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Connecting the Dots: The Kinetics and Thermodynamics of Hot, Cold, and Surface-Trapped Excitons in Semiconductor Nanocrystals

The excitonics of semiconductor nanocrystals (NC) depend upon temperature in a complex manner due to the interplay between the kinetics of hot exciton relaxation/trapping and the thermodynamics leading to cold exciton recombination. We apply a semiclassical electron transfer model of surface trappin... Full description

Journal Title: The Journal of Physical Chemistry C 04/10/2014, Vol.118(14), pp.7730-7739
Main Author: Mooney, Jonathan
Other Authors: Krause, Michael M. , Kambhampati, Patanjali
Format: Electronic Article Electronic Article
Language: English
Subjects:
Quelle: American Chemical Society (via CrossRef)
ID: ISSN: 1932-7447 ; E-ISSN: 1932-7455 ; DOI: http://dx.doi.org/10.1021/jp502102a
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recordid: crossref10.1021/jp502102a
title: Connecting the Dots: The Kinetics and Thermodynamics of Hot, Cold, and Surface-Trapped Excitons in Semiconductor Nanocrystals
format: Article
creator:
  • Mooney, Jonathan
  • Krause, Michael M.
  • Kambhampati, Patanjali
subjects:
  • Chemistry
ispartof: The Journal of Physical Chemistry C, 04/10/2014, Vol.118(14), pp.7730-7739
description: The excitonics of semiconductor nanocrystals (NC) depend upon temperature in a complex manner due to the interplay between the kinetics of hot exciton relaxation/trapping and the thermodynamics leading to cold exciton recombination. We apply a semiclassical electron transfer model of surface trapping to temperature-dependent absorption and emission data to elucidate a microscopic picture of the factors which govern the fate of hot and cold excitons. The linear absorption spectra reveal a unique temperature-dependence to the energies of higher excitonic states, while oscillator strength is shown to be temperature invariant. We identify the phonon based origin to the anomalous low temperature peak energy trend in photoluminescence (PL) spectra. PL intensities, PL lifetimes, and absorption spectra are used to demonstrate that variation of quantum yield with temperatures arises from the thermally controlled fraction of NC which emit, rather than from an activated nonradiative pathway...
language: eng
source: American Chemical Society (via CrossRef)
identifier: ISSN: 1932-7447 ; E-ISSN: 1932-7455 ; DOI: http://dx.doi.org/10.1021/jp502102a
fulltext: fulltext
issn:
  • 19327447
  • 1932-7447
  • 19327455
  • 1932-7455
url: Link


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descriptionThe excitonics of semiconductor nanocrystals (NC) depend upon temperature in a complex manner due to the interplay between the kinetics of hot exciton relaxation/trapping and the thermodynamics leading to cold exciton recombination. We apply a semiclassical electron transfer model of surface trapping to temperature-dependent absorption and emission data to elucidate a microscopic picture of the factors which govern the fate of hot and cold excitons. The linear absorption spectra reveal a unique temperature-dependence to the energies of higher excitonic states, while oscillator strength is shown to be temperature invariant. We identify the phonon based origin to the anomalous low temperature peak energy trend in photoluminescence (PL) spectra. PL intensities, PL lifetimes, and absorption spectra are used to demonstrate that variation of quantum yield with temperatures arises from the thermally controlled fraction of NC which emit, rather than from an activated nonradiative pathway...
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