Bonn 2025 – wissenschaftliches Programm

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MO: Fachverband Molekülphysik

MO 6: Molecular Spectroscopy of Liquid Jets II

MO 6.2: Vortrag

Dienstag, 11. März 2025, 11:15–11:30, HS XV

Electronic dynamics created at conical intersections and its dephasing in aqueous solution — •Yi-Ping Chang¹, Tadas Balciunas^1,2, Zhong Yin², Marin Sapunar³, Bruno Tenorio⁴, Alexander Paul⁵, Shota Tsuru⁶, Henrik Koch⁵, Jean-Pierre Wolf¹, Sonia Coriani⁴, and Hans Jakob Wörner² — ¹Universite de Geneve, Switzerland — ²ETH Zürich, Switzerland — ³Ruder Boskovic Institute, Croatia — ⁴DTU, Denmark — ⁵NTNU, Norway — ⁶Ruhr University Bochum, Germany

Understanding the electronic dynamics of molecular systems is important for many fields in photophysics and photochemistry. This is especially challenging in the vicinity of a conical intersection, where the Born-Oppenheimer approximation breaksdown. In this work [1], we present two experimental breakthroughs: (1) the observation of electronic and vibrational dynamics corresponding to a circular rearrangement of the electronic structure created by conical intersection dynamics and (2) the sub-40 fs dephasing induced by aqueous solvation. Using a state-of-the-art table-top HHG source covering the entire water window, we performed time-resolved X-ray absorption spectroscopy (XAS) of single-UV-photon-excited liquid and gaseous pyrazine samples. At the carbon and nitrogen K-edges, we observed different non-adiabatic dynamics between gas and liquid phases, showing large-amplitude rearrangement of the electronic structure caused by the conical intersection and dephasing of electronic dynamics due to solvation. [1]Y.-P. Chang*, T. Balciunas*, Z. Yin*, M. Sapunar*, B.N.C. Tenorio*, A. Paul* et al. Nat. Phys. (2024).

Keywords: X-ray absorption spectroscopy; Femtosecond; Liquid; Photoexcitation; Gas