Unraveling the dynamics of multiple excited states in a single-molecule transistor

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Abstract Characterizing charge transport through single molecules provides a fundamental route to explore correlated quantum states, forming the basis for nanodevices in which quantum effects govern operation. During the non-equilibrium electron transfer, a rich manifold of excited states emerges, whose dynamics encode many-body interactions at the single-molecule level. Disentangling these dynamics is crucial for understanding such interactions, however, has remained elusive due to synchronously experimental challenge of the time and energy resolution. Here, we resolved the dynamics of multiple excited states during non-equilibrium charge transport through a single-molecule radical junction using a nanosecond differential conductance spectroscopy. The participation of singlet and triplet states is revealed in both time and energy domains, and a continuous energy relaxation of ~440 meV occurring within ~150 ns is observed, mediated by doublet states. This provides a direct window into transient intermediates that fundamentally reshape our understanding of charge transport through radicals at the single-molecule level, and establish ultrafast manipulation strategies for quantum devices.
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Unraveling the dynamics of multiple excited states in a single-molecule transistor | 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 Unraveling the dynamics of multiple excited states in a single-molecule transistor Wenjing Hong, Hao Zhang, Lijue Chen, Ziheng Yuan, Jingyu Yang, and 12 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7395268/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 Characterizing charge transport through single molecules provides a fundamental route to explore correlated quantum states, forming the basis for nanodevices in which quantum effects govern operation. During the non-equilibrium electron transfer, a rich manifold of excited states emerges, whose dynamics encode many-body interactions at the single-molecule level. Disentangling these dynamics is crucial for understanding such interactions, however, has remained elusive due to synchronously experimental challenge of the time and energy resolution. Here, we resolved the dynamics of multiple excited states during non-equilibrium charge transport through a single-molecule radical junction using a nanosecond differential conductance spectroscopy. The participation of singlet and triplet states is revealed in both time and energy domains, and a continuous energy relaxation of ~440 meV occurring within ~150 ns is observed, mediated by doublet states. This provides a direct window into transient intermediates that fundamentally reshape our understanding of charge transport through radicals at the single-molecule level, and establish ultrafast manipulation strategies for quantum devices. Physical sciences/Nanoscience and technology/Nanoscale devices/Molecular electronics Physical sciences/Chemistry/Theoretical chemistry/Molecular dynamics Full Text Additional Declarations There is NO Competing Interest. Supplementary Files NatNanoEPPSI.docx Supplementary materials 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. 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