Hidden Spin-Valley-Locking Extends Room Temperature Spin Lifetime in 2D Perovskite Semiconductors

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Abstract Room-temperature control of spin, coupled with charge and light, remains a long-standing challenge for next-generation spin-optoelectronic applications. Although inversion symmetry breaking offers one path for spin control in semiconductors, strong spin dephasing at higher temperatures remains a persistent challenge. While hidden spin polarization (HSP) without global symmetry breaking provides another promising material design strategy, robust spin stabilization from HSP is yet to be experimentally realized. Here, we demonstrate that 2D hybrid organic-inorganic perovskites can provide spin stabilization at room temperature via hidden spin valley locking. We utilized functional nonprimary ammonium cations (NPACs) that induce giant spin splitting in 2D layers with varying spin-orbit coupling (employing Sn vs Pb) and enhanced dielectric screening, thereby restricting spin relaxation processes. Time-resolved experiments demonstrate optically generated spin-polarized carriers that persist for over four nanoseconds at room temperature without requiring an external magnetic field. Our design paradigm unlocks inversion-symmetric semiconductors with ultralong spin lifetimes, broadening the materials options for light-driven spin control.
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Hidden Spin-Valley-Locking Extends Room Temperature Spin Lifetime in 2D Perovskite Semiconductors | 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 Hidden Spin-Valley-Locking Extends Room Temperature Spin Lifetime in 2D Perovskite Semiconductors David Mitzi, Volker Blum, Matthew Beard, Yifan Dong, Rayan Chakraborty, and 4 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7530828/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 Room-temperature control of spin, coupled with charge and light, remains a long-standing challenge for next-generation spin-optoelectronic applications. Although inversion symmetry breaking offers one path for spin control in semiconductors, strong spin dephasing at higher temperatures remains a persistent challenge. While hidden spin polarization (HSP) without global symmetry breaking provides another promising material design strategy, robust spin stabilization from HSP is yet to be experimentally realized. Here, we demonstrate that 2D hybrid organic-inorganic perovskites can provide spin stabilization at room temperature via hidden spin valley locking. We utilized functional nonprimary ammonium cations (NPACs) that induce giant spin splitting in 2D layers with varying spin-orbit coupling (employing Sn vs Pb) and enhanced dielectric screening, thereby restricting spin relaxation processes. Time-resolved experiments demonstrate optically generated spin-polarized carriers that persist for over four nanoseconds at room temperature without requiring an external magnetic field. Our design paradigm unlocks inversion-symmetric semiconductors with ultralong spin lifetimes, broadening the materials options for light-driven spin control. Physical sciences/Materials science/Condensed-matter physics/Spintronics Physical sciences/Materials science/Condensed-matter physics/Semiconductors/Two-dimensional materials Full Text Additional Declarations There is NO Competing Interest. Supplementary Files AzXspinlifetimeSIrevised2clean.pdf Supplementary material file 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. 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