Population Pulsation Resonances of Excitons in Monolayer MoSe2 with Sub-1 μeV Linewidths

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

doi:10.1103/PhysRevLett.114.137402

Title: Population Pulsation Resonances of Excitons in Monolayer MoSe₂ with Sub-1 μeV Linewidths

Journal Article · Wed Apr 01 00:00:00 EDT 2015 · Physical Review Letters

DOI:https://doi.org/10.1103/PhysRevLett.114.137402· OSTI ID:1265565

Schaibley, John R. ^[1]; Karin, Todd ^[1]; Yu, Hongyi ^[2]; Ross, Jason S. ^[3]; Rivera, Pasqual ^[1]; Jones, Aaron M. ^[1]; Scott, Marie E. ^[1]; Yan, Jiaqiang ^[4]; Mandrus, D. G. ^[5]; Yao, Wang ^[2]; Fu, Kai-Mei ^[6]; Xu, Xiaodong ^[7]

Univ. of Washington, Seattle, WA (United States). Dept. of Physics
Univ. of Hong Kong (China). Dept. of Physics and Center of Theoretical and Computational Physics
Univ. of Washington, Seattle, WA (United States). Dept. of Materials Science and Engineering
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
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
Univ. of Washington, Seattle, WA (United States). Dept. of Physics; Univ. of Washington, Seattle, WA (United States). Dept. of Electrical Engineering
Univ. of Washington, Seattle, WA (United States). Dept. of Physics; Univ. of Washington, Seattle, WA (United States). Dept. of Materials Science and Engineering

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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Research Grants Council (RGC) of Hong Kong (China)

Grant/Contract Number:: AC05-00OR22725; SC0012509; SC0008145

OSTI ID:: 1265565

Alternate ID(s):: OSTI ID: 1179313

Journal Information:: Physical Review Letters, Vol. 114, Issue 13; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 22 works

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Valleytronics in 2D materials Schaibley, John R.; Yu, Hongyi; Clark, Genevieve Nature Reviews Materials, Vol. 1, Issue 11 https://doi.org/10.1038/natrevmats.2016.55	journal	August 2016
Directional interlayer spin-valley transfer in two-dimensional heterostructures Schaibley, John R.; Rivera, Pasqual; Yu, Hongyi Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13747	journal	December 2016
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Physics of excitons and their transport in two dimensional transition metal dichalcogenide semiconductors Kaviraj, Bhaskar; Sahoo, Dhirendra RSC Advances, Vol. 9, Issue 44 https://doi.org/10.1039/c9ra03769a	journal	January 2019
Exciton states in monolayer MoSe ₂ : impact on interband transitions Wang, G.; Gerber, I. C.; Bouet, L. 2D Materials, Vol. 2, Issue 4 https://doi.org/10.1088/2053-1583/2/4/045005	journal	November 2015
Many-body effects in nonlinear optical responses of 2D layered semiconductors Aivazian, Grant; Yu, Hongyi; Wu, Sanfeng 2D Materials, Vol. 4, Issue 2 https://doi.org/10.1088/2053-1583/aa56f1	journal	February 2017
Dark excitons and the elusive valley polarization in transition metal dichalcogenides Baranowski, M.; Surrente, A.; Maude, D. K. 2D Materials, Vol. 4, Issue 2 https://doi.org/10.1088/2053-1583/aa58a0	journal	February 2017
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Trion Formation Dynamics in Monolayer Transition Metal Dichalcogenides Singh, Akshay; Moody, Galan; Tran, Kha arXiv https://doi.org/10.48550/arxiv.1507.04463	text	January 2015
Many-body effects in nonlinear optical responses of 2D layered semiconductors Aivazian, Grant; Yu, Hongyi; Wu, Sanfeng arXiv https://doi.org/10.48550/arxiv.1612.02714	text	January 2016
Directional Interlayer Spin-Valley Transfer in Two-Dimensional Heterostructures Schaibley, John R.; Rivera, Pasqual; Yu, Hongyi arXiv https://doi.org/10.48550/arxiv.1612.04863	text	January 2016
Dark excitons and the elusive valley polarization in transition metal dichalcogenides Baranowski, M.; Surrente, A.; Maude, D. K. arXiv https://doi.org/10.48550/arxiv.1701.03070	text	January 2017

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