Improving Strain-localized GaSe Single Photon Emitters with Electrical Doping

Weijun Luo; Alexander Puretzky; Benjamin Lawrie; Qishuo Tan; Hongze Gao; Anna K. Swan; Liangbo Liang; Xi Ling

doi:10.1021/acs.nanolett.3c02308

Improving Strain-localized GaSe Single Photon Emitters with Electrical Doping

Weijun Luo, Alexander Puretzky, Benjamin Lawrie, Qishuo Tan, Hongze Gao, Anna K. Swan, Liangbo Liang, Xi Ling

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

2 Scopus citations

Abstract

Exciton localization through nanoscale strain has been used to create highly efficient single-photon emitters (SPEs) in 2D materials. However, the strong Coulomb interactions between excitons can lead to nonradiative recombination through exciton-exciton annihilation, negatively impacting SPE performance. Here, we investigate the effect of Coulomb interactions on the brightness, single photon purity, and operating temperatures of strain-localized GaSe SPEs by using electrostatic doping. By gating GaSe to the charge neutrality point, the exciton-exciton annihilation nonradiative pathway is suppressed, leading to ∼60% improvement of emission intensity and an enhancement of the single photon purity g⁽²⁾(0) from 0.55 to 0.28. The operating temperature also increased from 4.5 K to 85 K consequently. This research provides insight into many-body interactions in excitons confined by nanoscale strain and lays the groundwork for the optimization of SPEs for optoelectronics and quantum photonics.

Original language	English
Pages (from-to)	9740-9747
Number of pages	8
Journal	Nano Letters
Volume	23
Issue number	21
DOIs	https://doi.org/10.1021/acs.nanolett.3c02308
State	Published - Nov 8 2023

Funding

This material is based upon work supported by the National Science Foundation (NSF) under Grant No. (1945364). Work by X.L. was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) under Award DE-SC0021064. W.L., X.L., and A.K.S acknowledge the support of National Science Foundation (NSF) under Grant No. (2111160). The photoluminescence and photon statistics measurements were performed at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy Office of Science User Facility. W.L. acknowledges Dr. Y. Y. Pai from Oak Ridge National Laboratory for his help with experimental automation. X.L. and A.K.S. acknowledge the membership of the Photonics Center at Boston University. The computational work is performed using Shared Computing Cluster (BUSCC) at Boston University. This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). This material is based upon work supported by the National Science Foundation (NSF) under Grant No. (1945364). Work by X.L. was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES) under Award DE-SC0021064. W.L., X.L., and A.K.S acknowledge the support of National Science Foundation (NSF) under Grant No. (2111160). The photoluminescence and photon statistics measurements were performed at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy Office of Science User Facility. W.L. acknowledges Dr. Y. Y. Pai from Oak Ridge National Laboratory for his help with experimental automation. X.L. and A.K.S. acknowledge the membership of the Photonics Center at Boston University. The computational work is performed using Shared Computing Cluster (BUSCC) at Boston University. This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

Funders	Funder number
DOE Public Access Plan
National Science Foundation	1945364
U.S. Department of Energy
Office of Science
Basic Energy Sciences	DE-AC05-00OR22725, 2111160, DE-SC0021064
Boston University

Keywords

Fermi level
electrostatic doping
gallium selenide
single photon emission
strain engineering
two-dimensional materials

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10.1021/acs.nanolett.3c02308

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title = "Improving Strain-localized GaSe Single Photon Emitters with Electrical Doping",

abstract = "Exciton localization through nanoscale strain has been used to create highly efficient single-photon emitters (SPEs) in 2D materials. However, the strong Coulomb interactions between excitons can lead to nonradiative recombination through exciton-exciton annihilation, negatively impacting SPE performance. Here, we investigate the effect of Coulomb interactions on the brightness, single photon purity, and operating temperatures of strain-localized GaSe SPEs by using electrostatic doping. By gating GaSe to the charge neutrality point, the exciton-exciton annihilation nonradiative pathway is suppressed, leading to ∼60% improvement of emission intensity and an enhancement of the single photon purity g(2)(0) from 0.55 to 0.28. The operating temperature also increased from 4.5 K to 85 K consequently. This research provides insight into many-body interactions in excitons confined by nanoscale strain and lays the groundwork for the optimization of SPEs for optoelectronics and quantum photonics.",

keywords = "Fermi level, electrostatic doping, gallium selenide, single photon emission, strain engineering, two-dimensional materials",

author = "Weijun Luo and Alexander Puretzky and Benjamin Lawrie and Qishuo Tan and Hongze Gao and Swan, {Anna K.} and Liangbo Liang and Xi Ling",

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AU - Luo, Weijun

AU - Puretzky, Alexander

AU - Lawrie, Benjamin

AU - Tan, Qishuo

AU - Gao, Hongze

AU - Swan, Anna K.

AU - Liang, Liangbo

AU - Ling, Xi

PY - 2023/11/8

Y1 - 2023/11/8

N2 - Exciton localization through nanoscale strain has been used to create highly efficient single-photon emitters (SPEs) in 2D materials. However, the strong Coulomb interactions between excitons can lead to nonradiative recombination through exciton-exciton annihilation, negatively impacting SPE performance. Here, we investigate the effect of Coulomb interactions on the brightness, single photon purity, and operating temperatures of strain-localized GaSe SPEs by using electrostatic doping. By gating GaSe to the charge neutrality point, the exciton-exciton annihilation nonradiative pathway is suppressed, leading to ∼60% improvement of emission intensity and an enhancement of the single photon purity g(2)(0) from 0.55 to 0.28. The operating temperature also increased from 4.5 K to 85 K consequently. This research provides insight into many-body interactions in excitons confined by nanoscale strain and lays the groundwork for the optimization of SPEs for optoelectronics and quantum photonics.

AB - Exciton localization through nanoscale strain has been used to create highly efficient single-photon emitters (SPEs) in 2D materials. However, the strong Coulomb interactions between excitons can lead to nonradiative recombination through exciton-exciton annihilation, negatively impacting SPE performance. Here, we investigate the effect of Coulomb interactions on the brightness, single photon purity, and operating temperatures of strain-localized GaSe SPEs by using electrostatic doping. By gating GaSe to the charge neutrality point, the exciton-exciton annihilation nonradiative pathway is suppressed, leading to ∼60% improvement of emission intensity and an enhancement of the single photon purity g(2)(0) from 0.55 to 0.28. The operating temperature also increased from 4.5 K to 85 K consequently. This research provides insight into many-body interactions in excitons confined by nanoscale strain and lays the groundwork for the optimization of SPEs for optoelectronics and quantum photonics.

KW - Fermi level

KW - electrostatic doping

KW - gallium selenide

KW - single photon emission

KW - strain engineering

KW - two-dimensional materials

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Improving Strain-localized GaSe Single Photon Emitters with Electrical Doping

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Keywords

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