Influence of Morphology on Blinking Mechanisms and Excitonic Fine Structure of Single Colloidal Nanoplatelets

Hu, Zhongjian; Singh, Ajay; Goupalov, Serguei; Hollingsworth, Jennifer; Htoon, Han

doi:10.1039/C8NR06234J

Title: Influence of Morphology on Blinking Mechanisms and Excitonic Fine Structure of Single Colloidal Nanoplatelets

Abstract

Colloidal semiconductor nanoplatelets with electronic structure as quantum wells have recently emerged as exciting materials for optoelectronic applications. Here we investigate how morpholo-gy affects important photoluminescence properties of single CdSe and core/shell CdSe/CdZnS na-noplatelets. By analyzing photoluminescence intensity-lifetime correlation and second-order pho-ton correlation results, we demonstrate that, irrespective of morphology, Auger recombination plays only a minor role in dictating the blinking behavior of the nanoplatelets. We find that a rough shell induces additional nonradiative channels presumably related to defects or traps of an imper-fect shell. However, polarization-resolved spectroscopy analysis reveals exciton fine-structure splitting on the order of several tens of meV in rough-shell nanoplatelets at room temperature, which is attributed to exciton localization and substantiated with theoretical calculations taking into account the nanoplatelet shape and electron-hole exchange interaction.

Authors:

^[1]; Singh, Ajay ^[1]; Goupalov, Serguei ^[2];

^[1];

^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Jackson State Univ., Jackson, MS (United States); Ioffe Institute, St. Petersburg (Russia)

Publication Date:: Thu Nov 08 00:00:00 EST 2018

Research Org.:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE Laboratory Directed Research and Development (LDRD) Program

OSTI Identifier:: 1482958

Alternate Identifier(s):: OSTI ID: 1483902

Report Number(s):: LA-UR-18-28802
Journal ID: ISSN 2040-3364

Grant/Contract Number:: 89233218CNA000001

Resource Type:: Accepted Manuscript

Journal Name:: Nanoscale

Additional Journal Information:: Journal Volume: 10; Journal Issue: 48; Journal ID: ISSN 2040-3364

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

Subject:: 77 NANOSCIENCE AND NANOTECHNOLOGY; Material Science

Citation Formats


                    Hu, Zhongjian, Singh, Ajay, Goupalov, Serguei, Hollingsworth, Jennifer, and Htoon, Han. Influence of Morphology on Blinking Mechanisms and Excitonic Fine Structure of Single Colloidal Nanoplatelets.  United States: N. p., 2018. 
Web.  doi:10.1039/C8NR06234J.

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                    Hu, Zhongjian, Singh, Ajay, Goupalov, Serguei, Hollingsworth, Jennifer, & Htoon, Han. Influence of Morphology on Blinking Mechanisms and Excitonic Fine Structure of Single Colloidal Nanoplatelets.  United States.  https://doi.org/10.1039/C8NR06234J

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                    Hu, Zhongjian, Singh, Ajay, Goupalov, Serguei, Hollingsworth, Jennifer, and Htoon, Han. Thu .  
"Influence of Morphology on Blinking Mechanisms and Excitonic Fine Structure of Single Colloidal Nanoplatelets".  United States.  https://doi.org/10.1039/C8NR06234J.  https://www.osti.gov/servlets/purl/1482958.

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@article{osti_1482958,

  title        = {Influence of Morphology on Blinking Mechanisms and Excitonic Fine Structure of Single Colloidal Nanoplatelets},

  author       = {Hu, Zhongjian and Singh, Ajay and Goupalov, Serguei and Hollingsworth, Jennifer and Htoon, Han},

  abstractNote = {Colloidal semiconductor nanoplatelets with electronic structure as quantum wells have recently emerged as exciting materials for optoelectronic applications. Here we investigate how morpholo-gy affects important photoluminescence properties of single CdSe and core/shell CdSe/CdZnS na-noplatelets. By analyzing photoluminescence intensity-lifetime correlation and second-order pho-ton correlation results, we demonstrate that, irrespective of morphology, Auger recombination plays only a minor role in dictating the blinking behavior of the nanoplatelets. We find that a rough shell induces additional nonradiative channels presumably related to defects or traps of an imper-fect shell. However, polarization-resolved spectroscopy analysis reveals exciton fine-structure splitting on the order of several tens of meV in rough-shell nanoplatelets at room temperature, which is attributed to exciton localization and substantiated with theoretical calculations taking into account the nanoplatelet shape and electron-hole exchange interaction.},

  doi          = {10.1039/C8NR06234J},

  journal      = {Nanoscale},

  number       = 48,

  volume       = 10,

  place        = {United States},

  year         = {Thu Nov 08 00:00:00 EST 2018},

  month        = {Thu Nov 08 00:00:00 EST 2018}

}

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Title: Influence of Morphology on Blinking Mechanisms and Excitonic Fine Structure of Single Colloidal Nanoplatelets

Abstract

Citation Formats

Origin and control of blinking in quantum dots journal, August 2016

Continuous-wave biexciton lasing at room temperature using solution-processed quantum wells journal, October 2014

Nonmonotonic Dependence of Auger Recombination Rate on Shell Thickness for CdSe/CdS Core/Shell Nanoplatelets journal, October 2017

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Continuous Transition from 3D to 1D Confinement Observed during the Formation of CdSe Nanoplatelets journal, March 2011

Core/Shell Colloidal Semiconductor Nanoplatelets journal, November 2012

Quasi-2D Colloidal Semiconductor Nanoplatelets for Narrow Electroluminescence journal, July 2013

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Electron and Hole g Factors and Exchange Interaction from Studies of the Exciton Fine Structure in In 0.60 Ga 0.40 As Quantum Dots journal, February 1999

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Spectroscopic and Device Aspects of Nanocrystal Quantum Dots journal, September 2016

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Defect-Induced Photoluminescence Blinking of Single Epitaxial InGaAs Quantum Dots journal, March 2015

Additional waves and Fabry-Perot interference of photoexcitons (polaritons) in thin II–VI crystals journal, November 1975

Electronic Structure and Exciton–Phonon Interaction in Two-Dimensional Colloidal CdSe Nanosheets journal, May 2012

Origin and control of blinking in quantum dots
journal, August 2016

Continuous-wave biexciton lasing at room temperature using solution-processed quantum wells
journal, October 2014

Nonmonotonic Dependence of Auger Recombination Rate on Shell Thickness for CdSe/CdS Core/Shell Nanoplatelets
journal, October 2017

Red, Yellow, Green, and Blue Amplified Spontaneous Emission and Lasing Using Colloidal CdSe Nanoplatelets
journal, September 2015

Area- and Thickness-Dependent Biexciton Auger Recombination in Colloidal CdSe Nanoplatelets: Breaking the “Universal Volume Scaling Law”
journal, April 2017

Tight-binding calculations of image-charge effects in colloidal nanoscale platelets of CdSe
journal, January 2014

Continuous Transition from 3D to 1D Confinement Observed during the Formation of CdSe Nanoplatelets
journal, March 2011

Core/Shell Colloidal Semiconductor Nanoplatelets
journal, November 2012

Quasi-2D Colloidal Semiconductor Nanoplatelets for Narrow Electroluminescence
journal, July 2013

Engineering of Semiconductor Nanocrystals for Light Emitting Applications
journal, August 2016

Size-Dependent Biexciton Quantum Yields and Carrier Dynamics of Quasi-Two-Dimensional Core/Shell Nanoplatelets
journal, September 2017

Electron and Hole $g$ Factors and Exchange Interaction from Studies of the Exciton Fine Structure in ${In}_{0.60} {Ga}_{0.40} As$ Quantum Dots
journal, February 1999

Temporary Charge Carrier Separation Dominates the Photoluminescence Decay Dynamics of Colloidal CdSe Nanoplatelets
journal, February 2016

Spectroscopic and Device Aspects of Nanocrystal Quantum Dots
journal, September 2016

Spectroscopy of Colloidal Semiconductor Core/Shell Nanoplatelets with High Quantum Yield
journal, June 2013

Two-Dimensional Colloidal Metal Chalcogenides Semiconductors: Synthesis, Spectroscopy, and Applications
journal, December 2014

Ultralow-threshold multiphoton-pumped lasing from colloidal nanoplatelets in solution
journal, September 2015

Directed emission of CdSe nanoplatelets originating from strongly anisotropic 2D electronic structure
journal, September 2017

Room temperature measurements of the 3D orientation of single CdSe quantum dots using polarization microscopy
journal, January 2003

Lateral Size-Dependent Spontaneous and Stimulated Emission Properties in Colloidal CdSe Nanoplatelets
journal, May 2015

Auger Recombination of Biexcitons and Negative and Positive Trions in Individual Quantum Dots
journal, June 2014

Nature and Decay Pathways of Photoexcited States in CdSe and CdSe/CdS Nanoplatelets
journal, November 2014

$p$ -State Luminescence in CdSe Nanoplatelets: Role of Lateral Confinement and a Longitudinal Optical Phonon Bottleneck
journal, March 2016

Biexciton Quantum Yield of Single Semiconductor Nanocrystals from Photon Statistics
journal, March 2011

Trion Decay in Colloidal Quantum Dots
journal, March 2009

Efficient Exciton Concentrators Built from Colloidal Core/Crown CdSe/CdS Semiconductor Nanoplatelets
journal, December 2013

Colloidal Quantum Dot Solar Cells
journal, June 2015

Bright-exciton fine structure and anisotropic exchange in $CdSe$ nanocrystal quantum dots
journal, June 2006

Amplified Spontaneous Emission and Lasing in Colloidal Nanoplatelets
journal, June 2014

Colloidal Atomic Layer Deposition (c-ALD) using Self-Limiting Reactions at Nanocrystal Surface Coupled to Phase Transfer between Polar and Nonpolar Media
journal, November 2012

Bimolecular Auger Recombination of Electron–Hole Pairs in Two-Dimensional CdSe and CdSe/CdZnS Core/Shell Nanoplatelets
journal, October 2013

Competition between Auger Recombination and Hot-Carrier Trapping in PL Intensity Fluctuations of Type II Nanocrystals
journal, April 2014

Two-dimensional electronic spectroscopy of CdSe nanoparticles at very low pulse power
journal, January 2013

Two-Dimensional Colloidal Nanocrystals
journal, July 2016

Fine structure of localized exciton levels in quantum wells
journal, February 1998

Recombination Dynamics of Band Edge Excitons in Quasi-Two-Dimensional CdSe Nanoplatelets
journal, February 2014

Colloidal nanoplatelets with two-dimensional electronic structure
journal, October 2011

Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots
journal, November 2011

Anomalous Circular Polarization of Photoluminescence Spectra of Individual CdSe Nanocrystals in an Applied Magnetic Field
journal, January 2009

Biexciton Quantum Yield Heterogeneities in Single CdSe (CdS) Core (Shell) Nanocrystals and Its Correlation to Exciton Blinking
journal, January 2012

Quasi 2D Colloidal CdSe Platelets with Thicknesses Controlled at the Atomic Level
journal, December 2008

Ultrathin One- and Two-Dimensional Colloidal Semiconductor Nanocrystals: Pushing Quantum Confinement to the Limit
journal, August 2017

Probing the Fluorescence Dipoles of Single Cubic CdSe/CdS Nanoplatelets with Vertical or Horizontal Orientations
journal, March 2018

Fluorescence intermittency in single cadmium selenide nanocrystals
journal, October 1996

Temperature dependent radiative and non-radiative recombination dynamics in CdSe–CdTe and CdTe–CdSe type II hetero nanoplatelets
journal, January 2016

Spectroscopy of Single CdSe Nanoplatelets
journal, July 2012

Two-Color Antibunching from Band-Gap Engineered Colloidal Semiconductor Nanocrystals
journal, May 2012

Linearly polarized ‘fine structure’ of the bright exciton state in individual CdSe nanocrystal quantum dots
journal, January 2008

Anisotropic exchange splitting of excitonic levels in small quantum systems
journal, June 1998

Defect-Induced Photoluminescence Blinking of Single Epitaxial InGaAs Quantum Dots
journal, March 2015

Additional waves and Fabry-Perot interference of photoexcitons (polaritons) in thin II–VI crystals
journal, November 1975

Electronic Structure and Exciton–Phonon Interaction in Two-Dimensional Colloidal CdSe Nanosheets
journal, May 2012