Ultrafast phonon-mediated dephasing of color centers in hexagonal boron nitride probed by electron beams

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Abstract Defect centers in hexagonal boron nitride (hBN) have been extensively studied as room-temperature single-photon sources. The electronic structure of these defects exhibits strong coupling to phonons, as evidenced by the observation of phonon sidebands in both photoluminescence and cathodoluminescence spectra. However, the dynamics of the electron-phonon coupling as well as phonon-mediated dephasing of the color centers in hBN remain unexplored. Here, we apply a novel time-resolved CL spectroscopy technique (Nature Physics 19, 869–876 (2023)) to explore the population decay to phonon states and the dephasing time T2 with sub-femtosecond time resolution. We demonstrate an ultrafast dephasing time of only 200 fs and a radiative decay of about 585 fs at room temperature, in contrast with all-optical time-resolved photoluminescence techniques that report a decay of a few nanoseconds. This behavior is attributed to efficient electron-beam excitation of coherent phonon-polaritons in hBN, resulting in faster dephasing of electronic transitions. Our results demonstrate the capability of our sequential cathodoluminescence spectroscopy technique to probe the ultrafast dephasing time of single emitters in quantum materials with sub-femtosecond time resolution, heralding access to quantum-path interferences in single emitters coupled to their complex environment.
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Ultrafast phonon-mediated dephasing of color centers in hexagonal boron nitride probed by electron beams | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Ultrafast phonon-mediated dephasing of color centers in hexagonal boron nitride probed by electron beams Nahid Talebi, Masoud Taleb, Paul Bittorf, Maximilian Black, Mario Hentschel, and 5 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-3857268/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 08 Mar, 2025 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Abstract Defect centers in hexagonal boron nitride (hBN) have been extensively studied as room-temperature single-photon sources. The electronic structure of these defects exhibits strong coupling to phonons, as evidenced by the observation of phonon sidebands in both photoluminescence and cathodoluminescence spectra. However, the dynamics of the electron-phonon coupling as well as phonon-mediated dephasing of the color centers in hBN remain unexplored. Here, we apply a novel time-resolved CL spectroscopy technique ( Nature Physics 19 , 869–876 (2023)) to explore the population decay to phonon states and the dephasing time T 2 with sub-femtosecond time resolution. We demonstrate an ultrafast dephasing time of only 200 fs and a radiative decay of about 585 fs at room temperature, in contrast with all-optical time-resolved photoluminescence techniques that report a decay of a few nanoseconds. This behavior is attributed to efficient electron-beam excitation of coherent phonon-polaritons in hBN, resulting in faster dephasing of electronic transitions. Our results demonstrate the capability of our sequential cathodoluminescence spectroscopy technique to probe the ultrafast dephasing time of single emitters in quantum materials with sub-femtosecond time resolution, heralding access to quantum-path interferences in single emitters coupled to their complex environment. Physical sciences/Optics and photonics/Optical materials and structures/Nanoparticles Physical sciences/Optics and photonics/Optical physics/Polaritons Full Text Additional Declarations There is NO Competing Interest. Supplementary Files hBNEDPHSTalebiSupplementary.pdf Cite Share Download PDF Status: Published Journal Publication published 08 Mar, 2025 Read the published version in Nature Communications → Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. 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