Photoluminescence Induced by Substitutional Nitrogen in Single-Layer Tungsten Disulfide

Qingkai Qian; Wenjing Wu; Lintao Peng; Yuanxi Wang; Anne Marie Z. Tan; Liangbo Liang; Saban M. Hus; Ke Wang; Tanushree H. Choudhury; Joan M. Redwing; Alexander A. Puretzky; David B. Geohegan; Richard G. Hennig; Xuedan Ma; Shengxi Huang

doi:10.1021/acsnano.1c09809

Photoluminescence Induced by Substitutional Nitrogen in Single-Layer Tungsten Disulfide

Qingkai Qian, Wenjing Wu, Lintao Peng, Yuanxi Wang, Anne Marie Z. Tan, Liangbo Liang, Saban M. Hus, Ke Wang, Tanushree H. Choudhury, Joan M. Redwing, Alexander A. Puretzky, David B. Geohegan, Richard G. Hennig, Xuedan Ma, Shengxi Huang

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11 Scopus citations

Abstract

The electronic and optical properties of two-dimensional materials can be strongly influenced by defects, some of which can find significant implementations, such as controllable doping, prolonged valley lifetime, and single-photon emissions. In this work, we demonstrate that defects created by remote N₂ plasma exposure in single-layer WS₂ can induce a distinct low-energy photoluminescence (PL) peak at 1.59 eV, which is in sharp contrast to that caused by remote Ar plasma. This PL peak has a critical requirement on the N₂ plasma exposure dose, which is strongest for WS₂ with about 2.0% sulfur deficiencies (including substitutions and vacancies) and vanishes at 5.6% or higher sulfur deficiencies. Both experiments and first-principles calculations suggest that this 1.59 eV PL peak is caused by defects related to the sulfur substitutions by nitrogen, even though low-temperature PL measurements also reveal that not all the sulfur vacancies are remedied by the substitutional nitrogen. The distinct low-energy PL peak suggests that the substitutional nitrogen defect in single-layer WS₂ can potentially serve as an isolated artificial atom for creating single-photon emitters, and its intensity can also be used to monitor the doping concentrations of substitutional nitrogen.

Original language	English
Pages (from-to)	7428-7437
Number of pages	10
Journal	ACS Nano
Volume	16
Issue number	5
DOIs	https://doi.org/10.1021/acsnano.1c09809
State	Published - May 24 2022

Funding

S.H. and W.W. acknowledge the support from the National Science Foundation under grant number ECCS-1943895. First-principles calculations for this research were performed on the Pennsylvania State University\u2019s Institute for Computational and Data Sciences Advanced CyberInfrastructure (ICDS-ACI). 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. Part of low-temperature PL measurements was supported by the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. The MOCVD WS2 samples were produced in the 2D Crystal Consortium-Materials Innovation Platform (2DCC-MIP) facility under NSF cooperative agreements DMR-1539916 and DMR-2039351. S.H. and W.W. acknowledge the support from the National Science Foundation under grant number ECCS-1943895. First-principles calculations for this research were performed on the Pennsylvania State University\u2019s Institute for Computational and Data Sciences Advanced CyberInfrastructure (ICDS-ACI). 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. Part of low-temperature PL measurements was supported by the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. The MOCVD WS samples were produced in the 2D Crystal Consortium-Materials Innovation Platform (2DCC-MIP) facility under NSF cooperative agreements DMR-1539916 and DMR-2039351. 2

Keywords

WS
first-principles calculations
nitrogen plasma
photoluminescence
substitution

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title = "Photoluminescence Induced by Substitutional Nitrogen in Single-Layer Tungsten Disulfide",

abstract = "The electronic and optical properties of two-dimensional materials can be strongly influenced by defects, some of which can find significant implementations, such as controllable doping, prolonged valley lifetime, and single-photon emissions. In this work, we demonstrate that defects created by remote N2 plasma exposure in single-layer WS2 can induce a distinct low-energy photoluminescence (PL) peak at 1.59 eV, which is in sharp contrast to that caused by remote Ar plasma. This PL peak has a critical requirement on the N2 plasma exposure dose, which is strongest for WS2 with about 2.0% sulfur deficiencies (including substitutions and vacancies) and vanishes at 5.6% or higher sulfur deficiencies. Both experiments and first-principles calculations suggest that this 1.59 eV PL peak is caused by defects related to the sulfur substitutions by nitrogen, even though low-temperature PL measurements also reveal that not all the sulfur vacancies are remedied by the substitutional nitrogen. The distinct low-energy PL peak suggests that the substitutional nitrogen defect in single-layer WS2 can potentially serve as an isolated artificial atom for creating single-photon emitters, and its intensity can also be used to monitor the doping concentrations of substitutional nitrogen.",

keywords = "WS, first-principles calculations, nitrogen plasma, photoluminescence, substitution",

author = "Qingkai Qian and Wenjing Wu and Lintao Peng and Yuanxi Wang and Tan, {Anne Marie Z.} and Liangbo Liang and Hus, {Saban M.} and Ke Wang and Choudhury, {Tanushree H.} and Redwing, {Joan M.} and Puretzky, {Alexander A.} and Geohegan, {David B.} and Hennig, {Richard G.} and Xuedan Ma and Shengxi Huang",

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language = "English",

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AU - Qian, Qingkai

AU - Wu, Wenjing

AU - Peng, Lintao

AU - Wang, Yuanxi

AU - Tan, Anne Marie Z.

AU - Liang, Liangbo

AU - Hus, Saban M.

AU - Wang, Ke

AU - Choudhury, Tanushree H.

AU - Redwing, Joan M.

AU - Puretzky, Alexander A.

AU - Geohegan, David B.

AU - Hennig, Richard G.

AU - Ma, Xuedan

AU - Huang, Shengxi

PY - 2022/5/24

Y1 - 2022/5/24

N2 - The electronic and optical properties of two-dimensional materials can be strongly influenced by defects, some of which can find significant implementations, such as controllable doping, prolonged valley lifetime, and single-photon emissions. In this work, we demonstrate that defects created by remote N2 plasma exposure in single-layer WS2 can induce a distinct low-energy photoluminescence (PL) peak at 1.59 eV, which is in sharp contrast to that caused by remote Ar plasma. This PL peak has a critical requirement on the N2 plasma exposure dose, which is strongest for WS2 with about 2.0% sulfur deficiencies (including substitutions and vacancies) and vanishes at 5.6% or higher sulfur deficiencies. Both experiments and first-principles calculations suggest that this 1.59 eV PL peak is caused by defects related to the sulfur substitutions by nitrogen, even though low-temperature PL measurements also reveal that not all the sulfur vacancies are remedied by the substitutional nitrogen. The distinct low-energy PL peak suggests that the substitutional nitrogen defect in single-layer WS2 can potentially serve as an isolated artificial atom for creating single-photon emitters, and its intensity can also be used to monitor the doping concentrations of substitutional nitrogen.

AB - The electronic and optical properties of two-dimensional materials can be strongly influenced by defects, some of which can find significant implementations, such as controllable doping, prolonged valley lifetime, and single-photon emissions. In this work, we demonstrate that defects created by remote N2 plasma exposure in single-layer WS2 can induce a distinct low-energy photoluminescence (PL) peak at 1.59 eV, which is in sharp contrast to that caused by remote Ar plasma. This PL peak has a critical requirement on the N2 plasma exposure dose, which is strongest for WS2 with about 2.0% sulfur deficiencies (including substitutions and vacancies) and vanishes at 5.6% or higher sulfur deficiencies. Both experiments and first-principles calculations suggest that this 1.59 eV PL peak is caused by defects related to the sulfur substitutions by nitrogen, even though low-temperature PL measurements also reveal that not all the sulfur vacancies are remedied by the substitutional nitrogen. The distinct low-energy PL peak suggests that the substitutional nitrogen defect in single-layer WS2 can potentially serve as an isolated artificial atom for creating single-photon emitters, and its intensity can also be used to monitor the doping concentrations of substitutional nitrogen.

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Photoluminescence Induced by Substitutional Nitrogen in Single-Layer Tungsten Disulfide

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