High-Efficiency Polycrystalline Perovskite Light-Emitting Diodes Based on Mixed Cations.

We have achieved high-efficiency polycrystalline perovskite light-emitting diodes (PeLEDs) based on formamidinium (FA) and cesium (Cs) mixed cations without quantum dot synthesis. Uniform single-phase FA1- xCs xPbBr3 polycrystalline films were fabricated by one-step formation with various FA:Cs molar proportions; then the influences of chemical composition on film morphology, crystal structure, photoluminescence (PL), and electroluminescence (EL) were systematically investigated. Incorporation of Cs+ cations in FAPbBr3 significantly reduced the average grain size (to 199 nm for FA:Cs = 90:10) and trap density; these changes consequently increased PL quantum efficiency (PLQE) and PL lifetime of FA1- xCs xPbBr3 films and current efficiency (CE) of PeLEDs. Further increase in Cs molar proportion from 10 mol % decreased crystallinity and purity, increased trap density, and correspondingly decreased PLQE, PL lifetime, and CE. Incorporation of Cs also increased photostability of FA1- xCs xPbBr3 films, possibly due to suppressed formation of light-induced metastable states. FA1- xCs xPbBr3 PeLEDs show the maximum CE = 14.5 cd A-1 at FA:Cs = 90:10 with very narrow EL spectral width (21-24 nm); this is the highest CE among FA-Cs-based PeLEDs reported to date. This work provides an understanding of the influences of Cs incorporation on the chemical, structural, and luminescent properties of FAPbBr3 polycrystalline films and a breakthrough to increase the efficiency of FA1- xCs xPbBr3 PeLEDs.

[1]  Junsheng Yu,et al.  Phase Engineering for Highly Efficient Quasi-Two-Dimensional All-Inorganic Perovskite Light-Emitting Diodes via Adjusting the Ratio of Cs Cation , 2019, Nanoscale Research Letters.

[2]  Christoph Wolf,et al.  Improving the Stability of Metal Halide Perovskite Materials and Light‐Emitting Diodes , 2018, Advanced materials.

[3]  W. Stark,et al.  Ultrapure Green Light-Emitting Diodes Using Two-Dimensional Formamidinium Perovskites: Achieving Recommendation 2020 Color Coordinates. , 2017, Nano letters.

[4]  H. Boyen,et al.  Band Gap Tuning via Lattice Contraction and Octahedral Tilting in Perovskite Materials for Photovoltaics. , 2017, Journal of the American Chemical Society.

[5]  Woosung Kwon,et al.  High efficiency perovskite light-emitting diodes of ligand-engineered colloidal formamidinium lead bromide nanoparticles , 2017 .

[6]  S. Yoo,et al.  Universal high work function flexible anode for simplified ITO-free organic and perovskite light-emitting diodes with ultra-high efficiency , 2017 .

[7]  R. Friend,et al.  Highly Efficient Light-Emitting Diodes of Colloidal Metal-Halide Perovskite Nanocrystals beyond Quantum Size. , 2017, ACS nano.

[8]  Joo Sung Kim,et al.  High‐Efficiency Solution‐Processed Inorganic Metal Halide Perovskite Light‐Emitting Diodes , 2017, Advanced materials.

[9]  Oleksandr Voznyy,et al.  Tailoring the Energy Landscape in Quasi-2D Halide Perovskites Enables Efficient Green-Light Emission. , 2017, Nano letters.

[10]  R. Friend,et al.  Amine-Based Passivating Materials for Enhanced Optical Properties and Performance of Organic-Inorganic Perovskites in Light-Emitting Diodes. , 2017, The journal of physical chemistry letters.

[11]  B. Rand,et al.  In Situ Preparation of Metal Halide Perovskite Nanocrystal Thin Films for Improved Light-Emitting Devices. , 2017, ACS nano.

[12]  Min-ho Park,et al.  Efficient Flexible Organic/Inorganic Hybrid Perovskite Light‐Emitting Diodes Based on Graphene Anode , 2017, Advanced materials.

[13]  Bo Wang,et al.  Morphology Evolution and Degradation of CsPbBr3 Nanocrystals under Blue Light-Emitting Diode Illumination. , 2017, ACS applied materials & interfaces.

[14]  Dong Hoe Kim,et al.  Do grain boundaries dominate non-radiative recombination in CH3NH3PbI3 perovskite thin films? , 2017, Physical chemistry chemical physics : PCCP.

[15]  Barry P Rand,et al.  Efficient perovskite light-emitting diodes featuring nanometre-sized crystallites , 2017, Nature Photonics.

[16]  Jay B. Patel,et al.  Photovoltaic mixed-cation lead mixed-halide perovskites: links between crystallinity, photo-stability and electronic properties , 2017 .

[17]  Ho Won Jang,et al.  Investigation of Energy Levels and Crystal Structures of Cesium Lead Halides and Their Application in Full‐Color Light‐Emitting Diodes , 2017 .

[18]  W. Tisdale,et al.  Tunable Light-Emitting Diodes Utilizing Quantum-Confined Layered Perovskite Emitters , 2017 .

[19]  Hybrid Perovskite Light-Emitting Diodes Based on Perovskite Nanocrystals with Organic-Inorganic Mixed Cations. , 2017, Advanced materials.

[20]  Gang Li,et al.  Pure Formamidinium‐Based Perovskite Light‐Emitting Diodes with High Efficiency and Low Driving Voltage , 2017, Advanced materials.

[21]  H. Demir,et al.  High brightness formamidinium lead bromide perovskite nanocrystal light emitting devices , 2016, Scientific Reports.

[22]  Nana Wang,et al.  Perovskite light-emitting diodes based on solution-processed self-organized multiple quantum wells , 2016, Nature Photonics.

[23]  H. Demir,et al.  Solution-processed highly bright and durable cesium lead halide perovskite light-emitting diodes. , 2016, Nanoscale.

[24]  Anders Hagfeldt,et al.  Incorporation of rubidium cations into perovskite solar cells improves photovoltaic performance , 2016, Science.

[25]  M. Weller,et al.  Phase behaviour and composition in the formamidinium–methylammonium hybrid lead iodide perovskite solid solution , 2016 .

[26]  Oleksandr Voznyy,et al.  Perovskite energy funnels for efficient light-emitting diodes. , 2016, Nature nanotechnology.

[27]  Himchan Cho,et al.  Metal halide perovskite light emitters , 2016, Proceedings of the National Academy of Sciences.

[28]  Himchan Cho,et al.  Effects of thermal treatment on organic-inorganic hybrid perovskite films and luminous efficiency of light-emitting diodes , 2016 .

[29]  Richard H. Friend,et al.  Efficient Visible Quasi‐2D Perovskite Light‐Emitting Diodes , 2016, Advanced materials.

[30]  Xi Yuan,et al.  Temperature-dependent photoluminescence of inorganic perovskite nanocrystal films , 2016 .

[31]  Oleksandr Voznyy,et al.  Highly Efficient Perovskite‐Quantum‐Dot Light‐Emitting Diodes by Surface Engineering , 2016, Advanced materials.

[32]  David S. Ginger,et al.  Photoluminescence Lifetimes Exceeding 8 μs and Quantum Yields Exceeding 30% in Hybrid Perovskite Thin Films by Ligand Passivation , 2016 .

[33]  Wentao Xu,et al.  Organometal Halide Perovskite Artificial Synapses , 2016, Advanced materials.

[34]  Claudine Katan,et al.  Light-activated photocurrent degradation and self-healing in perovskite solar cells , 2016, Nature Communications.

[35]  P. Pikhitsa,et al.  Trapped charge-driven degradation of perovskite solar cells , 2016, Nature Communications.

[36]  Ayan A. Zhumekenov,et al.  Formamidinium Lead Halide Perovskite Crystals with Unprecedented Long Carrier Dynamics and Diffusion Length , 2016 .

[37]  Prashant V Kamat,et al.  How Lead Halide Complex Chemistry Dictates the Composition of Mixed Halide Perovskites. , 2016, The journal of physical chemistry letters.

[38]  Shangfeng Yang,et al.  Crystallinity and defect state engineering in organo-lead halide perovskite for high-efficiency solar cells , 2016 .

[39]  M. Green,et al.  Mobile Ion Induced Slow Carrier Dynamics in Organic-Inorganic Perovskite CH₃NH₃PbBr₃. , 2016, ACS applied materials & interfaces.

[40]  S. Chang,et al.  A perovskite cell with a record-high-V(oc) of 1.61 V based on solvent annealed CH3NH3PbBr3/ICBA active layer. , 2016, Nanoscale.

[41]  Ursula Rothlisberger,et al.  Entropic stabilization of mixed A-cation ABX3 metal halide perovskites for high performance perovskite solar cells , 2016 .

[42]  Yongbo Yuan,et al.  Ion Migration in Organometal Trihalide Perovskite and Its Impact on Photovoltaic Efficiency and Stability. , 2016, Accounts of chemical research.

[43]  M. Roeffaers,et al.  Degradation of Methylammonium Lead Iodide Perovskite Structures through Light and Electron Beam Driven Ion Migration , 2016, The journal of physical chemistry letters.

[44]  S. Gradečak,et al.  Impacts of Ion Segregation on Local Optical Properties in Mixed Halide Perovskite Films. , 2016, Nano letters.

[45]  Huijun Zhao,et al.  Functionalization of perovskite thin films with moisture-tolerant molecules , 2016, Nature Energy.

[46]  J. Berry,et al.  Stabilizing Perovskite Structures by Tuning Tolerance Factor: Formation of Formamidinium and Cesium Lead Iodide Solid-State Alloys , 2016 .

[47]  Bernd Rech,et al.  A mixed-cation lead mixed-halide perovskite absorber for tandem solar cells , 2016, Science.

[48]  David Cahen,et al.  Cesium Enhances Long-Term Stability of Lead Bromide Perovskite-Based Solar Cells. , 2015, The journal of physical chemistry letters.

[49]  Abhishek Swarnkar,et al.  Colloidal CsPbBr3 Perovskite Nanocrystals: Luminescence beyond Traditional Quantum Dots. , 2015, Angewandte Chemie.

[50]  Richard H. Friend,et al.  Overcoming the electroluminescence efficiency limitations of perovskite light-emitting diodes , 2015, Science.

[51]  Nam-Gyu Park,et al.  Stability Issues on Perovskite Solar Cells , 2015 .

[52]  H. Demir,et al.  Inorganic Halide Perovskites for Efficient Light-Emitting Diodes. , 2015, The journal of physical chemistry letters.

[53]  Sung Min Cho,et al.  Formamidinium and Cesium Hybridization for Photo‐ and Moisture‐Stable Perovskite Solar Cell , 2015 .

[54]  Kaibo Zheng,et al.  Mechanistic insights into perovskite photoluminescence enhancement: light curing with oxygen can boost yield thousandfold. , 2015, Physical chemistry chemical physics : PCCP.

[55]  Alain Goriely,et al.  High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization , 2015, Nature Communications.

[56]  Sang Il Seok,et al.  High-performance photovoltaic perovskite layers fabricated through intramolecular exchange , 2015, Science.

[57]  A. Zaban,et al.  Photoinduced Reversible Structural Transformations in Free-Standing CH3NH3PbI3 Perovskite Films. , 2015, The journal of physical chemistry letters.

[58]  Michael C. Heiber,et al.  Identification of Trap States in Perovskite Solar Cells. , 2015, The journal of physical chemistry letters.

[59]  Shinuk Cho,et al.  High‐Performance Planar Perovskite Optoelectronic Devices: A Morphological and Interfacial Control by Polar Solvent Treatment , 2015, Advanced materials.

[60]  D. Ginger,et al.  Impact of microstructure on local carrier lifetime in perovskite solar cells , 2015, Science.

[61]  H. Snaith,et al.  Direct measurement of the exciton binding energy and effective masses for charge carriers in organic–inorganic tri-halide perovskites , 2015, Nature Physics.

[62]  Chang-Lyoul Lee,et al.  Multicolored Organic/Inorganic Hybrid Perovskite Light‐Emitting Diodes , 2015, Advanced materials.

[63]  T. Han,et al.  Elucidating the crucial role of hole injection layer in degradation of organic light-emitting diodes. , 2015, ACS applied materials & interfaces.

[64]  Christopher H. Hendon,et al.  Nanocrystals of Cesium Lead Halide Perovskites (CsPbX3, X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut , 2015, Nano letters.

[65]  Felix Deschler,et al.  Bright light-emitting diodes based on organometal halide perovskite. , 2014, Nature nanotechnology.

[66]  W. Geng,et al.  First-Principles Study of Lead Iodide Perovskite Tetragonal and Orthorhombic Phases for Photovoltaics , 2014 .

[67]  Thomas Bein,et al.  Efficient Planar Heterojunction Perovskite Solar Cells Based on Formamidinium Lead Bromide. , 2014, The journal of physical chemistry letters.

[68]  P. Umari,et al.  Cation-induced band-gap tuning in organohalide perovskites: interplay of spin-orbit coupling and octahedra tilting. , 2014, Nano letters.

[69]  Nripan Mathews,et al.  Low-temperature solution-processed wavelength-tunable perovskites for lasing. , 2014, Nature materials.

[70]  Zhifu Liu,et al.  Crystal Growth of the Perovskite Semiconductor CsPbBr3: A New Material for High-Energy Radiation Detection , 2013 .

[71]  Richard H. Friend,et al.  An improved experimental determination of external photoluminescence quantum efficiency , 1997 .

[72]  Jay R. Knutson,et al.  Simultaneous analysis of multiple fluorescence decay curves: A global approach , 1983 .