Ultrafast Photodynamics of Glucose
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- We have investigated the photodynamics of \(\beta\)-D-glucose employing our field-induced surface hopping method (FISH), which allows us to simulate the coupled electron-nuclear dynamics, including explicitly nonadiabatic effects and light-induced excitation. Our results reveal that from the initially populated S\(_{1}\) and S\(_{2}\) states, glucose returns nonradiatively to the ground state within about 200 fs. This takes place mainly via conical intersections (CIs) whose geometries in most cases involve the elongation of a single O-H bond,We have investigated the photodynamics of \(\beta\)-D-glucose employing our field-induced surface hopping method (FISH), which allows us to simulate the coupled electron-nuclear dynamics, including explicitly nonadiabatic effects and light-induced excitation. Our results reveal that from the initially populated S\(_{1}\) and S\(_{2}\) states, glucose returns nonradiatively to the ground state within about 200 fs. This takes place mainly via conical intersections (CIs) whose geometries in most cases involve the elongation of a single O-H bond, while in some instances ring-opening due to dissociation of a C-O bond is observed. Experimentally, excitation to a distinct excited electronic state is improbable due to the presence of a dense manifold of states bearing similar oscillator strengths. Our FISH simulations explicitly including a UV laser pulse of 6.43 eV photon energy reveals that after initial excitation the population is almost equally spread over several close-lying electronic states. This is followed by a fast nonradiative decay on the time scale of 100-200 fs, with the final return to the ground state proceeding via the S\(_{1}\) state through the same types of CIs as observed in the field-free simulations.…
Autor(en): | Jens PetersenORCiD, Joachim O. Lindner, Roland MitricORCiD |
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URN: | urn:nbn:de:bvb:20-opus-159155 |
Dokumentart: | Preprint (Vorabdruck) |
Institute der Universität: | Fakultät für Chemie und Pharmazie / Institut für Physikalische und Theoretische Chemie |
Sprache der Veröffentlichung: | Englisch |
Titel des übergeordneten Werkes / der Zeitschrift (Englisch): | Journal of Physical Chemistry B |
Erscheinungsjahr: | 2018 |
Originalveröffentlichung / Quelle: | Journal of Physical Chemistry B 122, 1, 19-27. DOI:10.1021/acs.jpcb.7b08602 |
DOI: | https://doi.org/10.1021/acs.jpcb.7b08602 |
Allgemeine fachliche Zuordnung (DDC-Klassifikation): | 5 Naturwissenschaften und Mathematik / 54 Chemie / 541 Physikalische Chemie |
Freie Schlagwort(e): | carbohydrates; conical intersections; nonadiabatic dynamics; photodynamics |
Fachklassifikation Physik (PACS): | 30.00.00 ATOMIC AND MOLECULAR PHYSICS |
Datum der Freischaltung: | 19.03.2018 |
EU-Projektnummer / Contract (GA) number: | 646737 |
OpenAIRE: | OpenAIRE |
Anmerkungen: | This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Journal of Physical Chemistry, copyright © American Chemical Society after peer review. To access the final edited and published work see doi:10.1021/acs.jpcb.7b08602 |
Lizenz (Deutsch): | Deutsches Urheberrecht |