Mainz 2026 – scientific programme

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MO: Fachverband Molekülphysik

MO 30: Poster – Molecular Spectroscopy

MO 30.8: Poster

Thursday, March 5, 2026, 17:00–19:00, Philo 1. OG

Probing Electronic-Nuclear Coupling with MIR-XUV Spectroscopy — •Pankaj Seliya, Lina Hedewig, Carlo Kleine, Christian Ott, and Thomas Pfeifer — Max-Planck-Institut für Kernphysik, Saupfercheckweg 1, 69117 Heidelberg, Germany

The interplay between vibrational and electronic motions governs various molecular phenomena including energy dissipation, delocalization, and charge transfer [1]. Existing methods to study electronic-nuclear coupling, such as impulsive Raman [2] and two-dimensional vibrational-electronic (2DVE)/electronic-vibrational (2DEV) [3] spectroscopy provide selectivity only either along vibrational or electronic coordinates, but not both. Impulsive Raman with XUV/soft-X-ray probe provides electronic selectivity, but broadband near-IR/UV-Vis excitation drives multiple vibrational modes [2]. In contrast, 2DVE offer vibrational selectivity via resonant mid-IR(MIR) excitation, but visible probes lack electronic specificity. Here, we introduce an approach that accesses vibronic coupling with both vibrational and electronic selectivity, using resonant MIR pulses for mode-specific vibrational excitation and XUV pulses for element-specific probing of electronic dynamics. We test our setup with helium atoms, observing light-induced states [4] generated by exciting the 1sns /1snd states via one-photon XUV absorption together with absorption/emission of a one MIR photon. Experiments are currently being extended to molecules such as SF6 and N2O. References: [1] Struct. Dyn. 4, 061508 (2017) [2] J. Chem. Phys. 156, 114304 (2022) [3] J. Chem. Phys. 147, 094202 (2017) [4] Physical Review A 86, 063408 (2012)

Keywords: High-Harmonic Generation; Vibronic Coupling; Vibrational Spectroscopy