Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

Selig, Malte; Berghäuser, Gunnar; Raja, Archana; Nagler, Philipp; Schüller, Christian; Heinz, Tony F.; Korn, Tobias; Chernikov, Alexey; Malic, Ermin; Knorr, Andreas

doi:10.1038/ncomms13279

Title: Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

Journal Article · Mon Nov 07 00:00:00 EST 2016 · Nature Communications

DOI:https://doi.org/10.1038/ncomms13279· OSTI ID:1348911

Selig, Malte ^[1]; Berghäuser, Gunnar ^[1]; Raja, Archana ^[2]; Nagler, Philipp ^[3]; Schüller, Christian ^[3]; Heinz, Tony F. ^[4]; Korn, Tobias ^[3]; Chernikov, Alexey ^[5]; Malic, Ermin ^[6]; Knorr, Andreas ^[1]

Technical Univ. of Berlin (Germany). Inst. for Theoretical Physics
Columbia Univ., New York, NY (United States). Dept. of Chemistry; Stanford Univ., CA (United States). Dept. of Applied Physics
Univ. of Regensburg (Germany). Inst. for Experimental and Applied Physics
Stanford Univ., CA (United States). Dept. of Applied Physics; SLAC National Accelerator Lab., Menlo Park, CA (United States); Columbia Univ., New York, NY (United States). Dept. of Physics and Electrical Engineering
Univ. of Regensburg (Germany). Inst. for Experimental and Applied Physics; Columbia Univ., New York, NY (United States). Dept. of Physics and Electrical Engineering
Chalmers Univ. of Technology, Gothenburg (Sweden). Dept. of Physics

Atomically thin transition metal dichalcogenides are direct-gap semiconductors with strong light–matter and Coulomb interactions. The latter accounts for tightly bound excitons, which dominate their optical properties. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in the optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. We investigate the microscopic origin of the excitonic coherence lifetime in two representative materials (WS₂ and MoSe₂) through a study combining microscopic theory with spectroscopic measurements. We also show that the excitonic coherence lifetime is determined by phonon-induced intravalley scattering and intervalley scattering into dark excitonic states. Particularly, we identify exciton relaxation processes involving phonon emission into lower-lying dark states that are operative at all temperatures, in WS₂.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1348911

Journal Information:: Nature Communications, Vol. 7; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 319 works

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Experimental observation of a negative grey trion in an electron-rich WSe 2 monolayer Tu, Jhih-Sian; Borghardt, Sven; Grützmacher, Detlev RWTH Aachen University https://doi.org/10.18154/rwth-2020-04434	text	January 2019
Polariton hyperspectral imaging of two-dimensional semiconductor crystals Gebhardt, Christian; Förg, Michael; Yamaguchi, Hisato Karlsruhe https://doi.org/10.5445/ir/1000098461	text	January 2019
Exciton-phonon relaxation bottleneck and radiative decay of thermal exciton reservoir in two-dimensional materials Slobodeniuk, A. O.; Basko, D. M. arXiv https://doi.org/10.48550/arxiv.1606.08213	text	January 2016
Interlayer exciton dynamics in a dichalcogenide monolayer heterostructure Nagler, Philipp; Plechinger, Gerd; Ballottin, Mariana V. arXiv https://doi.org/10.48550/arxiv.1703.00379	text	January 2017
Direct exciton emission from atomically thin transition metal dichalcogenide heterostructures near the lifetime limit Wierzbowski, Jakob; Klein, Julian; Sigger, Florian arXiv https://doi.org/10.48550/arxiv.1705.00348	text	January 2017
Photonic-Crystal Exciton-Polaritons in Monolayer Semiconductors Zhang, Long; Gogna, Rahul; Burg, Will arXiv https://doi.org/10.48550/arxiv.1706.08464	text	January 2017
Dark excitons in transition metal dichalcogenides Malic, Ermin; Selig, Malte; Feierabend, Maja arXiv https://doi.org/10.48550/arxiv.1709.00941	text	January 2017
Exciton Relaxation Cascade in Two-dimensional Transition-metal dichalcogenides Brem, Samuel; Berghaeuser, Gunnar; Selig, Malte arXiv https://doi.org/10.48550/arxiv.1712.04808	text	January 2017
Two-dimensional semiconductors in the regime of strong light-matter coupling Schneider, Christian; Glazov, Mikhail M.; Korn, Tobias arXiv https://doi.org/10.48550/arxiv.1804.06771	text	January 2018
Exciton diffusion and halo effects in monolayer semiconductors Kulig, Marvin; Zipfel, Jonas; Nagler, Philipp arXiv https://doi.org/10.48550/arxiv.1804.09386	text	January 2018
Investigation of indirect excitons in bulk $2H$-MoS$_2$ using transmission electron energy-loss spectroscopy Habenicht, Carsten; Schuster, Roman; Knupfer, Martin arXiv https://doi.org/10.48550/arxiv.1805.01826	text	January 2018
Impact of strain on the excitonic linewidth in transition metal dichalcogenides Khatibi, Zahra; Feierabend, Maja; Selig, Malte arXiv https://doi.org/10.48550/arxiv.1806.07315	text	January 2018
Nonlinear excitonic spin Hall effect in monolayer transition metal dichalcogenides Taghizadeh, Alireza; Pedersen, T. G. arXiv https://doi.org/10.48550/arxiv.1812.02596	preprint	January 2018
Fundamental exciton linewidth broadening in monolayer transition metal dichalcogenides Gupta, Garima; Majumdar, Kausik arXiv https://doi.org/10.48550/arxiv.1901.04391	text	January 2019
Controlling excitons in an atomically thin membrane with a mirror Zhou, You; Scuri, Giovanni; Sung, Jiho arXiv https://doi.org/10.48550/arxiv.1901.08500	text	January 2019
Long valley lifetime of dark excitons in single-layer WSe2 Tang, Yanhao; Mak, Kin Fai; Shan, Jie arXiv https://doi.org/10.48550/arxiv.1903.12586	text	January 2019
Intrinsic Lifetime of Higher Excitonic States in Tungsten Diselenide Monolayers Brem, Samuel; Zipfel, Jonas; Selig, Malte arXiv https://doi.org/10.48550/arxiv.1904.04729	text	January 2019
Phonon wind and drag of excitons in monolayer semiconductors Glazov, M. M. arXiv https://doi.org/10.48550/arxiv.1905.01621	text	January 2019
Theory of exciton dynamics in time-resolved ARPES: intra- and intervalley scattering in two-dimensional semiconductors Christiansen, Dominik; Selig, Malte; Malic, Ermin arXiv https://doi.org/10.48550/arxiv.1907.01842	text	January 2019
Optical fingerprint of bright and dark localized excitonic states in atomically thin 2D materials Feierabend, Maja; Brem, Samuel; Malic, Ermin arXiv https://doi.org/10.48550/arxiv.1908.05071	text	January 2019
Colloquium : Excitons in atomically thin transition metal dichalcogenides Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M. Universität Regensburg https://doi.org/10.5283/epub.40518	text	January 2018
Phase-matching-free parametric oscillators based on two-dimensional semiconductors Ciattoni, Alessandro; Marini, Andrea; Rizza, Carlo Light: Science & Applications, Vol. 7, Issue 1 https://doi.org/10.1038/s41377-018-0011-3	journal	May 2018
Dispersion and decay rate of exciton-polaritons and radiative modes in transition metal dichalcogenide monolayers Alpeggiani, Filippo; Gong, Su-Hyun; Kuipers, L. Physical Review B, Vol. 97, Issue 20 https://doi.org/10.1103/physrevb.97.205436	journal	May 2018
Time- and angle-resolved photoemission spectroscopy on bidimensional semiconductors with a 500 kHz extreme ultraviolet light source Puppin, Michele Freie Universität Berlin https://doi.org/10.17169/refubium-804	other	January 2018
Excitonic linewidth approaching the homogeneous limit in MoS2 based van der Waals heterostructures : accessing spin-valley dynamics Cadiz, F.; Courtade, E.; Robert, C. arXiv https://doi.org/10.48550/arxiv.1702.00323	text	January 2017
Exciton-exciton interaction in transition-metal dichalcogenide monolayers Shahnazaryan, V.; Iorsh, I.; Shelykh, I. A. arXiv https://doi.org/10.48550/arxiv.1706.01817	text	January 2017
Superior valley polarization and coherence of 2s excitons in monolayer WSe2 Chen, Shao-Yu; Goldstein, Thomas; Tong, Jiayue arXiv https://doi.org/10.48550/arxiv.1712.02924	text	January 2017
Interlayer exciton dynamics in van der Waals heterostructures Ovesen, Simon; Brem, Samuel; Linderälv, Christopher arXiv https://doi.org/10.48550/arxiv.1804.08412	preprint	January 2018
Mapping of the energetically lowest exciton in bulk $1T$-HfS$_2$ Habenicht, Carsten; Sponza, Lorenzo; Schuster, Roman arXiv https://doi.org/10.48550/arxiv.1808.01641	text	January 2018
Many-Body Simulation of Two-Dimensional Electronic Spectroscopy of Excitons and Trions in Monolayer Transition-Metal Dichalcogenides Tempelaar, Roel; Berkelbach, Timothy C. arXiv https://doi.org/10.48550/arxiv.1810.06570	text	January 2018
Self-consistent screening enhances stability of the nonequilibrium excitonic insulator phase Perfetto, E.; Marini, A.; Stefanucci, G. arXiv https://doi.org/10.48550/arxiv.2008.11417	text	January 2020
Hybridized intervalley moiré excitons and flat bands in twisted WSe2 bilayers Brem, Samuel; Lin, Kai-Qiang; Gillen, Roland Universität Regensburg https://doi.org/10.5283/epub.43868	text	January 2020

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