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Title: Bandgap Inhomogeneity of a PbSe Quantum Dot Ensemble from Two-Dimensional Spectroscopy and Comparison to Size Inhomogeneity from Electron Microscopy

Abstract

Femtosecond two-dimensional Fourier transform spectroscopy is used to determine the static bandgap inhomogeneity of a colloidal PbSe quantum dot ensemble. It is shown that the absorption bandgap inhomogeneity is robustly determined by the slope of the nodal line separating positive and negative peaks in the 2D spectrum around the bandgap transition; this nodal line slope is independent of excited state parameters not known from the absorption and emission spectra. The absorption bandgap inhomogeneity is compared to a size and shape distribution determined by electron microscopy. The electron microscopy images are analyzed using new 2D histograms that correlate major and minor image projections to reveal elongated nanocrystals, a conclusion supported by grazing incidence small angle X-ray scattering and high resolution transmission electron microscopy. Lastly, the absorption bandgap inhomogeneity quantitatively agrees with the bandgap variations calculated from the size and shape distribution, placing upper bounds on any surface contributions.

Authors:
 [1]; ORCiD logo [1];  [1];  [1]; ; ; ORCiD logo; ORCiD logo [1]
  1. Department of Chemistry and Biochemistry and Renewable and Sustainable Energy Institute, University of Colorado, Boulder, Colorado 80309, United States
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Univ. of Colorado, Boulder, CO (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1337889
Alternate Identifier(s):
OSTI ID: 1338409; OSTI ID: 1344807; OSTI ID: 1346934
Report Number(s):
SAND-2016-12917J
Journal ID: ISSN 1530-6984
Grant/Contract Number:  
FG02-07ER15912; AC02- 06CH11357; AC04-94AL85000; AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Nano Letters
Additional Journal Information:
Journal Name: Nano Letters Journal Volume: 17 Journal Issue: 2; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
47 OTHER INSTRUMENTATION; Quantum dots; inhomogeneity; size dispersion; shape dispersion; 2D spectroscopy; line width; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; quantum dots; linewidth

Citation Formats

Park, Samuel D., Baranov, Dmitry, Ryu, Jisu, Cho, Byungmoon, Halder, Avik, Seifert, Sönke, Vajda, Stefan, and Jonas, David M. Bandgap Inhomogeneity of a PbSe Quantum Dot Ensemble from Two-Dimensional Spectroscopy and Comparison to Size Inhomogeneity from Electron Microscopy. United States: N. p., 2017. Web. doi:10.1021/acs.nanolett.6b03874.
Park, Samuel D., Baranov, Dmitry, Ryu, Jisu, Cho, Byungmoon, Halder, Avik, Seifert, Sönke, Vajda, Stefan, & Jonas, David M. Bandgap Inhomogeneity of a PbSe Quantum Dot Ensemble from Two-Dimensional Spectroscopy and Comparison to Size Inhomogeneity from Electron Microscopy. United States. https://doi.org/10.1021/acs.nanolett.6b03874
Park, Samuel D., Baranov, Dmitry, Ryu, Jisu, Cho, Byungmoon, Halder, Avik, Seifert, Sönke, Vajda, Stefan, and Jonas, David M. Tue . "Bandgap Inhomogeneity of a PbSe Quantum Dot Ensemble from Two-Dimensional Spectroscopy and Comparison to Size Inhomogeneity from Electron Microscopy". United States. https://doi.org/10.1021/acs.nanolett.6b03874.
@article{osti_1337889,
title = {Bandgap Inhomogeneity of a PbSe Quantum Dot Ensemble from Two-Dimensional Spectroscopy and Comparison to Size Inhomogeneity from Electron Microscopy},
author = {Park, Samuel D. and Baranov, Dmitry and Ryu, Jisu and Cho, Byungmoon and Halder, Avik and Seifert, Sönke and Vajda, Stefan and Jonas, David M.},
abstractNote = {Femtosecond two-dimensional Fourier transform spectroscopy is used to determine the static bandgap inhomogeneity of a colloidal PbSe quantum dot ensemble. It is shown that the absorption bandgap inhomogeneity is robustly determined by the slope of the nodal line separating positive and negative peaks in the 2D spectrum around the bandgap transition; this nodal line slope is independent of excited state parameters not known from the absorption and emission spectra. The absorption bandgap inhomogeneity is compared to a size and shape distribution determined by electron microscopy. The electron microscopy images are analyzed using new 2D histograms that correlate major and minor image projections to reveal elongated nanocrystals, a conclusion supported by grazing incidence small angle X-ray scattering and high resolution transmission electron microscopy. Lastly, the absorption bandgap inhomogeneity quantitatively agrees with the bandgap variations calculated from the size and shape distribution, placing upper bounds on any surface contributions.},
doi = {10.1021/acs.nanolett.6b03874},
journal = {Nano Letters},
number = 2,
volume = 17,
place = {United States},
year = {Tue Jan 03 00:00:00 EST 2017},
month = {Tue Jan 03 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acs.nanolett.6b03874

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Works referencing / citing this record:

Measuring Ultrafast Spectral Diffusion and Correlation Dynamics by Two‐Dimensional Electronic Spectroscopy
journal, October 2019

  • Do, Thanh Nhut; Khyasudeen, M. Faisal; Nowakowski, Paweł J.
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Elucidating ultrafast electron dynamics at surfaces using extreme ultraviolet (XUV) reflection–absorption spectroscopy
journal, January 2018

  • Biswas, Somnath; Husek, Jakub; Baker, L. Robert
  • Chemical Communications, Vol. 54, Issue 34
  • DOI: 10.1039/c8cc01745j