Surface crossing and energy flow in many-dimensional quantum systems

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dc.citation.articleNumbere2221690120en_US
dc.citation.issueNumber9en_US
dc.citation.journalTitleProceedings of the National Academy of Sciencesen_US
dc.citation.volumeNumber120en_US
dc.contributor.authorZhang, Chenghaoen_US
dc.contributor.authorGruebele, Martinen_US
dc.contributor.authorLogan, David E.en_US
dc.contributor.authorWolynes, Peter G.en_US
dc.contributor.orgCenter for Theoretical Biological Physicsen_US
dc.date.accessioned2023-03-10T19:04:17Zen_US
dc.date.available2023-03-10T19:04:17Zen_US
dc.date.issued2023en_US
dc.description.abstractEnergy flow in molecules, like the dynamics of other many-dimensional finite systems, involves quantum transport across a dense network of near-resonant states. For molecules in their electronic ground state, the network is ordinarily provided by anharmonic vibrational Fermi resonances. Surface crossing between different electronic states provides another route to chaotic motion and energy redistribution. We show that nonadiabatic coupling between electronic energy surfaces facilitates vibrational energy flow and, conversely, anharmonic vibrational couplings facilitate nonadiabatic electronic state mixing. A generalization of the Logan–Wolynes theory of quantum energy flow in many-dimensional Fermi resonance systems to the two-surface case gives a phase diagram describing the boundary between localized quantum dynamics and global energy flow. We explore these predictions and test them using a model inspired by the problem of electronic excitation energy transfer in the photosynthetic reaction center. Using an explicit numerical solution of the time-dependent Schrödinger equation for this ten-dimensional model, we find quite good agreement with the expectations from the approximate analytical theory.en_US
dc.identifier.citationZhang, Chenghao, Gruebele, Martin, Logan, David E., et al.. "Surface crossing and energy flow in many-dimensional quantum systems." <i>Proceedings of the National Academy of Sciences,</i> 120, no. 9 (2023) PNAS: https://doi.org/10.1073/pnas.2221690120.en_US
dc.identifier.digitalpnas-2221690120en_US
dc.identifier.doihttps://doi.org/10.1073/pnas.2221690120en_US
dc.identifier.urihttps://hdl.handle.net/1911/114508en_US
dc.language.isoengen_US
dc.publisherPNASen_US
dc.rightsThis article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND).en_US
dc.rights.urihttps://creativecommons.org/licenses/by-nc-nd/4.0/en_US
dc.titleSurface crossing and energy flow in many-dimensional quantum systemsen_US
dc.typeJournal articleen_US
dc.type.dcmiTexten_US
dc.type.publicationpublisher versionen_US
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