Intrinsic donor-bound excitons in ultraclean monolayer semiconductors

Pasqual Rivera, Minhao He, Bumho Kim, Song Liu, Carmen Rubio-Verdú, Hyowon Moon, Lukas Mennel, Daniel A. Rhodes, Hongyi Yu, Takashi Taniguchi, Kenji Watanabe, Jiaqiang Yan, David G. Mandrus, Hanan Dery, Abhay Pasupathy, Dirk Englund, James Hone (), Wang Yao () and Xiaodong Xu ()
Additional contact information
Pasqual Rivera: University of Washington
Minhao He: University of Washington
Bumho Kim: Columbia University
Song Liu: Columbia University
Carmen Rubio-Verdú: Columbia University
Hyowon Moon: Massachusetts Institute of Technology
Lukas Mennel: Massachusetts Institute of Technology
Daniel A. Rhodes: Columbia University
Hongyi Yu: and HKU-UCAS Joint Institute of Theoretical and Computational Physics at Hong Kong
Takashi Taniguchi: National Institute for Materials Science, Tsukuba
Kenji Watanabe: National Institute for Materials Science, Tsukuba
Jiaqiang Yan: Oak Ridge National Laboratory
David G. Mandrus: Oak Ridge National Laboratory
Hanan Dery: University of Rochester
Abhay Pasupathy: Columbia University
Dirk Englund: Massachusetts Institute of Technology
James Hone: Columbia University
Wang Yao: and HKU-UCAS Joint Institute of Theoretical and Computational Physics at Hong Kong
Xiaodong Xu: University of Washington

Nature Communications, 2021, vol. 12, issue 1, 1-8

Abstract: 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 satellitesʼ 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.

Date: 2021
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DOI: 10.1038/s41467-021-21158-8

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