Low-Temperature Electron–Phonon Interaction of Quantum Emitters in Hexagonal Boron Nitride

Grosso, G; Moon, H; Ciccarino, CJ; Flick, J; Mendelson, N; Mennel, L; Toth, M; Aharonovich, I; Narang, P; Englund, DR

Low-Temperature Electron–Phonon Interaction of Quantum Emitters in Hexagonal Boron Nitride

Grosso, G Moon, H Ciccarino, CJ Flick, J Mendelson, N Mennel, L Toth, M

Aharonovich, I

Narang, P Englund, DR

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Publisher:: American Chemical Society
Publication Type:: Journal Article
Citation:: ACS Photonics, 2020, 7, (6), pp. 1410-1417
Issue Date:: 2020-05-21

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Field	Value	Language
dc.contributor.author	Grosso, G
dc.contributor.author	Moon, H
dc.contributor.author	Ciccarino, CJ
dc.contributor.author	Flick, J
dc.contributor.author	Mendelson, N
dc.contributor.author	Mennel, L
dc.contributor.author	Toth, M https://orcid.org/0000-0003-1564-4899
dc.contributor.author	Aharonovich, I https://orcid.org/0000-0003-4304-3935
dc.contributor.author	Narang, P
dc.contributor.author	Englund, DR
dc.date.accessioned	2020-12-17T04:02:19Z
dc.date.available	2020-12-17T04:02:19Z
dc.date.issued	2020-05-21
dc.identifier.citation	ACS Photonics, 2020, 7, (6), pp. 1410-1417
dc.identifier.issn	2330-4022
dc.identifier.issn	2330-4022
dc.identifier.uri	http://hdl.handle.net/10453/144803
dc.description.abstract	© 2020 American Chemical Society. Single photon sources based on atomic defects in layered hexagonal boron nitride (hBN) have emerged as promising solid state quantum emitters with atom-like photophysical and quantum optoelectronic properties. Similar to other atom-like emitters, defect-phonon coupling in hBN governs the characteristic single-photon emission and provides an opportunity to investigate the atomic and electronic structure of emitters as well as the coupling of their spin- and charge-dependent electronic states to phonons. Here, we investigate these questions using photoluminescence excitation (PLE) experiments at T = 4 K on single-photon emitters in multilayer hBN grown by chemical vapor deposition. By scanning up to 250 meV from the zero phonon line (ZPL), we can precisely measure the emitter's coupling efficiency to different phonon modes. Our results show that excitation mediated by the absorption of one in-plane optical phonon increases the emitter absorption probability 10-fold compared to that mediated by acoustic or out-of-plane optical phonons. We perform complementary theoretical predictions by first-principles density-functional theory of four defect candidates for which we calculate prevalent charge states and their spin-dependent coupling to bulk and local phonon modes. We discuss possible hypotheses to overcome the disparity between experimental results and theoretical predictions. Our work illuminates the phonon-coupled dynamics in hBN quantum emitters at cryogenic temperature, with implications more generally for mesoscopic quantum emitter systems in 2D materials, and represents possible applications in solid-state quantum technologies.
dc.language	en
dc.publisher	American Chemical Society
dc.relation.ispartof	ACS Photonics
dc.relation.isbasedon	http://dx.doi.org/10.1021/acsphotonics.9b01789
dc.rights	info:eu-repo/semantics/restrictedAccess
dc.subject	0205 Optical Physics, 0206 Quantum Physics, 0906 Electrical and Electronic Engineering
dc.title	Low-Temperature Electron–Phonon Interaction of Quantum Emitters in Hexagonal Boron Nitride
dc.type	Journal Article
utslib.citation.volume	7
utslib.for	0205 Optical Physics
utslib.for	0206 Quantum Physics
utslib.for	0906 Electrical and Electronic Engineering
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
pubs.organisational-group	/University of Technology Sydney
pubs.organisational-group	/University of Technology Sydney/Strength - MTEE - Research Centre Materials and Technology for Energy Efficiency
utslib.copyright.status	closed_access	*
pubs.consider-herdc	false
dc.date.updated	2020-12-17T04:02:09Z
pubs.issue	6
pubs.publication-status	Published online
pubs.volume	7
utslib.citation.issue	6

Abstract:

© 2020 American Chemical Society. Single photon sources based on atomic defects in layered hexagonal boron nitride (hBN) have emerged as promising solid state quantum emitters with atom-like photophysical and quantum optoelectronic properties. Similar to other atom-like emitters, defect-phonon coupling in hBN governs the characteristic single-photon emission and provides an opportunity to investigate the atomic and electronic structure of emitters as well as the coupling of their spin- and charge-dependent electronic states to phonons. Here, we investigate these questions using photoluminescence excitation (PLE) experiments at T = 4 K on single-photon emitters in multilayer hBN grown by chemical vapor deposition. By scanning up to 250 meV from the zero phonon line (ZPL), we can precisely measure the emitter's coupling efficiency to different phonon modes. Our results show that excitation mediated by the absorption of one in-plane optical phonon increases the emitter absorption probability 10-fold compared to that mediated by acoustic or out-of-plane optical phonons. We perform complementary theoretical predictions by first-principles density-functional theory of four defect candidates for which we calculate prevalent charge states and their spin-dependent coupling to bulk and local phonon modes. We discuss possible hypotheses to overcome the disparity between experimental results and theoretical predictions. Our work illuminates the phonon-coupled dynamics in hBN quantum emitters at cryogenic temperature, with implications more generally for mesoscopic quantum emitter systems in 2D materials, and represents possible applications in solid-state quantum technologies.

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