Coherent and Incoherent Coupling Dynamics between Neutral and Charged Excitons in Monolayer MoSe2
Abstract
The optical properties of semiconducting transition metal dichalcogenides are dominated by both neutral excitons (electron–hole pairs) and charged excitons (trions) that are stable even at room temperature. While trions directly influence charge transport properties in optoelectronic devices, excitons may be relevant through exciton–trion coupling and conversion phenomena. Here in this work, we reveal the coherent and incoherent nature of exciton–trion coupling and the relevant time scales in monolayer MoSe2 using optical two-dimensional coherent spectroscopy. Coherent interaction between excitons and trions is definitively identified as quantum beating of cross peaks in the spectra that persists for a few hundred femtoseconds. For longer times up to 10 ps, surprisingly, the relative intensity of the cross peaks increases, which is attributed to incoherent energy transfer likely due to phonon-assisted up-conversion and down-conversion processes that are efficient even at cryogenic temperature.
- Authors:
-
- Univ. of Texas, Austin, TX (United States). Dept. of Physics and Center for Complex Quantum Systems
- Univ. of Regensburg (Germany). Dept. of Physics
- National Inst. of Standards and Technology (NIST), Boulder, CO (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Spins and Heat in Nanoscale Electronic Systems (SHINES)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1388923
- Grant/Contract Number:
- SC0012670
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nano Letters
- Additional Journal Information:
- Journal Volume: 16; Journal Issue: 8; Related Information: SHINES partners with University of California, Riverside (lead); Arizona State University; Colorado State University; Johns Hopkins University; University of California Irvine; University of California Los Angeles; University of Texas at Austin; Journal ID: ISSN 1530-6984
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; phonons; thermal conductivity; thermoelectric; spin dynamics; spintronics
Citation Formats
Hao, Kai, Xu, Lixiang, Nagler, Philipp, Singh, Akshay, Tran, Kha, Dass, Chandriker Kavir, Schüller, Christian, Korn, Tobias, Li, Xiaoqin, and Moody, Galan. Coherent and Incoherent Coupling Dynamics between Neutral and Charged Excitons in Monolayer MoSe2. United States: N. p., 2016.
Web. doi:10.1021/acs.nanolett.6b02041.
Hao, Kai, Xu, Lixiang, Nagler, Philipp, Singh, Akshay, Tran, Kha, Dass, Chandriker Kavir, Schüller, Christian, Korn, Tobias, Li, Xiaoqin, & Moody, Galan. Coherent and Incoherent Coupling Dynamics between Neutral and Charged Excitons in Monolayer MoSe2. United States. https://doi.org/10.1021/acs.nanolett.6b02041
Hao, Kai, Xu, Lixiang, Nagler, Philipp, Singh, Akshay, Tran, Kha, Dass, Chandriker Kavir, Schüller, Christian, Korn, Tobias, Li, Xiaoqin, and Moody, Galan. Fri .
"Coherent and Incoherent Coupling Dynamics between Neutral and Charged Excitons in Monolayer MoSe2". United States. https://doi.org/10.1021/acs.nanolett.6b02041. https://www.osti.gov/servlets/purl/1388923.
@article{osti_1388923,
title = {Coherent and Incoherent Coupling Dynamics between Neutral and Charged Excitons in Monolayer MoSe2},
author = {Hao, Kai and Xu, Lixiang and Nagler, Philipp and Singh, Akshay and Tran, Kha and Dass, Chandriker Kavir and Schüller, Christian and Korn, Tobias and Li, Xiaoqin and Moody, Galan},
abstractNote = {The optical properties of semiconducting transition metal dichalcogenides are dominated by both neutral excitons (electron–hole pairs) and charged excitons (trions) that are stable even at room temperature. While trions directly influence charge transport properties in optoelectronic devices, excitons may be relevant through exciton–trion coupling and conversion phenomena. Here in this work, we reveal the coherent and incoherent nature of exciton–trion coupling and the relevant time scales in monolayer MoSe2 using optical two-dimensional coherent spectroscopy. Coherent interaction between excitons and trions is definitively identified as quantum beating of cross peaks in the spectra that persists for a few hundred femtoseconds. For longer times up to 10 ps, surprisingly, the relative intensity of the cross peaks increases, which is attributed to incoherent energy transfer likely due to phonon-assisted up-conversion and down-conversion processes that are efficient even at cryogenic temperature.},
doi = {10.1021/acs.nanolett.6b02041},
journal = {Nano Letters},
number = 8,
volume = 16,
place = {United States},
year = {Fri Jul 22 00:00:00 EDT 2016},
month = {Fri Jul 22 00:00:00 EDT 2016}
}
Web of Science
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