Utilizing Ultraviolet Photons to Generate Single-Photon Emitters in Semiconductor Monolayers

Wei Wang; Leighton O. Jones; Jia Shiang Chen; George C. Schatz; Xuedan Ma

doi:10.1021/acsnano.2c09209

Utilizing Ultraviolet Photons to Generate Single-Photon Emitters in Semiconductor Monolayers

Wei Wang, Leighton O. Jones, Jia Shiang Chen, George C. Schatz, Xuedan Ma^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

Abstract

The understanding and controlled creation of atomic defects in semiconductor transition metal dichalcogenides (TMDs) are highly relevant to their applications in high-performance quantum optics and nanoelectronic devices. Here, we demonstrate a versatile approach in generating single-photon emitters in MoS₂monolayers using widely attainable UV light. We discover that only defects engendered by UV photons in vacuum exhibit single-photon-emitter characteristics, whereas those created in air lack quantum emission attributes. In combination with theoretical calculations, we assign the defects generated in vacuum to unpassivated sulfur vacancies, whose highly localized midgap states give rise to single-photon emission. In contrast, UV irradiation of the MoS₂monolayers in air results in oxygen-passivated sulfur vacancies, whose optical properties are likely governed by their pristine band-To-defect band optical transitions. These findings suggest that widely available light sources such as UV light can be utilized for creating quantum photon sources in TMDs.

Original language	English (US)
Pages (from-to)	21240-21247
Number of pages	8
Journal	ACS nano
Volume	16
Issue number	12
DOIs	https://doi.org/10.1021/acsnano.2c09209
State	Published - Dec 27 2022

Keywords

oxygen-passivated defect
quantum defect
single-photon emitter
sulfur vacancy
transition metal dichalcogenides
UV irradiation

ASJC Scopus subject areas

Materials Science(all)
Engineering(all)
Physics and Astronomy(all)

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10.1021/acsnano.2c09209

Cite this

@article{e267aa4dfb324001a2fafb01421be104,

title = "Utilizing Ultraviolet Photons to Generate Single-Photon Emitters in Semiconductor Monolayers",

abstract = "The understanding and controlled creation of atomic defects in semiconductor transition metal dichalcogenides (TMDs) are highly relevant to their applications in high-performance quantum optics and nanoelectronic devices. Here, we demonstrate a versatile approach in generating single-photon emitters in MoS2monolayers using widely attainable UV light. We discover that only defects engendered by UV photons in vacuum exhibit single-photon-emitter characteristics, whereas those created in air lack quantum emission attributes. In combination with theoretical calculations, we assign the defects generated in vacuum to unpassivated sulfur vacancies, whose highly localized midgap states give rise to single-photon emission. In contrast, UV irradiation of the MoS2monolayers in air results in oxygen-passivated sulfur vacancies, whose optical properties are likely governed by their pristine band-To-defect band optical transitions. These findings suggest that widely available light sources such as UV light can be utilized for creating quantum photon sources in TMDs.",

keywords = "oxygen-passivated defect, quantum defect, single-photon emitter, sulfur vacancy, transition metal dichalcogenides, UV irradiation",

author = "Wei Wang and Jones, {Leighton O.} and Chen, {Jia Shiang} and Schatz, {George C.} and Xuedan Ma",

note = "Funding Information: We acknowledge support from the Center for Molecular Quantum Transduction, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under award no. DE-SC0021314 (theoretical calculations). W.W. acknowledges support from the National Science Foundation DMR Program under award no. DMR-1905990 (sample preparation). X.M. acknowledges support from the U.S. Department of Energy, Office of Science, National Quantum Information Science Research Centers for manuscript preparation. Work performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, was supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Publisher Copyright: {\textcopyright} 2022 American Chemical Society. All rights reserved.",

year = "2022",

month = dec,

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doi = "10.1021/acsnano.2c09209",

language = "English (US)",

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journal = "ACS Nano",

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AU - Wang, Wei

AU - Jones, Leighton O.

AU - Chen, Jia Shiang

AU - Schatz, George C.

AU - Ma, Xuedan

N1 - Funding Information: We acknowledge support from the Center for Molecular Quantum Transduction, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under award no. DE-SC0021314 (theoretical calculations). W.W. acknowledges support from the National Science Foundation DMR Program under award no. DMR-1905990 (sample preparation). X.M. acknowledges support from the U.S. Department of Energy, Office of Science, National Quantum Information Science Research Centers for manuscript preparation. Work performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, was supported by the U.S. DOE, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Publisher Copyright: © 2022 American Chemical Society. All rights reserved.

PY - 2022/12/27

Y1 - 2022/12/27

N2 - The understanding and controlled creation of atomic defects in semiconductor transition metal dichalcogenides (TMDs) are highly relevant to their applications in high-performance quantum optics and nanoelectronic devices. Here, we demonstrate a versatile approach in generating single-photon emitters in MoS2monolayers using widely attainable UV light. We discover that only defects engendered by UV photons in vacuum exhibit single-photon-emitter characteristics, whereas those created in air lack quantum emission attributes. In combination with theoretical calculations, we assign the defects generated in vacuum to unpassivated sulfur vacancies, whose highly localized midgap states give rise to single-photon emission. In contrast, UV irradiation of the MoS2monolayers in air results in oxygen-passivated sulfur vacancies, whose optical properties are likely governed by their pristine band-To-defect band optical transitions. These findings suggest that widely available light sources such as UV light can be utilized for creating quantum photon sources in TMDs.

AB - The understanding and controlled creation of atomic defects in semiconductor transition metal dichalcogenides (TMDs) are highly relevant to their applications in high-performance quantum optics and nanoelectronic devices. Here, we demonstrate a versatile approach in generating single-photon emitters in MoS2monolayers using widely attainable UV light. We discover that only defects engendered by UV photons in vacuum exhibit single-photon-emitter characteristics, whereas those created in air lack quantum emission attributes. In combination with theoretical calculations, we assign the defects generated in vacuum to unpassivated sulfur vacancies, whose highly localized midgap states give rise to single-photon emission. In contrast, UV irradiation of the MoS2monolayers in air results in oxygen-passivated sulfur vacancies, whose optical properties are likely governed by their pristine band-To-defect band optical transitions. These findings suggest that widely available light sources such as UV light can be utilized for creating quantum photon sources in TMDs.

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Utilizing Ultraviolet Photons to Generate Single-Photon Emitters in Semiconductor Monolayers

Abstract

Keywords

ASJC Scopus subject areas

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