Solvent‐Polarity‐Engineered Controllable Synthesis of Highly Fluorescent Cesium Lead Halide Perovskite Quantum Dots and Their Use in White Light‐Emitting Diodes

Cesium lead halide quantum dots (QDs) have tunable photoluminescence that is capable of covering the entire visible spectrum and have high quantum yields, which make them a new fluorescent materials for various applications. Here, the synthesis of CsPbX3 (X = Cl, Br, I, or mixed Cl/Br and Br/I) QDs by direct ion reactions in ether solvents is reported, and for the first time the synergetic effects of solvent polarity and reaction temperature on the nucleation and growth of QDs are demonstrated. The use of solvent with a low polarity enables controlled growth of QDs, which facilitates the synthesis of high‐quality CsPbX3 QDs with broadly tunable luminescence, narrow emission width, and high quantum yield. A QD white LED (WLED) is demonstrated by coating the highly fluorescent green‐emissive CsPbBr3 QDs together with red phosphors on a blue InGaN chip, which presents excellent warm white light emission with a high rendering index of 93.2 and color temperature of 5447 K, suggesting the potential applications of highly fluorescent cesium lead halide perovskite QDs as an alternative color converter in the fabrication of WLEDs.

[1]  C. K. Møller.  Crystal Structure and Photoconductivity of Cæsium Plumbohalides , 1958 .

[2]  P. Bowen,et al.  Precipitation of Self-Organized Copper Oxalate Polycrystalline Particles in the Presence of Hydroxypropylmethylcellulose (HPMC): Control of Morphology , 2000 .

[3]  Yadong Yin,et al.  Colloidal nanocrystal synthesis and the organic–inorganic interface , 2005, Nature.

[4]  F. Huang,et al.  Progress of nanocrystalline growth kinetics based on oriented attachment. , 2010, Nanoscale.

[5]  M. Kovalenko,et al.  Prospects of colloidal nanocrystals for electronic and optoelectronic applications. , 2010, Chemical reviews.

[6]  T. Hyeon,et al.  Formation mechanisms of uniform nanocrystals via hot-injection and heat-up methods. , 2011, Small.

[7]  R. L. Penn,et al.  Effect of Ionic Strength on the Kinetics of Crystal Growth by Oriented Aggregation , 2012 .

[8]  Jillian F Banfield,et al.  Direction-Specific Interactions Control Crystal Growth by Oriented Attachment , 2012, Science.

[9]  V. Bulović,et al.  Emergence of colloidal quantum-dot light-emitting technologies , 2012, Nature Photonics.

[10]  Yugang Zhang,et al.  High quantum-yield CdSexS1−x/ZnS core/shell quantum dots for warm white light-emitting diodes with good color rendering , 2013, Nanotechnology.

[11]  A. Rogach,et al.  Quantum dot field effect transistors , 2013 .

[12]  Cuong Dang,et al.  Light Extraction Efficiency Enhancement of Colloidal Quantum Dot Light‐Emitting Diodes Using Large‐Scale Nanopillar Arrays , 2014 .

[13]  Nguyen T. K. Thanh,et al.  Mechanisms of nucleation and growth of nanoparticles in solution. , 2014, Chemical reviews.

[14]  Olga Malinkiewicz,et al.  Nontemplate synthesis of CH3NH3PbBr3 perovskite nanoparticles. , 2014, Journal of the American Chemical Society.

[15]  Shawn P. Shields,et al.  Kinetics and Mechanisms of Aggregative Nanocrystal Growth , 2014 .

[16]  Yizheng Jin,et al.  Solution-processed, high-performance light-emitting diodes based on quantum dots , 2014, Nature.

[17]  J. Bisquert,et al.  High-efficiency "green" quantum dot solar cells. , 2014, Journal of the American Chemical Society.

[18]  Inverted quantum-dot solar cells with depleted heterojunction structure employing CdS as the electron acceptor , 2015 .

[19]  H. Zeng,et al.  Quantum Dot Light‐Emitting Diodes Based on Inorganic Perovskite Cesium Lead Halides (CsPbX3) , 2015, Advanced materials.

[20]  Cherie R. Kagan,et al.  Prospects of nanoscience with nanocrystals. , 2015, ACS nano.

[21]  Tianquan Lian,et al.  Ultrafast Interfacial Electron and Hole Transfer from CsPbBr3 Perovskite Quantum Dots. , 2015, Journal of the American Chemical Society.

[22]  A Paul Alivisatos,et al.  Highly Luminescent Colloidal Nanoplates of Perovskite Cesium Lead Halide and Their Oriented Assemblies. , 2015, Journal of the American Chemical Society.

[23]  Jiating He,et al.  Thermodynamics versus kinetics in nanosynthesis. , 2015, Angewandte Chemie.

[24]  S. Haigh,et al.  Near-Unity Quantum Yields from Chloride Treated CdTe Colloidal Quantum Dots , 2014, Small.

[25]  E. Sargent,et al.  Colloidal quantum dot solar cells , 2012, Nature Photonics.

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

[27]  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.

[28]  Oleksandr Voznyy,et al.  Efficient Luminescence from Perovskite Quantum Dot Solids. , 2015, ACS applied materials & interfaces.

[29]  H. Zeng,et al.  All‐Inorganic Colloidal Perovskite Quantum Dots: A New Class of Lasing Materials with Favorable Characteristics , 2015, Advanced materials.

[30]  A. Vomiero,et al.  Metal oxide semiconductors for dye- and quantum-dot-sensitized solar cells. , 2015, Small.

[31]  Liberato Manna,et al.  Tuning the Optical Properties of Cesium Lead Halide Perovskite Nanocrystals by Anion Exchange Reactions , 2015, Journal of the American Chemical Society.

[32]  M. Kovalenko,et al.  Fast Anion-Exchange in Highly Luminescent Nanocrystals of Cesium Lead Halide Perovskites (CsPbX3, X = Cl, Br, I) , 2015, Nano letters.

[33]  Guopeng Li,et al.  A water–ethanol phase assisted co-precipitation approach toward high quality quantum dot–inorganic salt composites and their application for WLEDs , 2015 .

[34]  Shaojun Guo,et al.  Room Temperature Single-Photon Emission from Individual Perovskite Quantum Dots. , 2015, ACS nano.

[35]  J. Pérez‐Prieto,et al.  Maximizing the emissive properties of CH3NH3PbBr3 perovskite nanoparticles , 2015 .

[36]  Haizheng Zhong,et al.  Brightly Luminescent and Color-Tunable Colloidal CH3NH3PbX3 (X = Br, I, Cl) Quantum Dots: Potential Alternatives for Display Technology. , 2015, ACS nano.

[37]  H. Zeng,et al.  Healing All‐Inorganic Perovskite Films via Recyclable Dissolution–Recyrstallization for Compact and Smooth Carrier Channels of Optoelectronic Devices with High Stability , 2016 .

[38]  Oleksandr Isaienko,et al.  Spectral and Dynamical Properties of Single Excitons, Biexcitons, and Trions in Cesium-Lead-Halide Perovskite Quantum Dots. , 2016, Nano letters.

[39]  Min-Sang Lee,et al.  All-inorganic cesium lead halide perovskite nanocrystals for photodetector applications. , 2016, Chemical communications.

[40]  Weida Hu,et al.  Generalized colloidal synthesis of high-quality, two-dimensional cesium lead halide perovskite nanosheets and their applications in photodetectors. , 2016, Nanoscale.

[41]  Andrew J. deMello,et al.  Synthesis of Cesium Lead Halide Perovskite Nanocrystals in a Droplet-Based Microfluidic Platform: Fast Parametric Space Mapping. , 2016, Nano letters.

[42]  Yu Zhang,et al.  Enhancing the Brightness of Cesium Lead Halide Perovskite Nanocrystal Based Green Light-Emitting Devices through the Interface Engineering with Perfluorinated Ionomer. , 2016, Nano letters.

[43]  H. Zeng,et al.  Nonlinear Absorption and Low-Threshold Multiphoton Pumped Stimulated Emission from All-Inorganic Perovskite Nanocrystals. , 2016, Nano letters.

[44]  H. Zeng,et al.  CsPbX3 Quantum Dots for Lighting and Displays: Room‐Temperature Synthesis, Photoluminescence Superiorities, Underlying Origins and White Light‐Emitting Diodes , 2016 .

[45]  Aifei Wang,et al.  Ligand-Mediated Synthesis of Shape-Controlled Cesium Lead Halide Perovskite Nanocrystals via Reprecipitation Process at Room Temperature. , 2016, ACS nano.