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Following the Nonadiabatic Ultrafast Dynamics of Uracil via Simulated X-ray Absorption Spectra
Stockholm University, Faculty of Science, Department of Physics. LMU Munich, Germany.ORCID iD: 0000-0003-4538-811X
Number of Authors: 42023 (English)In: Journal of Physical Chemistry A, ISSN 1089-5639, E-ISSN 1520-5215, Vol. 127, no 46, p. 9787-9796Article in journal (Refereed) Published
Abstract [en]

The nucleobase uracil exhibits high photostability due to ultrafast relaxation processes mediated by conical intersections (CoIns), where the interplay between nuclear and electron dynamics becomes crucial. In our previous study, we observed seemingly long-lived traces of electronic coherence for the relaxation process through the S-2/S-1 CoIn by applying our ansatz for coupled nuclear and electron dynamics in molecules (NEMol). In this work, we theoretically investigate how time-dependent transient X-ray absorption spectroscopy can be used to observe this ultrafast dynamics. Therefore, we calculated X-ray absorption spectra (XAS) for the oxygen K-edge, using a multireference protocol in combination with NEMol dynamics. Thus, we have access to both the transient XAS based on the nuclear wavepacket dynamics and the modulation of the signals caused by the electronic coherence induced by the excitation process and the presence of a CoIn seam. In both cases, we were able to qualitatively predict its influence on the resulting XAS.

Place, publisher, year, edition, pages
2023. Vol. 127, no 46, p. 9787-9796
National Category
Atom and Molecular Physics and Optics
Identifiers
URN: urn:nbn:se:su:diva-226580DOI: 10.1021/acs.jpca.3c06509ISI: 001142981000001PubMedID: 37955656Scopus ID: 2-s2.0-85178122553OAI: oai:DiVA.org:su-226580DiVA, id: diva2:1837623
Available from: 2024-02-14 Created: 2024-02-14 Last updated: 2024-02-14Bibliographically approved

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Schnappinger, Thomas

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