Ultrastrong Coupling Leads to Slowed Cooling of Hot Excitons in Few-Layer Transition-Metal Dichalcogenides
Abstract
The excited-state dynamics of few-layer molybdenum disulfide (FL-MoS2) are studied in conditions of strong light-matter coupling to plasmon polaritons. Hot carrier extraction in these systems has been proposed due to the observation of slow cooling of the high-energy C exciton relative to the bandgap A exciton. Here, we show that in conditions of ultrastrong coupling to plasmon polaritons, the lifetimes of the two slowest C exciton decay processes are extended by factors of 1.5 and 5.8 in FL-MoS2. We hypothesize that strong coupling delocalization suppresses multiple decay mechanisms throughout the visible spectrum in MoS2 such as defect scattering, intervalley scattering of band-nested excitations to the K-valley band edges, and exciton-exciton annihilation. We also find that decay from the upper to the lower hybrid mode is not ultrafast as seen in organic systems but in fact introduces an additional delay of ~20 ps. Our observations show that strong coupling can be used to extend the lifetimes of hot excitons in FL-MoS2 and potentially in other two-dimensional transition-metal dichalcogenides, with potential for above-bandgap photophysics and photochemistry applications such as hot carrier extraction, which could lead to more efficient solar energy conversion.
- Authors:
-
[1];
[1];
[1];
[1]
- National Renewable Energy Laboratory, 15013 Denver W Parkway, Golden, Colorado 80401, United States
- Publication Date:
- Research Org.:
- National Renewable Energy Laboratory (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
- OSTI Identifier:
- 1868375
- Alternate Identifier(s):
- OSTI ID: 1871529
- Report Number(s):
- NREL/JA-5900-82245
Journal ID: ISSN 1932-7447
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Published Article
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Name: Journal of Physical Chemistry. C Journal Volume: 126 Journal Issue: 20; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; carrier dynamics; exciton-polariton; MoS2; solar-photochemistry; strong coupling; surface plasmon polariton; transition-metal dichalcogenide; two-dimensional materials; ultrafast spectroscopy
Citation Formats
Rose, Aaron H., Aubry, Taylor J., Zhang, Hanyu, Vigil-Fowler, Derek, and van de Lagemaat, Jao. Ultrastrong Coupling Leads to Slowed Cooling of Hot Excitons in Few-Layer Transition-Metal Dichalcogenides. United States: N. p., 2022.
Web. doi:10.1021/acs.jpcc.2c01262.
Rose, Aaron H., Aubry, Taylor J., Zhang, Hanyu, Vigil-Fowler, Derek, & van de Lagemaat, Jao. Ultrastrong Coupling Leads to Slowed Cooling of Hot Excitons in Few-Layer Transition-Metal Dichalcogenides. United States. https://doi.org/10.1021/acs.jpcc.2c01262
Rose, Aaron H., Aubry, Taylor J., Zhang, Hanyu, Vigil-Fowler, Derek, and van de Lagemaat, Jao. Tue .
"Ultrastrong Coupling Leads to Slowed Cooling of Hot Excitons in Few-Layer Transition-Metal Dichalcogenides". United States. https://doi.org/10.1021/acs.jpcc.2c01262.
@article{osti_1868375,
title = {Ultrastrong Coupling Leads to Slowed Cooling of Hot Excitons in Few-Layer Transition-Metal Dichalcogenides},
author = {Rose, Aaron H. and Aubry, Taylor J. and Zhang, Hanyu and Vigil-Fowler, Derek and van de Lagemaat, Jao},
abstractNote = {The excited-state dynamics of few-layer molybdenum disulfide (FL-MoS2) are studied in conditions of strong light-matter coupling to plasmon polaritons. Hot carrier extraction in these systems has been proposed due to the observation of slow cooling of the high-energy C exciton relative to the bandgap A exciton. Here, we show that in conditions of ultrastrong coupling to plasmon polaritons, the lifetimes of the two slowest C exciton decay processes are extended by factors of 1.5 and 5.8 in FL-MoS2. We hypothesize that strong coupling delocalization suppresses multiple decay mechanisms throughout the visible spectrum in MoS2 such as defect scattering, intervalley scattering of band-nested excitations to the K-valley band edges, and exciton-exciton annihilation. We also find that decay from the upper to the lower hybrid mode is not ultrafast as seen in organic systems but in fact introduces an additional delay of ~20 ps. Our observations show that strong coupling can be used to extend the lifetimes of hot excitons in FL-MoS2 and potentially in other two-dimensional transition-metal dichalcogenides, with potential for above-bandgap photophysics and photochemistry applications such as hot carrier extraction, which could lead to more efficient solar energy conversion.},
doi = {10.1021/acs.jpcc.2c01262},
journal = {Journal of Physical Chemistry. C},
number = 20,
volume = 126,
place = {United States},
year = {Tue May 17 00:00:00 EDT 2022},
month = {Tue May 17 00:00:00 EDT 2022}
}
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