Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides

Moody, Galan; Dass, Chandriker Kavir; Hao, Kai; Chen, Chang -Hsiao; Li, Lain -Jong; Singh, Akshay; Tran, Kha; Clark, Genevieve; Xu, Xiaodong; Berghauser, Gunnar; Malic, Ermin; Knorr, Andreas; Li, Xiaoqin

doi:10.1038/ncomms9315

Title: Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides

Journal Article · 17 September 2015 · Nature Communications

DOI: https://doi.org/10.1038/ncomms9315 · OSTI ID:1441157

Moody, Galan ^[1]; Dass, Chandriker Kavir ^[2]; Hao, Kai ^[3]; Chen, Chang -Hsiao ^[4]; Li, Lain -Jong ^[2]; Singh, Akshay ^[2]; Tran, Kha ^[2]; Clark, Genevieve ^[5]; Xu, Xiaodong ^[5]; Berghauser, Gunnar ^[6]; Malic, Ermin ^[7]; Knorr, Andreas ^[6]; Li, Xiaoqin ^[2]

Univ. of Texas at Austin, Austin, TX (United States); National Institute of Standards & Technology, Boulder, CO (United States); University of Texas
Univ. of Texas at Austin, Austin, TX (United States)
Feng Chia Univ., Taichung (Taiwan)
King Abdullah Univ. of Science & Technology (KAUST), Thuwal (Saudi Arabia)
Univ. of Washington, Seattle, WA (United States)
Technische Univ. Berlin, Berlin (Germany)
Chalmers Univ. of Technology, Gothenburg (Sweden)

In this paper, the band-edge optical response of transition metal dichalcogenides, an emerging class of atomically thin semiconductors, is dominated by tightly bound excitons localized at the corners of the Brillouin zone (valley excitons). A fundamental yet unknown property of valley excitons in these materials is the intrinsic homogeneous linewidth, which reflects irreversible quantum dissipation arising from system (exciton) and bath (vacuum and other quasiparticles) interactions and determines the timescale during which excitons can be coherently manipulated. Here we use optical two-dimensional Fourier transform spectroscopy to measure the exciton homogeneous linewidth in monolayer tungsten diselenide (WSe₂). The homogeneous linewidth is found to be nearly two orders of magnitude narrower than the inhomogeneous width at low temperatures. We evaluate quantitatively the role of exciton–exciton and exciton–phonon interactions and population relaxation as linewidth broadening mechanisms. The key insights reported here—strong many-body effects and intrinsically rapid radiative recombination—are expected to be ubiquitous in atomically thin semiconductors.

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Research Organization:: Univ. of Washington, Seattle, WA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0008145

OSTI ID:: 1441157

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 6; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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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
Exciton-plasmon Coupling and Electromagnetically Induced Transparency in Monolayer Semiconductors Hybridized with Ag Nanoparticles Weijie, Zhao; Shunfeng, Wang; Bo, Liu arXiv https://doi.org/10.48550/arxiv.1601.05573	text	January 2016
Exciton Radiative Lifetime in Transition Metal Dichalcogenide Monolayers Robert, C.; Lagarde, D.; Cadiz, F. arXiv https://doi.org/10.48550/arxiv.1603.00277	text	January 2016
Nonequilibrium Carrier Dynamics in Transition Metal Dichalcogenide Semiconductors Steinhoff, Alexander; Florian, Matthias; Rösner, Malte arXiv https://doi.org/10.48550/arxiv.1603.03633	text	January 2016
Two-dimensional Fröhlich interaction in transition-metal dichalcogenide monolayers: Theoretical modeling and first-principles calculations Sohier, Thibault; Calandra, Matteo; Mauri, Francesco arXiv https://doi.org/10.48550/arxiv.1605.08207	text	January 2016
Probing Many-Body Interactions in Monolayer Transition-Metal Dichalcogenides Van Tuan, Dinh; Scharf, Benedikt; Wang, Zefang arXiv https://doi.org/10.48550/arxiv.1606.07101	text	January 2016
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
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
Impact of environment on dynamics of exciton complexes in a WS$_2$ monolayer Jakubczyk, T.; Nogajewski, K.; Molas, M. R. arXiv https://doi.org/10.48550/arxiv.1709.02658	preprint	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
Complexes of dipolar excitons in layered quasi-two-dimensional nanostructures Bondarev, Igor V.; Vladimirova, Maria R. arXiv https://doi.org/10.48550/arxiv.1712.10312	text	January 2017
Dynamical screening in monolayer transition-metal dichalcogenides and its manifestations in the exciton spectrum Scharf, Benedikt; Van Tuan, Dinh; Žutić, Igor arXiv https://doi.org/10.48550/arxiv.1801.06217	text	January 2018
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
Virtual trions in the photoluminescence of monolayer transition-metal dichalcogenides Van Tuan, Dinh; Jones, Aaron M.; Yang, Min arXiv https://doi.org/10.48550/arxiv.1805.08722	text	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
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
Chiral light-matter interactions using spin-valley states in transition metal dichalcogenides Yang, Zhili; Aghaeimeibodi, Shahriar; Waks, Edo arXiv https://doi.org/10.48550/arxiv.1904.12349	text	January 2019
Enhanced screening and spectral diversity in many-body elastic scattering of excitons in two-dimensional hybrid metal-halide perovskites Thouin, Félix; Cortecchia, Daniele; Petrozza, Annamaria arXiv https://doi.org/10.48550/arxiv.1904.12402	text	January 2019
Excitonic magneto-optics in monolayer transition metal dichalcogenides: From nanoribbons to two-dimensional response Have, J.; Peres, N. M. R.; Pedersen, T. G. arXiv https://doi.org/10.48550/arxiv.1905.06651	text	January 2019
Room temperature nanocavity laser with interlayer excitons in 2D heterostructures Liu, Yuanda; Fang, Hanlin; Rasmita, Abdullah arXiv https://doi.org/10.48550/arxiv.1911.12629	preprint	January 2019
Mapping of the dark exciton landscape in transition metal dichalcogenides Berghäuser, Gunnar; Steinleitner, Philipp; Merkl, Philipp Universität Regensburg https://doi.org/10.5283/epub.37987	text	January 2018
Quantum interference in second-harmonic generation from monolayer WSe2 Lin, Kai-Qiang; Bange, Sebastian; Lupton, John M. Universität Regensburg https://doi.org/10.5283/epub.40543	text	January 2019
Dielectric Properties of NbxW1-xSe2 Alloys Rigosi, Albert F.; Hill, Heather; Krylyuk, Sergiy Journal of Research of the National Institute of Standards and Technology, Vol. 124 https://doi.org/10.6028/jres.124.035	journal	January 2019

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