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Title: Population Pulsation Resonances of Excitons in Monolayer MoSe 2 with Sub-1 μeV Linewidths

Abstract

Monolayer transition metal dichalcogenides, a new class of atomically thin semiconductors, possess optically coupled 2D valley excitons. The nature of exciton relaxation in these systems is currently poorly understood. In this paper, we investigate exciton relaxation in monolayer MoSe 2 using polarization-resolved coherent nonlinear optical spectroscopy with high spectral resolution. We report strikingly narrow population pulsation resonances with two different characteristic linewidths of 1 and <0.2 μeV at low temperature. These linewidths are more than 3 orders of magnitude narrower than the photoluminescence and absorption linewidth, and indicate that a component of the exciton relaxation dynamics occurs on time scales longer than 1 ns. Finally, the ultranarrow resonance (<0.2 μeV) emerges with increasing excitation intensity, and implies the existence of a long-lived state whose lifetime exceeds 6 ns.

Authors:
 [1];  [1];  [2];  [3];  [1];  [1];  [1];  [4];  [5];  [2];  [6];  [7]
  1. Univ. of Washington, Seattle, WA (United States). Dept. of Physics
  2. Univ. of Hong Kong (China). Dept. of Physics and Center of Theoretical and Computational Physics
  3. Univ. of Washington, Seattle, WA (United States). Dept. of Materials Science and Engineering
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Physics and Astronomy
  6. Univ. of Washington, Seattle, WA (United States). Dept. of Physics; Univ. of Washington, Seattle, WA (United States). Dept. of Electrical Engineering
  7. Univ. of Washington, Seattle, WA (United States). Dept. of Physics; Univ. of Washington, Seattle, WA (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); Research Grants Council (RGC) of Hong Kong (China)
OSTI Identifier:
1265565
Alternate Identifier(s):
OSTI ID: 1179313
Grant/Contract Number:
AC05-00OR22725; SC0012509; SC0008145
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 114; Journal Issue: 13; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Schaibley, John R., Karin, Todd, Yu, Hongyi, Ross, Jason S., Rivera, Pasqual, Jones, Aaron M., Scott, Marie E., Yan, Jiaqiang, Mandrus, D. G., Yao, Wang, Fu, Kai-Mei, and Xu, Xiaodong. Population Pulsation Resonances of Excitons in Monolayer MoSe2 with Sub-1 μeV Linewidths. United States: N. p., 2015. Web. doi:10.1103/PhysRevLett.114.137402.
Schaibley, John R., Karin, Todd, Yu, Hongyi, Ross, Jason S., Rivera, Pasqual, Jones, Aaron M., Scott, Marie E., Yan, Jiaqiang, Mandrus, D. G., Yao, Wang, Fu, Kai-Mei, & Xu, Xiaodong. Population Pulsation Resonances of Excitons in Monolayer MoSe2 with Sub-1 μeV Linewidths. United States. doi:10.1103/PhysRevLett.114.137402.
Schaibley, John R., Karin, Todd, Yu, Hongyi, Ross, Jason S., Rivera, Pasqual, Jones, Aaron M., Scott, Marie E., Yan, Jiaqiang, Mandrus, D. G., Yao, Wang, Fu, Kai-Mei, and Xu, Xiaodong. Wed . "Population Pulsation Resonances of Excitons in Monolayer MoSe2 with Sub-1 μeV Linewidths". United States. doi:10.1103/PhysRevLett.114.137402. https://www.osti.gov/servlets/purl/1265565.
@article{osti_1265565,
title = {Population Pulsation Resonances of Excitons in Monolayer MoSe2 with Sub-1 μeV Linewidths},
author = {Schaibley, John R. and Karin, Todd and Yu, Hongyi and Ross, Jason S. and Rivera, Pasqual and Jones, Aaron M. and Scott, Marie E. and Yan, Jiaqiang and Mandrus, D. G. and Yao, Wang and Fu, Kai-Mei and Xu, Xiaodong},
abstractNote = {Monolayer transition metal dichalcogenides, a new class of atomically thin semiconductors, possess optically coupled 2D valley excitons. The nature of exciton relaxation in these systems is currently poorly understood. In this paper, we investigate exciton relaxation in monolayer MoSe2 using polarization-resolved coherent nonlinear optical spectroscopy with high spectral resolution. We report strikingly narrow population pulsation resonances with two different characteristic linewidths of 1 and <0.2 μeV at low temperature. These linewidths are more than 3 orders of magnitude narrower than the photoluminescence and absorption linewidth, and indicate that a component of the exciton relaxation dynamics occurs on time scales longer than 1 ns. Finally, the ultranarrow resonance (<0.2 μeV) emerges with increasing excitation intensity, and implies the existence of a long-lived state whose lifetime exceeds 6 ns.},
doi = {10.1103/PhysRevLett.114.137402},
journal = {Physical Review Letters},
number = 13,
volume = 114,
place = {United States},
year = {Wed Apr 01 00:00:00 EDT 2015},
month = {Wed Apr 01 00:00:00 EDT 2015}
}

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