Revealing Ultrafast Population Transfer between Nearly Degenerate Electronic States.


Journal

The journal of physical chemistry letters
ISSN: 1948-7185
Titre abrégé: J Phys Chem Lett
Pays: United States
ID NLM: 101526034

Informations de publication

Date de publication:
20 Feb 2020
Historique:
pubmed: 11 1 2020
medline: 11 1 2020
entrez: 11 1 2020
Statut: ppublish

Résumé

The response of a molecule to photoexcitation is governed by the coupling of its electronic states. However, if the energetic spacing between the electronically excited states at the Franck-Condon window becomes sufficiently small, it is infeasible to selectively excite and monitor individual states with conventional time-resolved spectroscopy, preventing insight into the energy transfer and relaxation dynamics of the molecule. Here, we demonstrate how the combination of time-resolved spectroscopy and extensive surface hopping dynamics simulations with a global fit approach on individually excited ensembles overcomes this limitation and resolves the dynamics in the n3p Rydberg states in acetone. Photoelectron transients of the three closely spaced states n3p

Identifiants

pubmed: 31918552
doi: 10.1021/acs.jpclett.9b03462
pmc: PMC7052817
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

1443-1449

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Auteurs

Pascal Heim (P)

Institute of Experimental Physics , Graz University of Technology , Petersgasse 16 , A-8010 Graz , Austria.

Sebastian Mai (S)

Institute of Theoretical Chemistry, Faculty of Chemistry , University of Vienna , Währinger Str. 17 , A-1090 Vienna , Austria.

Bernhard Thaler (B)

Institute of Experimental Physics , Graz University of Technology , Petersgasse 16 , A-8010 Graz , Austria.

Stefan Cesnik (S)

Institute of Experimental Physics , Graz University of Technology , Petersgasse 16 , A-8010 Graz , Austria.

Davide Avagliano (D)

Institute of Theoretical Chemistry, Faculty of Chemistry , University of Vienna , Währinger Str. 17 , A-1090 Vienna , Austria.

Dimitra Bella-Velidou (D)

Institute of Theoretical Chemistry, Faculty of Chemistry , University of Vienna , Währinger Str. 17 , A-1090 Vienna , Austria.

Wolfgang E Ernst (WE)

Institute of Experimental Physics , Graz University of Technology , Petersgasse 16 , A-8010 Graz , Austria.

Leticia González (L)

Institute of Theoretical Chemistry, Faculty of Chemistry , University of Vienna , Währinger Str. 17 , A-1090 Vienna , Austria.

Markus Koch (M)

Institute of Experimental Physics , Graz University of Technology , Petersgasse 16 , A-8010 Graz , Austria.

Classifications MeSH