Acceleration of Biexciton Radiative Recombination at Low Temperature in CdSe Nanoplatelets
Abstract
Colloidal semiconductor nanocrystals offer bandgap tunability, high photoluminescence quantum yield, and colloidal processing of benefit to optoelectronics, however rapid nonradiative Auger recombination (AR) deleteriously affects device efficiencies at elevated excitation intensities. AR is understood to transition from temperature-dependent behavior in bulk semiconductors to temperature-independent behavior in zero-dimensional quantum dots (QDs) as a result of discretized band structure that facilitates satisfaction of linear momentum conservation. For nanoplatelets (NPLs), two-dimensional morphology renders prediction of photophysical behaviors challenging. Here, in this study, we investigate and compare the temperature dependence of excited-stated lifetime and fluence-dependent emission of CdSe NPLs and QDs. For NPLs, upon temperature reduction, biexciton lifetime surprisingly decreases (even becoming shorter lived than trion emission) and emission intensity increases nearly linearly with fluence rather than saturating, consistent with dominance of radiative recombination rather than AR. CdSe NPLs thus differ fundamentally from core-only QDs and foster increased utility of photogenerated excitons and multiexcitons at low temperatures.
- Authors:
-
- Northwestern Univ., Evanston, IL (United States)
- Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
- Northwestern Univ., Evanston, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF); 3M
- OSTI Identifier:
- 1986031
- Grant/Contract Number:
- AC02-06CH11357; 1808590; DGE-1842165
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nano Letters
- Additional Journal Information:
- Journal Volume: 22; Journal Issue: 17; Journal ID: ISSN 1530-6984
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; nanoplatelets; biexcitons; Auger recombination; quantum yield; temperature-dependent emission
Citation Formats
Brumberg, Alexandra, Watkins, Nicolas E., Diroll, Benjamin T., and Schaller, Richard D. Acceleration of Biexciton Radiative Recombination at Low Temperature in CdSe Nanoplatelets. United States: N. p., 2022.
Web. doi:10.1021/acs.nanolett.2c01791.
Brumberg, Alexandra, Watkins, Nicolas E., Diroll, Benjamin T., & Schaller, Richard D. Acceleration of Biexciton Radiative Recombination at Low Temperature in CdSe Nanoplatelets. United States. https://doi.org/10.1021/acs.nanolett.2c01791
Brumberg, Alexandra, Watkins, Nicolas E., Diroll, Benjamin T., and Schaller, Richard D. Fri .
"Acceleration of Biexciton Radiative Recombination at Low Temperature in CdSe Nanoplatelets". United States. https://doi.org/10.1021/acs.nanolett.2c01791. https://www.osti.gov/servlets/purl/1986031.
@article{osti_1986031,
title = {Acceleration of Biexciton Radiative Recombination at Low Temperature in CdSe Nanoplatelets},
author = {Brumberg, Alexandra and Watkins, Nicolas E. and Diroll, Benjamin T. and Schaller, Richard D.},
abstractNote = {Colloidal semiconductor nanocrystals offer bandgap tunability, high photoluminescence quantum yield, and colloidal processing of benefit to optoelectronics, however rapid nonradiative Auger recombination (AR) deleteriously affects device efficiencies at elevated excitation intensities. AR is understood to transition from temperature-dependent behavior in bulk semiconductors to temperature-independent behavior in zero-dimensional quantum dots (QDs) as a result of discretized band structure that facilitates satisfaction of linear momentum conservation. For nanoplatelets (NPLs), two-dimensional morphology renders prediction of photophysical behaviors challenging. Here, in this study, we investigate and compare the temperature dependence of excited-stated lifetime and fluence-dependent emission of CdSe NPLs and QDs. For NPLs, upon temperature reduction, biexciton lifetime surprisingly decreases (even becoming shorter lived than trion emission) and emission intensity increases nearly linearly with fluence rather than saturating, consistent with dominance of radiative recombination rather than AR. CdSe NPLs thus differ fundamentally from core-only QDs and foster increased utility of photogenerated excitons and multiexcitons at low temperatures.},
doi = {10.1021/acs.nanolett.2c01791},
journal = {Nano Letters},
number = 17,
volume = 22,
place = {United States},
year = {Fri Aug 26 00:00:00 EDT 2022},
month = {Fri Aug 26 00:00:00 EDT 2022}
}
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