Selective Anti-Stokes Excitation of a Single Defect Center in Hexagonal Boron Nitride

Okashiro, Y; Takashima, H; Shimazaki, K; Suzuki, K; Mukai, Y; Aharonovich, I; Takeuchi, S

Selective Anti-Stokes Excitation of a Single Defect Center in Hexagonal Boron Nitride

Okashiro, Y Takashima, H Shimazaki, K Suzuki, K Mukai, Y Aharonovich, I

Takeuchi, S

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Publisher:: AMER CHEMICAL SOC
Publication Type:: Journal Article
Citation:: ACS Photonics, 2024, 11, (9), pp. 3602-3609
Issue Date:: 2024-09-18

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Field	Value	Language
dc.contributor.author	Okashiro, Y
dc.contributor.author	Takashima, H
dc.contributor.author	Shimazaki, K
dc.contributor.author	Suzuki, K
dc.contributor.author	Mukai, Y
dc.contributor.author	Aharonovich, I https://orcid.org/0000-0003-4304-3935
dc.contributor.author	Takeuchi, S
dc.date.accessioned	2025-01-13T03:43:57Z
dc.date.available	2025-01-13T03:43:57Z
dc.date.issued	2024-09-18
dc.identifier.citation	ACS Photonics, 2024, 11, (9), pp. 3602-3609
dc.identifier.issn	2330-4022
dc.identifier.issn	2330-4022
dc.identifier.uri	http://hdl.handle.net/10453/183362
dc.description.abstract	Hexagonal boron nitride (hBN) with defect centers is attracting attention as a promising candidate for single-photon emitters because its emission spectrum shows sharp emission peaks and it exhibits ultrabright single-photon emission at room temperature. However, when hBN containing multiple defect centers with various transition frequencies is excited using a pump laser with a wavelength shorter than the emission wavelength of the target defect center, problems such as a broad emission spectrum and nonsingle photon emission often arise. In this paper, we present a method for selectively exciting a single defect center in hBN nanoflakes by anti-Stokes excitation, where the wavelength of the excitation laser is longer than the emission wavelength of the target defect center. By exciting an hBN nanoflake with multiple defect centers using a 637 nm laser, as opposed to the normal excitation using a 532 nm laser, we observed a sharp emission peak and an antibunching dip (g2(0) = 0.08 ± 0.05) in the second-order correlation function, indicating strong evidence of a single defect center. In addition, we explored the temperature dependence of the emission spectrum from the defect centers in a hBN nanoflake to clarify the mechanism of the anti-Stokes excitation. As a result, we confirmed that single-phonon-mediated anti-Stokes excitation plays a substantial role in suppressing shorter-wavelength emissions and improving g2(0). Because this method uses a long-wavelength laser for excitation, it is speculated to substantially reduce the background photons generated not only inside the hBN nanoflakes but also in the optical fiber guiding the pump light, which is often a severe problem.
dc.language	English
dc.publisher	AMER CHEMICAL SOC
dc.relation	http://purl.org/au-research/grants/arc/CE200100010
dc.relation	United States Department of the NavyN629092212028
dc.relation	http://purl.org/au-research/grants/arc/FT220100053
dc.relation.ispartof	ACS Photonics
dc.relation.isbasedon	10.1021/acsphotonics.4c00594
dc.rights	info:eu-repo/semantics/restrictedAccess
dc.subject	0205 Optical Physics, 0206 Quantum Physics, 0906 Electrical and Electronic Engineering
dc.subject.classification	5102 Atomic, molecular and optical physics
dc.title	Selective Anti-Stokes Excitation of a Single Defect Center in Hexagonal Boron Nitride
dc.type	Journal Article
utslib.citation.volume	11
utslib.for	0205 Optical Physics
utslib.for	0206 Quantum Physics
utslib.for	0906 Electrical and Electronic Engineering
pubs.organisational-group	University of Technology Sydney
pubs.organisational-group	University of Technology Sydney/Faculty of Science
pubs.organisational-group	University of Technology Sydney/Faculty of Science/School of Mathematical and Physical Sciences
utslib.copyright.status	in_progress	*
dc.date.updated	2025-01-13T03:43:56Z
pubs.issue	9
pubs.publication-status	Published
pubs.volume	11
utslib.citation.issue	9

Abstract:

Hexagonal boron nitride (hBN) with defect centers is attracting attention as a promising candidate for single-photon emitters because its emission spectrum shows sharp emission peaks and it exhibits ultrabright single-photon emission at room temperature. However, when hBN containing multiple defect centers with various transition frequencies is excited using a pump laser with a wavelength shorter than the emission wavelength of the target defect center, problems such as a broad emission spectrum and nonsingle photon emission often arise. In this paper, we present a method for selectively exciting a single defect center in hBN nanoflakes by anti-Stokes excitation, where the wavelength of the excitation laser is longer than the emission wavelength of the target defect center. By exciting an hBN nanoflake with multiple defect centers using a 637 nm laser, as opposed to the normal excitation using a 532 nm laser, we observed a sharp emission peak and an antibunching dip (g2(0) = 0.08 ± 0.05) in the second-order correlation function, indicating strong evidence of a single defect center. In addition, we explored the temperature dependence of the emission spectrum from the defect centers in a hBN nanoflake to clarify the mechanism of the anti-Stokes excitation. As a result, we confirmed that single-phonon-mediated anti-Stokes excitation plays a substantial role in suppressing shorter-wavelength emissions and improving g2(0). Because this method uses a long-wavelength laser for excitation, it is speculated to substantially reduce the background photons generated not only inside the hBN nanoflakes but also in the optical fiber guiding the pump light, which is often a severe problem.

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http://hdl.handle.net/10453/183362