Ultrafast Laser Induces Macroscopic Symmetry-Breaking of Diamond Color Centers

Ultrafast Laser Induces Macroscopic Symmetry-Breaking of Diamond Color Centers | 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 Laser Induces Macroscopic Symmetry-Breaking of Diamond Color Centers Chao Lian, Yang Gao, Qi-Zheng Ji, Chao-Bo Liu, Qi Xiao This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6809894/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted You are reading this latest preprint version Abstract We employ real-time time-dependent density functional theory (RT-TDDFT) to investigate the coupled electron-phonon-spin dynamics in negatively charged nitrogen-vacancy centers (NV$^{-}$). Laser excitation promotes minority-spin electrons within 100 fs, establishing a $C_{3v}$-symmetry breaking (3RSB) charge ordering. Subsequently, ionic motion on the potential energy surface of the excited electrons generates both symmetric oscillations of carbon-nitrogen bonds and dynamic Jahn-Teller distortions (DJT) with 3RSB. These distortions subsequently induce nonlocal coherent phonons in the diamond lattice, which propagate with 3RSB at the sound velocity ($\sim$2 \AA/fs). Meanwhile, the NV$^{-}$ spin state remains preserved during photoexcitation but undergoes rapid reorientation within 100~fs via enhanced spin-orbit-phonon coupling. Our RT-TDDFT simulations provide direct time-resolved visualization of these processes, offering novel insights into the microscopic interplay of electrons, phonons, and spins in NV$^{-}$ centers. Physical sciences/Physics/Condensed-matter physics/Electronic properties and materials Physical sciences/Physics/Optical physics/Ultrafast photonics Full Text Additional Declarations There is NO Competing Interest. Cite Share Download PDF Status: Under Review 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. Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-6809894","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":465904934,"identity":"e719936e-7fe7-47b9-989a-fc64325b29d8","order_by":0,"name":"Chao Lian","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA1klEQVRIiWNgGAWjYDACCSB+YMDAwM/MwEaClgSgFslm0rQAscEBYrXwz25++CChwC7P+Djvscc8DHbyDOxnD+C35M4xY4MEg+Ris8N86cY8DMmGDTx5CXi1GEgkmEkkGDAnbjvMYybNw8CcwCDBY0BAS/o3oJb6xM3NYC31xGjJAdlyOHEDM1jLYcJaJG7kFAP9cjxxxmG+NMk5BscN23hy8Gvhn5G+8cGHP9WJ/f1nj0m8qaiW52c/g18LEuBhYAI5idgIhWhh/EGC8lEwCkbBKBg5AAD4wTkfWUuivgAAAABJRU5ErkJggg==","orcid":"https://orcid.org/0000-0002-2583-9334","institution":"Inst. 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Laser excitation promotes minority-spin electrons within 100~fs, establishing a $C_{3v}$-symmetry breaking (3RSB) charge ordering. Subsequently, ionic motion on the potential energy surface of the excited electrons generates both symmetric oscillations of carbon-nitrogen bonds and dynamic Jahn-Teller distortions (DJT) with 3RSB. These distortions subsequently induce nonlocal coherent phonons in the diamond lattice, which propagate with 3RSB at the sound velocity ($\\sim$2~\\AA/fs). Meanwhile, the NV$^{-}$ spin state remains preserved during photoexcitation but undergoes rapid reorientation within 100~fs via enhanced spin-orbit-phonon coupling. 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