Excitonic luminescence upconversion in a two-dimensional semiconductor

Jones, Aaron M.; Yu, Hongyi; Schaibley, John R.; Yan, Jiaqiang; Mandrus, David G.; Taniguchi, Takashi; Watanabe, Kenji; Dery, Hanan; Yao, Wang; Xu, Xiaodong

doi:10.1038/nphys3604

Title: Excitonic luminescence upconversion in a two-dimensional semiconductor

Journal Article · Mon Dec 21 00:00:00 EST 2015 · Nature Physics

DOI:https://doi.org/10.1038/nphys3604· OSTI ID:1334437

^[1]; Yu, Hongyi ^[2]; Schaibley, John R. ^[1]; Yan, Jiaqiang ^[3]; Mandrus, David G. ^[3]; Taniguchi, Takashi ^[4];

^[4]; Dery, Hanan ^[5];

^[2];

^[6]

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
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
National Inst. for Materials Science (NIMS), Tsukuba (Japan). Advanced Materials Lab.
Univ. of Rochester, NY (United States). Dept. of Electrical and Computer Engineering
Univ. of Washington, Seattle, WA (United States). Dept. of Physics and Dept. of Materials Science and Engineering

Photon upconversion is an elementary light-matter interaction process in which an absorbed photon is re-emitted at higher frequency after extracting energy from the medium. Furthermore, this phenomenon lies at the heart of optical refrigeration in solids(1), where upconversion relies on anti-Stokes processes enabled either by rare-earth impurities(2) or exciton-phonon coupling(3). We demonstrate a luminescence upconversion process from a negatively charged exciton to a neutral exciton resonance in monolayer WSe2, producing spontaneous anti-Stokes emission with an energy gain of 30 meV. Polarization-resolved measurements find this process to be valley selective, unique to monolayer semiconductors(4). Since the charged exciton binding energy(5) closely matches the 31 meV A(1)' optical phonon(6-9), we ascribe the spontaneous excitonic anti-Stokes to doubly resonant Raman scattering, where the incident and outgoing photons are in resonance with the charged and neutral excitons, respectively. Additionally, we resolve a charged exciton doublet with a 7 meV splitting, probably induced by exchange interactions, and show that anti-Stokes scattering is efficient only when exciting the doublet peak resonant with the phonon, further confirming the excitonic doubly resonant picture.

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

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1334437

Journal Information:: Nature Physics, Vol. 12, Issue 4; ISSN 1745-2473

Publisher:: Nature Publishing Group (NPG)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 152 works

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In-plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules Wang, G.; Robert, C.; Glazov, M. M. arXiv https://doi.org/10.48550/arxiv.1704.05341	text	January 2017
Band nesting, massive Dirac Fermions and Valley Lande and Zeeman effects in transition metal dichalcogenides: a tight-binding model Bieniek, M.; Korkusiński, M.; Szulakowska, L. arXiv https://doi.org/10.48550/arxiv.1705.02917	text	January 2017
Enhanced interlayer neutral excitons and trions in trilayer van der Waals heterostructures Choi, Chanyeol; Huang, Jiahui; Cheng, Hung-Chieh arXiv https://doi.org/10.48550/arxiv.1706.05857	text	January 2017
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
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
Revealing the Biexciton and Trion-exciton Complexes in BN Encapsulated WSe2 Li, Zhipeng; Wang, Tianmeng; Lu, Zhengguang arXiv https://doi.org/10.48550/arxiv.1806.03775	text	January 2018
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
Electroluminescence from multi-particle exciton complexes in transition metal dichalcogenide semiconductors Paur, Matthias; Molina-Mendoza, Aday J.; Bratschitsch, Rudolf arXiv https://doi.org/10.48550/arxiv.1812.03832	text	January 2018

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