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:
-
- 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:
- Journal Article: 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. 2017.
"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},
url = {https://www.osti.gov/biblio/1337889},
journal = {Nano Letters},
issn = {1530-6984},
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}
}
Web of Science
Works referencing / citing this record:
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- Biswas, Somnath; Husek, Jakub; Baker, L. Robert
- Chemical Communications, Vol. 54, Issue 34