Mainz 2026 – scientific programme
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MO: Fachverband Molekülphysik
MO 9: Chirality II
MO 9.4: Talk
Tuesday, March 3, 2026, 12:00–12:15, P 110
Photoelectron circular dichroism modified by the Dynamic Stark effect — •Sudheendran Vasudevan1, Anton N. Artemyev1, Ignacio M. Casasús2, Nicolas Ladda1, Simon T. Ranecky1, Sagnik Das1, Tonio Rosen1, Fabian Westmeier1, Krishna Kant Singh1, Daniel M. Haubenreißer1, Eric Kutscher1, Jochen Mikosch1, Hendrike Braun1, Luis Bañares2, Philipp V. Demekhin1, Arne Senftleben1, and Thomas Baumert1 — 1Institute of Physics and CINSaT, University of Kassel, Heinrich-Plett-Strasse 40, 34132 Kassel, Germany — 2Dpto. de Química Física, Universidad Complutense de Madrid, Avenida de las Ciencias, 28040 Madrid, Spain
Photoelectron circular dichroism (PECD) is a highly sensitive, enantioselective probe of chirality that arises from electric-dipole interactions and appears as a forward/backward asymmetry in photoelectron angular distribution along the light propagation direction. In this work, we investigate how laser intensity affects the PECD of the chiral prototype molecule fenchone using bandwidth-limited near-UV pulses tuned between the 3s and 3p Rydberg states. Increasing intensity alters the Freeman resonances during the 2+1 REMPI process through dynamic Stark shifts and simultaneously reduces the observed PECD. Our time-dependent, single-center model suggests that the dynamic Stark effect mixes an increasingly large set of dipole-coupled virtual states into the effective polarizability of the intermediate state. This admixture of states with differing PECD signatures results in a partial cancellation and a net PECD approaching zero.
Keywords: Circular dichroism; Multiphoton ionization; Light-matter interaction; Chirality; Resonance enhanced multiphoton ionization