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

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 characteris...

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Main Authors: Moon, Hyowon, Englund, Dirk R.
Other Authors: Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science
Format: Article
Language:English
Published: American Chemical Society (ACS) 2021
Online Access:https://hdl.handle.net/1721.1/129609
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author Moon, Hyowon
Englund, Dirk R.
author2 Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science
author_facet Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science
Moon, Hyowon
Englund, Dirk R.
author_sort Moon, Hyowon
collection MIT
description 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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spelling mit-1721.1/1296092022-10-02T06:11:11Z Low-Temperature Electron–Phonon Interaction of Quantum Emitters in Hexagonal Boron Nitride Moon, Hyowon Englund, Dirk R. Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science 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. United States. Army Research Office. Multidisciplinary University Research Initiative (Grant W911NF-18-1-0431) 2021-02-01T18:54:58Z 2021-02-01T18:54:58Z 2020-05 2019-10 2020-12-14T18:49:56Z Article http://purl.org/eprint/type/JournalArticle 2330-4022 https://hdl.handle.net/1721.1/129609 Grosso​, Gabriele et al. “Low-Temperature Electron–Phonon Interaction of Quantum Emitters in Hexagonal Boron Nitride.” ACS Photonics, 7, 6 (May 2020): 1410–1417 © 2020 The Author(s) en 10.1021/ACSPHOTONICS.9B01789 ACS Photonics Creative Commons Attribution-Noncommercial-Share Alike http://creativecommons.org/licenses/by-nc-sa/4.0/ application/pdf American Chemical Society (ACS) arXiv
spellingShingle Moon, Hyowon
Englund, Dirk R.
Low-Temperature Electron–Phonon Interaction of Quantum Emitters in Hexagonal Boron Nitride
title Low-Temperature Electron–Phonon Interaction of Quantum Emitters in Hexagonal Boron Nitride
title_full Low-Temperature Electron–Phonon Interaction of Quantum Emitters in Hexagonal Boron Nitride
title_fullStr Low-Temperature Electron–Phonon Interaction of Quantum Emitters in Hexagonal Boron Nitride
title_full_unstemmed Low-Temperature Electron–Phonon Interaction of Quantum Emitters in Hexagonal Boron Nitride
title_short Low-Temperature Electron–Phonon Interaction of Quantum Emitters in Hexagonal Boron Nitride
title_sort low temperature electron phonon interaction of quantum emitters in hexagonal boron nitride
url https://hdl.handle.net/1721.1/129609
work_keys_str_mv AT moonhyowon lowtemperatureelectronphononinteractionofquantumemittersinhexagonalboronnitride
AT englunddirkr lowtemperatureelectronphononinteractionofquantumemittersinhexagonalboronnitride