small as 10 nm, which coincides well with the results of our theoretical analysis. Besides, an effect of the coupling-induced long wavelength shift of the exciton emission spectrum is detected and modeled. These results can be of i…
Engineering Sr-doping for enabling long-term stable FAPb1xSrxI3 quantum dots with 100% photoluminescence quantum yield
The Pb substitution in quantum dots (PQDs) with lesser toxic metals has been widely searched to be environmentally friendly, and be of comparable or improved performance compared to the lead-perovskite. However, the chemical nature of the lead substitute influences the incorporation mechanism into PQDs, which has not been explored in depth. In this work, we analyzed Sr-doping-induced changes in FAPbI3 perovskites by studying the optical, structural properties and chemical environment of FAPb1−xSrxI3 PQDs. The substitution of Pb by 7 at% Sr allows us to achieve FAPb1−xSrxI3 PQDs with 100% PLQY, high stability for 8 months under a relative humidity of 40–50%, and T80 = 6.5 m…
Inhibition of light emission from the metastable tetragonal phase at low temperatures in island-like films of lead iodide perovskites
Photonic applications based on halide perovskites, namely CH3NH3PbI3 (MAPbI3), have recently attracted remarkable attention due to the high efficiencies reported for photovoltaic and light emitting devices. Despite these outstanding results, there are many temperature-, laser excitation power-, and morphology-dependent phenomena that require further research to be completely understood. In this work, we have investigated in detail the nature of exciton optical transitions and recombination dynamics below and above the orthorhombic/tetragonal ('O'-/'T'-) temperature phase transition (∼150 K) depending on the material continuity (continuous-like) or discontinuity (island-like) in MAPbI3 films…
Single-Exciton Amplified Spontaneous Emission in Thin Films of CsPbX3 (X = Br, I) Perovskite Nanocrystals
CsPbX3 perovskite nanocrystals (PNCs) have emerged as an excellent material for stimulated emission purposes, with even more prospective applications than conventional colloidal quantum dots. However, a better understanding of the physical mechanisms responsible for amplified spontaneous emission (ASE) is required to achieve more ambitious targets (lasing under continuous wave optical or electrical excitation). Here, we establish the intrinsic mechanisms underlying ASE in PNCs of three different band gaps (CsPbBr3, CsPbBr1.5I1.5, and CsPbI3). Our characterization at cryogenic temperatures does not reveal any evidence of the biexciton mechanism in the formation of ASE. Instead, the measured …
Mechanisms of Spontaneous and Amplified Spontaneous Emission in CH3NH3PbI3 Perovskite Thin Films Integrated in an Optical Waveguide
In this paper, the physical mechanisms responsible for optical gain in ${\mathrm{CH}}_{3}{\mathrm{NH}}_{3}{\mathrm{Pb}\mathrm{I}}_{3}$ (MAPI) polycrystalline thin films are investigated experimentally and theoretically. Waveguide structures composed by a MAPI film embedded in between PMMA and silica layers are used as an efficient geometry to confine emitted light in MAPI films and minimize the energy threshold for amplified spontaneous emission (ASE). We show that photogenerated exciton density at the ASE threshold is as low as $(2.4\ensuremath{-}12)\ifmmode\times\else\texttimes\fi{}{10}^{16}\phantom{\rule{0.1em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$, which is below the Mott transition den…
From Dye Sensitized to Perovskite Solar Cells, The Missing Link
Fundamental working mechanisms of perovskite solar cells remain an elusive topic of research. Impedance Spectroscopy (IS) application to perovskite-based devices generates uncommon features and misleading outputs, mainly due to the lack of a stablished model for the interpretation of the results. In this work we control the perovskite precursor concentration to fabricate a series of perovskite-based solar cells with different amounts of perovskite absorber. Low concentration devices present the well-known dye sensitized solar cell (DSSCs) impedance pattern. As the amount of perovskite is increased, the characteristic impedance spectra of thin-film perovskite solar cells (PSCs) arises. This …
Structural characterization of bulk and nanoparticle lead halide perovskite thin films by (S)TEM techniques.
Lead halide (APbX3) perovskites, in polycrystalline thin films but also perovskite nanoparticles (NPs) has demonstrated excellent performance to implement a new generation of photovoltaic and photonic devices. The structural characterization of APbX3 thin films using (scanning) transmission electron microscopy ((S)TEM) techniques can provide valuable information that can be used to understand and model their optoelectronic performance and device properties. However, since APbX3 perovskites are soft materials, their characterization using (S)TEM is challenging. Here, we study and compare the structural properties of two different metal halide APbX3 perovskite thin films: bulk CH3NH3PbI3 prep…
MOCVD growth of CdTe on glass: analysis of in situ post-growth annealing
Abstract In this paper, we analyse the growth by MOCVD of CdTe on glass substrates using in situ post-growth annealing. First, in order to perform a systematic study, polycrystalline layers of CdTe were deposited by MOCVD on glass substrates. The structure and morphology of the layers was investigated as a function of different growth parameters, temperature, VI/II precursor molar ratio and substrate position on the susceptor. An activation energy of Ek=20.7 kcal/mol was obtained from the experimental data. In order to better understand the process and the effects of different growth parameters, a numerical model that simulated the gas flow in the reactor, was developed. Secondly we analyse…
Polymer/Perovskite Amplifying Waveguides for Active Hybrid Silicon Photonics
The emission properties of hybrid halide perovskites are exploited to implement a stable and very low power operation waveguide optical amplifier integrated in a silicon platform. By optimizing its design with a poly(methyl methacrylate) (PMMA) encapsulation, this novel photonic device presents a net gain of around 10 dB cm−1 and 3–4 nm linewidth with an energy threshold as low as 2 nJ pulse−1 and exhibiting no degradation after one year. This work was supported by Generalitat Valenciana (Project No. ISIC/2012/008), the Universitat Jaume I (Project No. 12I361.01/1), Spanish MINECO (Projects Nos. MAT2013-47192-C3-1-R and TEC2014-53727-C2-1-R) and EU-NAVOLCHI (Project No. 288869).
Morphology and Band Structure of Orthorhombic PbS Nanoplatelets: An Indirect Band Gap Material
PbS quantum dots and nanoplatelets (NPLs) are of enormous interest in the development of optoelectronic devices. However, some important aspects of their nature remain unclear. Recent studies have revealed that colloidal PbS NPLs may depart from the rock-salt crystal structure of bulk and form an orthorhombic (Pnma) modification instead. To gain insight into the implications of such a change over the optoelectronic properties, we have synthesized orthorhombic PbS NPLs and determined the lattice parameters by means of selected area electron diffraction measurements. We have then calculated the associated band structure using density functional theory with Perdew–Burke–Ernzerhof functional fo…
Interpretation of the photoluminescence decay kinetics in metal halide perovskite nanocrystals and thin polycrystalline films
Abstract In this paper we present critical analysis of different points of view on interpretation of the photoluminescence (PL) decay kinetics in lead halide perovskites prepared in the form of well passivated nanocrystals (PNCs) or thin polycrystalline layers. In addition to the literature data, our own measurements are also considered. For PNCs, a strong dependence of the PL lifetimes on the type of passivating ligand was observed with a consistently high PL quantum yield. It is shown that such ligand effects, as well as a decrease in the PL lifetime with decreasing temperature, are well qualitatively explained by the phenomenological model of thermally activated delayed luminescence, in …
Controlling the Phase Segregation in Mixed Halide Perovskites through Nanocrystal Size
Mixed halide perovskites are one of the promising candidates in developing solar cells and light-emitting diodes (LEDs), among other applications, because of their tunable optical properties. Nonetheless, photoinduced phase segregation, by formation of segregated Br-rich and I-rich domains, limits the overall applicability. We tracked the phase segregation with increasing crystalline size of CsPbBr3–xIx and their photoluminescence under continuous-wave laser irradiation (405 nm, 10 mW cm–2) and observed the occurrence of the phase segregation from the threshold size of 46 ± 7 nm. These results have an outstanding agreement with the diffusion length (45.8 nm) calculated also experimentally f…
Unravelling the Photocatalytic Behavior of All-Inorganic Mixed Halide Perovskites: The Role of Surface Chemical States
Within the most mesmerizing materials in the world of optoelectronics, mixed halide perovskites (MHPs) have been distinguished because of the tunability of their optoelectronic properties, balancing both the light-harvesting efficiency and the charge extraction into highly efficient solar devices. This feature has drawn the attention of analogous hot topics as photocatalysis for carrying out more efficiently the degradation of organic compounds. However, the photo-oxidation ability of perovskite depends not only on its excellent light-harvesting properties but also on the surface chemical environment provided during its synthesis. Accordingly, we studied the role of surface chemical states …
Study of the chemically activated sublimation of ZnSe
Abstract The reactions and processes involved in the growth of ZnSe by chemically activated sublimation in a H 2 atmosphere are studied. The rate of transport as a function of source and substrate temperatures and the difference between them are determined from close spacing vapour transport experiments. According to this process, ZnSe layers are deposited on sapphire substrates by short distance chemically assisted sublimation. The experimental results are analysed and the thermodynamic constants of the transport are determined using a theoretical model for kinetically controlled processes, assuming water to act as sublimation catalyst. A preliminary optical and structural characterisation…