Freiburg 2024 – wissenschaftliches Programm
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A: Fachverband Atomphysik
A 9: Strong-field Ionization and Imaging (joint session MO/A)
A 9.4: Vortrag
Montag, 11. März 2024, 17:45–18:00, HS 3044
Molecular self-probing for the visualisation of vibrational wave-packet dynamics and its laser-induced modification — •Gergana D. Borisova1, Paula Barber Belda1, Shuyuan Hu1, Paul Birk1, Veit Stooß1, Maximilian Hartmann1, Robert Moshammer1, Alejandro Saenz2, Christian Ott1, and Thomas Pfeifer1 — 1Max-Planck-Institut für Kernphysik, 69117 Heidelberg — 2Institut für Physik, Humboldt-Universität zu Berlin, 12489 Berlin
We present an all-optical pump-control scheme for molecular wave-packet (WP) visualisation and control, where the molecular ground state acts as an intrinsic self-probe of the system, imprinting the evolution of an excited wave packet onto the coherent dipole emission [1]. In a proof-of-principle experiment, coherent extreme ultraviolet (XUV) light creates a vibrational wave packet in the electronically excited D 1Πu3pπ state of neutral H2. Measured XUV absorption spectra of the D-state vibronic resonances provide access to the WP dynamics after reconstruction of the time-dependent dipole response [2], which probes the vibrating wave packet through the molecular ground state. An intense near-infrared (NIR) pulse, applied shortly after the WP excitation, is used to control the wave-packet evolution and through this its revival. With increasing NIR intensity the WP revival shifts to earlier times. We identify state-specific NIR-induced phase shifts as the origin of the observed time shifts, which can be applied even to complex molecular systems to coherently steer the recovery of vibrational wave packets on electronically excited potential-energy curves at a desired time. [1] arXiv:2301.03908 [2] PRL 121 (2018) 173005
Keywords: wave-packet dynamics; time-dependent dipole response; XUV spectroscopy; laser control