Bonn 2025 – wissenschaftliches Programm
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MO: Fachverband Molekülphysik
MO 4: Molecular Spectroscopy of Liquid Jets I
MO 4.2: Vortrag
Montag, 10. März 2025, 17:15–17:30, HS XVI
Exploring the origin of multiple plateaus in liquid high-harmonic generation — •Angana Mondal1, Ofer Neufeld2, Tadas Balciunas1, Zhong Yin1, Benedikt Wasser1, Serge Müller1, Angel Rubio3,4,5, Nicolas Tancogne-Dejean33,4, and Hans Jakob Wörner1 — 1Laboratorium für Physikalische Chemie, ETH Zürich, Switzerland — 2Technion Israel Institute of Technology, Israel — 3Max Planck Institute for the Structure and Dynamics of Matter, Germany — 4Center for Free-Electron Laser Science CFEL, DESY, Germany — 5Physics Department, University of Hamburg, Germany
Recent studies of liquid high-harmonic generation highlight scattering-limited electron trajectories as the key mechanism, with on-site recombination as the primary process[1]. However, this framework left unexplained the absence of higher-order nonlinearities with increasing laser power. Here we report, the observation of a second plateau in the liquid HHG spectrum, attributed to electron recombination with neighboring molecules, dominated by second solvation shell contributions via hole delocalization [2,3]. The plateau exhibits weak scaling with laser wavelength, intensity, and distinct ellipticity dependence, confirmed experimentally and theoretically. Our results predict the existence of higher-order plateaus linked to successive recombination events, establishing a pathway for attosecond-scale probing of electron dynamics in liquids and solutions. Reference 1. A Mondal et al. Nat. Phys. 19, 1813-1820 (2023) 2. I Jordan et al. Science 369, 974-979 (2020) 3. X Gong et al. Nature 609, 507-511 (2022)
Keywords: High-harmonic spectroscopy; Liquid phase dynamics; Ultrafast processes; Liquid flat-jet; High-harmonic generation