Intrinsic donor-bound excitons in ultraclean monolayer semiconductors

Rivera, Pasqual; He, Minhao; Kim, Bumho; Liu, Song; Rubio-Verdú, Carmen; Moon, Hyowon; Mennel, Lukas; Rhodes, Daniel A.; Yu, Hongyi; Taniguchi, Takashi; Watanabe, Kenji; Yan, Jiaqiang; Mandrus, David G.; Dery, Hanan; Pasupathy, Abhay; Englund, Dirk; Hone, James; Yao, Wang; Xu, Xiaodong

doi:10.1038/s41467-021-21158-8

Intrinsic donor-bound excitons in ultraclean monolayer semiconductors

Journal Article · Mon Feb 08 00:00:00 EST 2021 · Nature Communications

DOI:https://doi.org/10.1038/s41467-021-21158-8· OSTI ID:1779113

^[1]; ^[1]; Kim, Bumho ^[2]; Liu, Song ^[2]; Rubio-Verdú, Carmen ^[3]; Moon, Hyowon ^[4]; Mennel, Lukas ^[4]; Rhodes, Daniel A. ^[2]; Yu, Hongyi ^[5]; ^[6]; ^[7]; Yan, Jiaqiang ^[8]; Mandrus, David G. ^[9]; Dery, Hanan ^[10]; ^[3]; ^[4]; ^[2]; ^[5]; ^[11]

Univ. of Washington, Seattle, WA (United States). Dept. of Physics
Columbia Univ., New York, NY (United States). Dept. of Mechanical Engineering
Columbia Univ., New York, NY (United States). Dept. of Physics
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Electrical Engineering and Computer Science
Univ. of Hong Kong and HKU-UCAS Joint Institute of Theoretical and Computational Physics (Hong Kong)
National Inst. for Materials Science (NIMS), Tsukuba (Japan). International Center for Materials Nanoarchitectonics
National Inst. for Materials Science (NIMS), Tsukuba (Japan). Research Center for Functional Materials
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Div.; 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 Div.; 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 Rochester, NY (United States). Dept. of Electrical and Computer Engineering
Univ. of Washington, Seattle, WA (United States). Dept. of Physics; Univ. of Washington, Seattle, WA (United States). Dept. of Materials Science and Engineering

The monolayer transition metal dichalcogenides are an emergent semiconductor platform exhibiting rich excitonic physics with coupled spin-valley degree of freedom and optical addressability. Here, we report a new series of low energy excitonic emission lines in the photoluminescence spectrum of ultraclean monolayer WSe₂. These excitonic satellites are composed of three major peaks with energy separations matching known phonons, and appear only with electron doping. They possess homogenous spatial and spectral distribution, strong power saturation, and anomalously long population (>6 µs) and polarization lifetimes (>100 ns). Resonant excitation of the free inter- and intravalley bright trions leads to opposite optical orientation of the satellites, while excitation of the free dark trion resonance suppresses the satellites' photoluminescence. Defect-controlled crystal synthesis and scanning tunneling microscopy measurements provide corroboration that these features are dark excitons bound to dilute donors, along with associated phonon replicas. Our work opens opportunities to engineer homogenous single emitters and explore collective quantum optical phenomena using intrinsic donor-bound excitons in ultraclean 2D semiconductors.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1779113

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 12; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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