Intrinsic donor-bound excitons in ultraclean monolayer semiconductors
Abstract
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.
- Authors:
-
[1];
[1];
[6];
[7];
[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
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1779113
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
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, and Xu, Xiaodong. Intrinsic donor-bound excitons in ultraclean monolayer semiconductors. United States: N. p., 2021.
Web. doi:10.1038/s41467-021-21158-8.
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. Intrinsic donor-bound excitons in ultraclean monolayer semiconductors. United States. https://doi.org/10.1038/s41467-021-21158-8
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, and Xu, Xiaodong. Mon .
"Intrinsic donor-bound excitons in ultraclean monolayer semiconductors". United States. https://doi.org/10.1038/s41467-021-21158-8. https://www.osti.gov/servlets/purl/1779113.
@article{osti_1779113,
title = {Intrinsic donor-bound excitons in ultraclean monolayer semiconductors},
author = {Rivera, Pasqual and He, Minhao and Kim, Bumho and Liu, Song and Rubio-Verdú, Carmen and Moon, Hyowon and Mennel, Lukas and Rhodes, Daniel A. and Yu, Hongyi and Taniguchi, Takashi and Watanabe, Kenji and Yan, Jiaqiang and Mandrus, David G. and Dery, Hanan and Pasupathy, Abhay and Englund, Dirk and Hone, James and Yao, Wang and Xu, Xiaodong},
abstractNote = {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.},
doi = {10.1038/s41467-021-21158-8},
journal = {Nature Communications},
number = 1,
volume = 12,
place = {United States},
year = {Mon Feb 08 00:00:00 EST 2021},
month = {Mon Feb 08 00:00:00 EST 2021}
}
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