Efficient Solid‐State Light‐Emitting CuCdS Nanocrystals Synthesized in Air

Khan, Ali Hossain; Dalui, Amit; Mukherjee, Soham; Segre, Carlo U.; Sarma, D. D.; Acharya, Somobrata

doi:10.1002/anie.201409518

Title: Efficient Solid‐State Light‐Emitting CuCdS Nanocrystals Synthesized in Air

Abstract

Abstract Semiconductor nanocrystals (NCs) possess high photoluminescence (PL) typically in the solution phase. In contrary, PL rapidly quenches in the solid state. Efficient solid state luminescence can be achieved by inducing a large Stokes shift. Here we report on a novel synthesis of compositionally controlled CuCdS NCs in air avoiding the usual complexity of using inert atmosphere. These NCs show long‐range color tunability over the entire visible range with a remarkable Stokes shift up to about 1.25 eV. Overcoating the NCs leads to a high solid‐state PL quantum yield (QY) of ca. 55 % measured by using an integrating sphere. Unique charge carrier recombination mechanisms have been recognized from the NCs, which are correlated to the internal NC structure probed by using extended X‐ray absorption fine structure (EXAFS) spectroscopy. EXAFS measurements show a Cu‐rich surface and Cd‐rich interior with 46 % Cu ^I being randomly distributed within 84 % of the NC volume creating additional transition states for PL. Color‐tunable solid‐state luminescence remains stable in air enabling fabrication of light‐emitting diodes (LEDs).

Authors:: Khan, Ali Hossain; Dalui, Amit; Mukherjee, Soham; Segre, Carlo U.; Sarma, D. D.; Acharya, Somobrata

Publication Date:: Fri Jan 16 00:00:00 EST 2015

Sponsoring Org.:: USDOE

OSTI Identifier:: 1464386

Grant/Contract Number:: DE‐AC02‐06CH11357

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Angewandte Chemie (International Edition)

Additional Journal Information:: Journal Name: Angewandte Chemie (International Edition) Journal Volume: 54 Journal Issue: 9; Journal ID: ISSN 1433-7851

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Khan, Ali Hossain, Dalui, Amit, Mukherjee, Soham, Segre, Carlo U., Sarma, D. D., and Acharya, Somobrata. Efficient Solid‐State Light‐Emitting CuCdS Nanocrystals Synthesized in Air.  Germany: N. p., 2015. 
Web.  doi:10.1002/anie.201409518.

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                    Khan, Ali Hossain, Dalui, Amit, Mukherjee, Soham, Segre, Carlo U., Sarma, D. D., & Acharya, Somobrata. Efficient Solid‐State Light‐Emitting CuCdS Nanocrystals Synthesized in Air.  Germany.  https://doi.org/10.1002/anie.201409518

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                    Khan, Ali Hossain, Dalui, Amit, Mukherjee, Soham, Segre, Carlo U., Sarma, D. D., and Acharya, Somobrata. Fri .  
"Efficient Solid‐State Light‐Emitting CuCdS Nanocrystals Synthesized in Air".  Germany.  https://doi.org/10.1002/anie.201409518.

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@article{osti_1464386,

  title        = {Efficient Solid‐State Light‐Emitting CuCdS Nanocrystals Synthesized in Air},

  author       = {Khan, Ali Hossain and Dalui, Amit and Mukherjee, Soham and Segre, Carlo U. and Sarma, D. D. and Acharya, Somobrata},

  abstractNote = {Abstract Semiconductor nanocrystals (NCs) possess high photoluminescence (PL) typically in the solution phase. In contrary, PL rapidly quenches in the solid state. Efficient solid state luminescence can be achieved by inducing a large Stokes shift. Here we report on a novel synthesis of compositionally controlled CuCdS NCs in air avoiding the usual complexity of using inert atmosphere. These NCs show long‐range color tunability over the entire visible range with a remarkable Stokes shift up to about 1.25 eV. Overcoating the NCs leads to a high solid‐state PL quantum yield (QY) of ca. 55 % measured by using an integrating sphere. Unique charge carrier recombination mechanisms have been recognized from the NCs, which are correlated to the internal NC structure probed by using extended X‐ray absorption fine structure (EXAFS) spectroscopy. EXAFS measurements show a Cu‐rich surface and Cd‐rich interior with 46 % Cu I being randomly distributed within 84 % of the NC volume creating additional transition states for PL. Color‐tunable solid‐state luminescence remains stable in air enabling fabrication of light‐emitting diodes (LEDs).},

  doi          = {10.1002/anie.201409518},

  journal      = {Angewandte Chemie (International Edition)},

  number       = 9,

  volume       = 54,

  place        = {Germany},

  year         = {Fri Jan 16 00:00:00 EST 2015},

  month        = {Fri Jan 16 00:00:00 EST 2015}

}

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Title: Efficient Solid‐State Light‐Emitting CuCdS Nanocrystals Synthesized in Air

Abstract

Citation Formats

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT journal, June 2005

Synthesis and characterization of nearly monodisperse CdE (E = sulfur, selenium, tellurium) semiconductor nanocrystallites journal, September 1993

Electronic Energy Transfer in CdSe Quantum Dot Solids journal, February 1996

Investigation of the Internal Heterostructure of Highly Luminescent Quantum Dot−Quantum Well Nanocrystals journal, January 2009

Emergence of colloidal quantum-dot light-emitting technologies journal, December 2012

Composition-Tunable Alloyed Semiconductor Nanocrystals journal, May 2010

Color-Saturated Green-Emitting QD-LEDs journal, September 2006

Compositionally Tunable Photoluminescence Emission in Cu 2 ZnSn(S 1− x Se x ) 4 Nanocrystals journal, June 2013

Self-Purification in Semiconductor Nanocrystals journal, June 2006

Electroluminescence from single monolayers of nanocrystals in molecular organic devices journal, December 2002

Light-emitting diodes made from cadmium selenide nanocrystals and a semiconducting polymer journal, August 1994

Leuchtdioden mit Halbleiternanokristallen journal, August 2008

Copper-Doped Inverted Core/Shell Nanocrystals with “Permanent” Optically Active Holes journal, November 2011

Bright infrared quantum-dot light-emitting diodes through inter-dot spacing control journal, May 2012

EXAFS: Basic Principles and Data Analysis book, January 1986

Bright and Stable Alloy Core/Multishell Quantum Dots journal, November 2012

Size-Dependent Optical Properties of Colloidal PbS Quantum Dots journal, September 2009

High near-infrared photoluminescence quantum efficiency from PbS nanocrystals in polymer films journal, February 2005

Giant Nanocrystal Quantum Dots: Stable Down-Conversion Phosphors that Exploit a Large Stokes Shift and Efficient Shell-to-Core Energy Relaxation journal, May 2012

Formation of High-Quality I−III−VI Semiconductor Nanocrystals by Tuning Relative Reactivity of Cationic Precursors journal, April 2009

Using Shape to Control Photoluminescence from CdSe/CdS Core/Shell Nanorods journal, May 2011

Highly Efficient Blue–Green Quantum Dot Light-Emitting Diodes Using Stable Low-Cadmium Quaternary-Alloy ZnCdSSe/ZnS Core/Shell Nanocrystals journal, May 2013

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Chemistry and Properties of Nanocrystals of Different Shapes journal, April 2005

Investigation on Photovoltaic Performance based on Matchstick-Like Cu2S–In2S3 Heterostructure Nanocrystals and Polymer journal, October 2008

Formation of High-Quality CdS and Other II-VI Semiconductor Nanocrystals in Noncoordinating Solvents: Tunable Reactivity of Monomers journal, July 2002

Formation of High-Quality CdS and Other II-VI Semiconductor Nanocrystals in Noncoordinating Solvents: Tunable Reactivity of Monomers journal, July 2002

Tuning the Luminescence Properties of Colloidal I–III–VI Semiconductor Nanocrystals for Optoelectronics and Biotechnology Applications journal, October 2012

Atomic Positional Versus Electronic Order in Semiconducting ZnSe Nanoparticles journal, September 2009

Electron–electron and electron‐hole interactions in small semiconductor crystallites: The size dependence of the lowest excited electronic state journal, May 1984

Color-Saturated Green-Emitting QD-LEDs journal, September 2006

Prospects of Colloidal Nanocrystals for Electronic and Optoelectronic Applications journal, January 2010

Light-Emitting Diodes with Semiconductor Nanocrystals journal, August 2008

‘Giant’ CdSe/CdS Core/Shell Nanocrystal Quantum Dots As Efficient Electroluminescent Materials: Strong Influence of Shell Thickness on Light-Emitting Diode Performance journal, December 2011

Electroluminescence from heterostructures of poly(phenylene vinylene) and inorganic CdSe nanocrystals journal, June 1998

Synthesis, Structural, and Optical Properties of Stable ZnS:Cu,Cl Nanocrystals † journal, April 2009

IFEFFIT : interactive XAFS analysis and FEFF fitting journal, March 2001

Bright and Stable Alloy Core/Multishell Quantum Dots journal, November 2012

Compositionally Tunable Photoluminescence Emission in Cu 2 ZnSn(S 1− x Se x ) 4 Nanocrystals journal, June 2013

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ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
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Synthesis and characterization of nearly monodisperse CdE (E = sulfur, selenium, tellurium) semiconductor nanocrystallites
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Electronic Energy Transfer in CdSe Quantum Dot Solids
journal, February 1996

Investigation of the Internal Heterostructure of Highly Luminescent Quantum Dot−Quantum Well Nanocrystals
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Emergence of colloidal quantum-dot light-emitting technologies
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Composition-Tunable Alloyed Semiconductor Nanocrystals
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Compositionally Tunable Photoluminescence Emission in Cu ₂ ZnSn(S _{1− x} Se _x ) ₄ Nanocrystals
journal, June 2013

Self-Purification in Semiconductor Nanocrystals
journal, June 2006

Electroluminescence from single monolayers of nanocrystals in molecular organic devices
journal, December 2002

Light-emitting diodes made from cadmium selenide nanocrystals and a semiconducting polymer
journal, August 1994

Leuchtdioden mit Halbleiternanokristallen
journal, August 2008

Copper-Doped Inverted Core/Shell Nanocrystals with “Permanent” Optically Active Holes
journal, November 2011

Bright infrared quantum-dot light-emitting diodes through inter-dot spacing control
journal, May 2012

EXAFS: Basic Principles and Data Analysis
book, January 1986

Bright and Stable Alloy Core/Multishell Quantum Dots
journal, November 2012

Size-Dependent Optical Properties of Colloidal PbS Quantum Dots
journal, September 2009

High near-infrared photoluminescence quantum efficiency from PbS nanocrystals in polymer films
journal, February 2005

Giant Nanocrystal Quantum Dots: Stable Down-Conversion Phosphors that Exploit a Large Stokes Shift and Efficient Shell-to-Core Energy Relaxation
journal, May 2012

Formation of High-Quality I−III−VI Semiconductor Nanocrystals by Tuning Relative Reactivity of Cationic Precursors
journal, April 2009

Using Shape to Control Photoluminescence from CdSe/CdS Core/Shell Nanorods
journal, May 2011

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journal, March 2002

Chemistry and Properties of Nanocrystals of Different Shapes
journal, April 2005

Investigation on Photovoltaic Performance based on Matchstick-Like Cu2S–In2S3 Heterostructure Nanocrystals and Polymer
journal, October 2008

Formation of High-Quality CdS and Other II-VI Semiconductor Nanocrystals in Noncoordinating Solvents: Tunable Reactivity of Monomers
journal, July 2002

Formation of High-Quality CdS and Other II-VI Semiconductor Nanocrystals in Noncoordinating Solvents: Tunable Reactivity of Monomers
journal, July 2002

Tuning the Luminescence Properties of Colloidal I–III–VI Semiconductor Nanocrystals for Optoelectronics and Biotechnology Applications
journal, October 2012

Atomic Positional Versus Electronic Order in Semiconducting ZnSe Nanoparticles
journal, September 2009

Electron–electron and electron‐hole interactions in small semiconductor crystallites: The size dependence of the lowest excited electronic state
journal, May 1984

Color-Saturated Green-Emitting QD-LEDs
journal, September 2006

Prospects of Colloidal Nanocrystals for Electronic and Optoelectronic Applications
journal, January 2010

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journal, December 2011

Electroluminescence from heterostructures of poly(phenylene vinylene) and inorganic CdSe nanocrystals
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IFEFFIT : interactive XAFS analysis and FEFF fitting
journal, March 2001

Bright and Stable Alloy Core/Multishell Quantum Dots
journal, November 2012

Compositionally Tunable Photoluminescence Emission in Cu ₂ ZnSn(S _{1− x} Se _x ) ₄ Nanocrystals
journal, June 2013

Highly Emissive and Color-Tunable CuInS2-Based Colloidal Semiconductor Nanocrystals: Off-Stoichiometry Effects and Improved Electroluminescence Performance
journal, March 2012

Employing Heavy Metal-Free Colloidal Quantum Dots in Solution-Processed White Light-Emitting Diodes
journal, February 2011