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Excited state nonadiabatic dynamics of bare and hydrated anionic gold clusters Au\(^−_3\)[H\(_2\)O]\(_n\) (n=0-2)
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- We present a joint theoretical and experimental study of excited state dynamics in pure and hydrated anionic gold clusters Au\(^-_3\)[H\(_2\)O]\(_n\) (n = 0-2). We employ mixed quantum-classical dynamics combined with femtosecond time-resolved photoelectron spectroscopy in order to investigate the influence of hydration on excited state lifetimes and photo-dissociation dynamics. A gradual decrease of the excited state lifetime with the number of adsorbed water molecules as well as gold cluster fragmentation quenching by two or more waterWe present a joint theoretical and experimental study of excited state dynamics in pure and hydrated anionic gold clusters Au\(^-_3\)[H\(_2\)O]\(_n\) (n = 0-2). We employ mixed quantum-classical dynamics combined with femtosecond time-resolved photoelectron spectroscopy in order to investigate the influence of hydration on excited state lifetimes and photo-dissociation dynamics. A gradual decrease of the excited state lifetime with the number of adsorbed water molecules as well as gold cluster fragmentation quenching by two or more water molecules are observed both in experiment and in simulations. Non-radiative relaxation and dissociation in excited states are found to be responsible for the excited state population depletion. Time constants of these two processes strongly depend on the number of water molecules leading to the possibility to modulate excited state dynamics and fragmentation of the anionic cluster by adsorption of water molecules.…
Autor(en): | Polina Lisinetskaya, Christian Braun, Sebastian Proch, Young Dok Kim, Gerd Ganteför, Roland MitrićORCiD |
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URN: | urn:nbn:de:bvb:20-opus-159176 |
Dokumentart: | Artikel / Aufsatz in einer Zeitschrift |
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): | Physical Chemistry Chemical Physics |
ISSN: | 1463-9076 |
Erscheinungsjahr: | 2016 |
Band / Jahrgang: | 18 |
Heft / Ausgabe: | 9 |
Seitenangabe: | 6411-6419 |
Originalveröffentlichung / Quelle: | Physical Chemistry Chemical Physics, 2016, 18, 6411-6419. DOI: 10.1039/C5CP04297F |
URL der Erstveröffentlichung: | https://doi.org/10.1039/C5CP04297F |
DOI: | https://doi.org/10.1039/c5cp04297f |
PubMed-ID: | https://pubmed.ncbi.nlm.nih.gov/26478260 |
Sonstige beteiligte Institutionen: | Fachbereich Physik, Universität Konstanz, D-78464 Konstanz, Germany |
Sonstige beteiligte Institutionen: | Department of Chemistry, Sungkyunkwan University, 440-746 Suwon, Republic of Korea |
Allgemeine fachliche Zuordnung (DDC-Klassifikation): | 5 Naturwissenschaften und Mathematik / 54 Chemie / 541 Physikalische Chemie |
Freie Schlagwort(e): | metal cluster; nonadiabatic dynamics; time-resolved photoelectron spectroscopy |
Datum der Freischaltung: | 19.03.2018 |
EU-Projektnummer / Contract (GA) number: | 646737 |
OpenAIRE: | OpenAIRE |
Anmerkungen: | Accepted version |
Lizenz (Deutsch): | Deutsches Urheberrecht |