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; Xiaodong Xu

doi:10.1038/s41467-021-21158-8

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, Xiaodong Xu

Correlated Electron Materials

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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.

Original language	English
Article number	871
Journal	Nature Communications
Volume	12
Issue number	1
DOIs	https://doi.org/10.1038/s41467-021-21158-8
State	Published - Dec 1 2021

Funding

This work was mainly supported by Army Research Office (ARO) Multidisciplinary University Research Initiative (MURI) program (grant no. W911NF-18-1-0431) and NSF EFRI (Grant No. 1741656). Time-resolved measurements are supported by the Department of Energy, Basic Energy Sciences, Materials Sciences and Engineering Division (DE-SC0018171). H.M. acknowledges support from a Samsung Scholarship. DE acknowledges partial support from the NSF Center for Integrated Quantum Materials (CIQM). W.Y. and H.Y. were supported by the Research Grants Council of Hong Kong (C7036-17W), and the University of Hong Kong Seed Funding for Strategic Interdisciplinary Research. D.G.M. and J.Y. were supported by the US Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. WSe2 synthesis and STM characterization were supported by the NSF MRSEC program through Columbia in the Center for Precision Assembly of Superstratic and Superatomic Solids (DMR-1420634). K.W. and T.T. acknowledge the support from the Elemental Strategy Initiative conducted by the MEXT, Japan, Grant Number JPMXP0112101001, JSPS KAKENHI Grant Numbers JP20H00354 and the CREST(JPMJCR15F3), JST. H.D. is supported by the Department of Energy, Basic Energy Sciences, under Award No. DE-SC0014349. X.X. acknowledges the support from the State of Washington funded Clean Energy Institute and from the Boeing Distinguished Professorship in Physics.

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Rivera, P., He, M., Kim, B., Liu, S., Rubio-Verdú, C., Moon, H., Mennel, L., Rhodes, D. A., Yu, H., Taniguchi, T., Watanabe, K., Yan, J., Mandrus, D. G., Dery, H., Pasupathy, A., Englund, D., Hone, J., Yao, W., & Xu, X. (2021). Intrinsic donor-bound excitons in ultraclean monolayer semiconductors. Nature Communications, 12(1), Article 871. https://doi.org/10.1038/s41467-021-21158-8

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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.",

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AU - Dery, Hanan

AU - Pasupathy, Abhay

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AU - Yao, Wang

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N2 - 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.

AB - 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.

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Intrinsic donor-bound excitons in ultraclean monolayer semiconductors

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