Highly luminescent InP/GaP/ZnS QDs emitting in the entire color range via a heating up process

InP-based quantum dots (QDs) have attracted much attention for use in optical applications, and several types of QDs such as InP/ZnS, InP/ZnSeS, and InP/GaP/ZnS have been developed. However, early synthetic methods that involved rapid injection at high temperatures have not been able to reproducibly produce the required optical properties. They were also not able to support commercialization efforts successfully. Herein, we introduce a simple synthetic method for InP/GaP/ZnS core/shell/shell QDs via a heating process. The reaction was completed within 0.5 h and a full color range from blue to red was achieved. For emitting blue color, t-DDT was applied to prevent particle growth. From green to orange, color variation was achieved by adjusting the quantity of myristic acid. Utilizing large quantities of gallium chloride led to red color. With this method, we produced high-quality InP/GaP/ZnS QDs (blue QY: ~40%, FWHM: 50 nm; green QY: ~85%, FWHM: 41 nm; red QY: ~60%, FWHM: 65 nm). We utilized t-DDT as a new sulfur source. Compared with n-DDT, t-DDT was more reactive, which allowed for the formation of a thicker shell.

[1]  Jaehee Cho,et al.  Preparation of Highly Luminescent Nanocrystals and Their Application to Light‐Emitting Diodes , 2007 .

[2]  Xiaogang Peng,et al.  Formation of high-quality CdTe, CdSe, and CdS nanocrystals using CdO as precursor. , 2001, Journal of the American Chemical Society.

[3]  Gregory D. Scholes,et al.  Controlling the Optical Properties of Inorganic Nanoparticles , 2008 .

[4]  J. McKittrick,et al.  Review: Down Conversion Materials for Solid‐State Lighting , 2014 .

[5]  Jaehyun Park,et al.  CuInS2/ZnS core/shell quantum dots by cation exchange and their blue-shifted photoluminescence , 2011 .

[6]  Eugene A. Fitzgerald,et al.  Relaxed, high-quality InP on GaAs by using InGaAs and InGaP graded buffers to avoid phase separation , 2007 .

[7]  Liang Li,et al.  One-pot synthesis of highly luminescent InP/ZnS nanocrystals without precursor injection. , 2008, Journal of the American Chemical Society.

[8]  Sang-Wook Kim,et al.  Step-Wise Synthesis of InP/ZnS Core−Shell Quantum Dots and the Role of Zinc Acetate , 2009 .

[9]  Moungi G Bawendi,et al.  Ternary I-III-VI quantum dots luminescent in the red to near-infrared. , 2008, Journal of the American Chemical Society.

[10]  Eun Kyung Lee,et al.  Full-colour quantum dot displays fabricated by transfer printing , 2011 .

[11]  Tae‐Woo Lee,et al.  Electrospun polymer/quantum dot composite fibers as down conversion phosphor layers for white light-emitting diodes , 2014 .

[12]  Arthur J. Nozik,et al.  Size-Dependent Spectroscopy of InP Quantum Dots , 1997 .

[13]  V. Bulović,et al.  Color-saturated green-emitting QD-LEDs. , 2006, Angewandte Chemie.

[14]  R. Friend,et al.  Blue-Green Color Tunable Solution Processable Organolead Chloride–Bromide Mixed Halide Perovskites for Optoelectronic Applications , 2015, Nano letters.

[15]  Norris,et al.  Measurement of the size dependent hole spectrum in CdSe quantum dots. , 1994, Physical review letters.

[16]  R. Waser,et al.  Understanding the role of single molecular ZnS precursors in the synthesis of In(Zn)P/ZnS nanocrystals. , 2014, ACS applied materials & interfaces.

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

[18]  J. Parisi,et al.  Size and shape control of colloidal copper(I) sulfide nanorods. , 2012, ACS nano.

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

[20]  Liang Li,et al.  Highly Luminescent CuInS2/ZnS Core/Shell Nanocrystals: Cadmium-Free Quantum Dots for In Vivo Imaging , 2009 .

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

[22]  David Battaglia,et al.  Colloidal InP nanocrystals as efficient emitters covering blue to near-infrared. , 2007, Journal of the American Chemical Society.

[23]  H. Martínez,et al.  InP/ZnS nanocrystals: coupling NMR and XPS for fine surface and interface description. , 2012, Journal of the American Chemical Society.

[24]  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.

[25]  B. Cossairt,et al.  Role of Acid in Precursor Conversion During InP Quantum Dot Synthesis , 2013 .

[26]  J. Parisi,et al.  Synthesis and shape control of CuInS(2) nanoparticles. , 2010, Journal of the American Chemical Society.

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

[28]  Maity Gouranga,et al.  COMPREHENSIVE STUDY OF , 2018 .

[29]  O. Kwon,et al.  Origin of photoluminescence from colloidal gallium phosphide nanocrystals synthesized via a hot-injection method , 2015 .

[30]  Andreas Kornowski,et al.  Highly Luminescent Monodisperse CdSe and CdSe/ZnS Nanocrystals Synthesized in a Hexadecylamine-Trioctylphosphine Oxide-Trioctylphospine Mixture. , 2001, Nano letters.

[31]  Sandeep Kumar Pathak,et al.  Perovskite Crystals for Tunable White Light Emission , 2015 .

[32]  Nathan T. Shewmon,et al.  High-efficiency, low turn-on voltage blue-violet quantum-dot-based light-emitting diodes. , 2015, Nano letters.

[33]  Heesun Yang,et al.  Efficient White-Light-Emitting Diodes Fabricated from Highly Fluorescent Copper Indium Sulfide Core/Shell Quantum Dots , 2012 .

[34]  Weidong Yang,et al.  Shape control of CdSe nanocrystals , 2000, Nature.

[35]  S. Billinge,et al.  Two-Step Nucleation and Growth of InP Quantum Dots via Magic-Sized Cluster Intermediates , 2015 .

[36]  Wenhao Liu,et al.  Quantum Dots for LED Downconversion in Display Applications , 2013 .

[37]  Shuming Nie,et al.  Semiconductor nanocrystals: structure, properties, and band gap engineering. , 2010, Accounts of chemical research.

[38]  M. Bawendi,et al.  (CdSe)ZnS Core-Shell Quantum Dots - Synthesis and Characterization of a Size Series of Highly Luminescent Nanocrystallites , 1997 .

[39]  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.

[40]  P. J. van der Zaag,et al.  Temperature Dependence of the Photoluminescence of InP/ZnS Quantum Dots , 2008 .

[41]  M. Bawendi,et al.  Mechanistic insights into the formation of InP quantum dots. , 2009, Angewandte Chemie.

[42]  A. Cornejo,et al.  Surface chemistry of InP quantum dots: a comprehensive study. , 2010, Journal of the American Chemical Society.