Imaging Strain-Localized Single-Photon Emitters in Layered GaSe below the Diffraction Limit

Weijun Luo; Benjamin J. Lawrie; Alexander A. Puretzky; Qishuo Tan; Hongze Gao; David B. Lingerfelt; Gage Eichman; Edward Mcgee; Anna K. Swan; Liangbo Liang; Xi Ling

doi:10.1021/acsnano.3c05250

Imaging Strain-Localized Single-Photon Emitters in Layered GaSe below the Diffraction Limit

Weijun Luo, Benjamin J. Lawrie, Alexander A. Puretzky, Qishuo Tan, Hongze Gao, David B. Lingerfelt, Gage Eichman, Edward Mcgee, Anna K. Swan, Liangbo Liang, Xi Ling

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

1 Scopus citations

Abstract

Nanoscale strain control of exciton funneling is an increasingly critical tool for the scalable production of single photon emitters (SPEs) in two-dimensional materials. However, conventional far-field optical microscopies remain constrained in spatial resolution by the diffraction limit and thus can provide only a limited description of nanoscale strain localization of SPEs. Here, we quantify the effects of nanoscale heterogeneous strain on the energy and brightness of GaSe SPEs on nanopillars with correlative cathodoluminescence, photoluminescence, and atomic force microscopy, supported by density functional theory simulations. We report the strain-localized SPEs have a broad range of emission wavelengths from 620 to 900 nm. We reveal substantial strain-controlled SPE wavelength tunability over a ∼100 nm spectral range and 2 orders of magnitude enhancement in the SPE brightness at the pillar center due to Type-I exciton funneling. In addition, we show that radiative biexciton cascade processes contribute to observed CL photon superbunching. Also, the GaSe SPEs show excellent stability, where their properties remain unchanged after electron beam exposure. We anticipate that this comprehensive study on the nanoscale strain control of two-dimensional SPEs will provide key insights to guide the development of truly deterministic quantum photonics.

Original language	English
Pages (from-to)	23455-23465
Number of pages	11
Journal	ACS Nano
Volume	17
Issue number	23
DOIs	https://doi.org/10.1021/acsnano.3c05250
State	Published - Dec 12 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 CL microscopy was supported by the U.S. Department of Energy, Office of Science, National Quantum Information Science Research Centers, Quantum Science Center. The PL and CL spectroscopies were supported by the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy Office of Science User Facility. 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.

Keywords

2D materials
cathodoluminescence
exciton funneling
gallium selenide
single photon emission
strain engineering

Access to Document

10.1021/acsnano.3c05250

Cite this

@article{8f5eef943f5e4eb8a70eb846dd7616a6,

title = "Imaging Strain-Localized Single-Photon Emitters in Layered GaSe below the Diffraction Limit",

abstract = "Nanoscale strain control of exciton funneling is an increasingly critical tool for the scalable production of single photon emitters (SPEs) in two-dimensional materials. However, conventional far-field optical microscopies remain constrained in spatial resolution by the diffraction limit and thus can provide only a limited description of nanoscale strain localization of SPEs. Here, we quantify the effects of nanoscale heterogeneous strain on the energy and brightness of GaSe SPEs on nanopillars with correlative cathodoluminescence, photoluminescence, and atomic force microscopy, supported by density functional theory simulations. We report the strain-localized SPEs have a broad range of emission wavelengths from 620 to 900 nm. We reveal substantial strain-controlled SPE wavelength tunability over a ∼100 nm spectral range and 2 orders of magnitude enhancement in the SPE brightness at the pillar center due to Type-I exciton funneling. In addition, we show that radiative biexciton cascade processes contribute to observed CL photon superbunching. Also, the GaSe SPEs show excellent stability, where their properties remain unchanged after electron beam exposure. We anticipate that this comprehensive study on the nanoscale strain control of two-dimensional SPEs will provide key insights to guide the development of truly deterministic quantum photonics.",

keywords = "2D materials, cathodoluminescence, exciton funneling, gallium selenide, single photon emission, strain engineering",

author = "Weijun Luo and Lawrie, {Benjamin J.} and Puretzky, {Alexander A.} and Qishuo Tan and Hongze Gao and Lingerfelt, {David B.} and Gage Eichman and Edward Mcgee and Swan, {Anna K.} and Liangbo Liang and Xi Ling",

note = "Publisher Copyright: {\textcopyright} 2023 American Chemical Society.",

year = "2023",

month = dec,

day = "12",

doi = "10.1021/acsnano.3c05250",

language = "English",

volume = "17",

pages = "23455--23465",

journal = "ACS Nano",

issn = "1936-0851",

publisher = "American Chemical Society",

number = "23",

}

TY - JOUR

T1 - Imaging Strain-Localized Single-Photon Emitters in Layered GaSe below the Diffraction Limit

AU - Luo, Weijun

AU - Lawrie, Benjamin J.

AU - Puretzky, Alexander A.

AU - Tan, Qishuo

AU - Gao, Hongze

AU - Lingerfelt, David B.

AU - Eichman, Gage

AU - Mcgee, Edward

AU - Swan, Anna K.

AU - Liang, Liangbo

AU - Ling, Xi

PY - 2023/12/12

Y1 - 2023/12/12

N2 - Nanoscale strain control of exciton funneling is an increasingly critical tool for the scalable production of single photon emitters (SPEs) in two-dimensional materials. However, conventional far-field optical microscopies remain constrained in spatial resolution by the diffraction limit and thus can provide only a limited description of nanoscale strain localization of SPEs. Here, we quantify the effects of nanoscale heterogeneous strain on the energy and brightness of GaSe SPEs on nanopillars with correlative cathodoluminescence, photoluminescence, and atomic force microscopy, supported by density functional theory simulations. We report the strain-localized SPEs have a broad range of emission wavelengths from 620 to 900 nm. We reveal substantial strain-controlled SPE wavelength tunability over a ∼100 nm spectral range and 2 orders of magnitude enhancement in the SPE brightness at the pillar center due to Type-I exciton funneling. In addition, we show that radiative biexciton cascade processes contribute to observed CL photon superbunching. Also, the GaSe SPEs show excellent stability, where their properties remain unchanged after electron beam exposure. We anticipate that this comprehensive study on the nanoscale strain control of two-dimensional SPEs will provide key insights to guide the development of truly deterministic quantum photonics.

AB - Nanoscale strain control of exciton funneling is an increasingly critical tool for the scalable production of single photon emitters (SPEs) in two-dimensional materials. However, conventional far-field optical microscopies remain constrained in spatial resolution by the diffraction limit and thus can provide only a limited description of nanoscale strain localization of SPEs. Here, we quantify the effects of nanoscale heterogeneous strain on the energy and brightness of GaSe SPEs on nanopillars with correlative cathodoluminescence, photoluminescence, and atomic force microscopy, supported by density functional theory simulations. We report the strain-localized SPEs have a broad range of emission wavelengths from 620 to 900 nm. We reveal substantial strain-controlled SPE wavelength tunability over a ∼100 nm spectral range and 2 orders of magnitude enhancement in the SPE brightness at the pillar center due to Type-I exciton funneling. In addition, we show that radiative biexciton cascade processes contribute to observed CL photon superbunching. Also, the GaSe SPEs show excellent stability, where their properties remain unchanged after electron beam exposure. We anticipate that this comprehensive study on the nanoscale strain control of two-dimensional SPEs will provide key insights to guide the development of truly deterministic quantum photonics.

KW - 2D materials

KW - cathodoluminescence

KW - exciton funneling

KW - gallium selenide

KW - single photon emission

KW - strain engineering

UR - http://www.scopus.com/inward/record.url?scp=85180004343&partnerID=8YFLogxK

U2 - 10.1021/acsnano.3c05250

DO - 10.1021/acsnano.3c05250

M3 - Article

C2 - 38044592

AN - SCOPUS:85180004343

SN - 1936-0851

VL - 17

SP - 23455

EP - 23465

JO - ACS Nano

JF - ACS Nano

IS - 23

ER -

Imaging Strain-Localized Single-Photon Emitters in Layered GaSe below the Diffraction Limit

Abstract

Funding

Keywords

Access to Document

Other files and links

Fingerprint

Cite this