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MO: Fachverband Molekülphysik
MO 5: Ultrafast Dynamics I
MO 5.3: Vortrag
Dienstag, 11. März 2025, 11:30–11:45, HS XVI
Ultrafast Light-Induced Dynamics of Competing Reaction Pathways in Molecular Rings — •Vesna Erić1, Francesco Montorsi1,2, Simona Djumayska1, and Daniel Keefer1 — 1Max Planck Institute for Polymer Research, Mainz, Germany — 2University of Bologna, Bologna, Italy
Conical intersections mediate ultrafast light-induced processes in molecular systems. Due to the strong coupling of electronic and nuclear degrees of freedom, conical intersections open channels for fast energy transfer between excited states. Recent theoretical studies reveal the potential of stimulated X-ray Raman spectroscopy to provide distinct spectral signals of the passage through conical intersections, which previously remained elusive. Here, we extend this concept towards spectrally distinguishing competing conical intersection-mediated pathways. We employ computational modelling to investigate the photochemistry of 2,5-dichlorofuran molecules exhibiting competing reaction pathways, ring puckering and opening, as typically observed in molecular ring structures. Our simulation protocol includes multireference (CASPT2) electronic structure calculations, quantum dynamics, and evaluation of stimulated X-ray Raman signals. Finally, we discuss the possibility of the spectral separation between the competing conical intersections by tuning the X-ray probe pulse to the pre-edge of the Carbon, Nitrogen and Oxygen transitions.
Keywords: ultrafast molecular dynamics; molecular spectroscopy; X-ray spectroscopy; conical intersection; computational modelling