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MO: Fachverband Molekülphysik
MO 19: MO Poster 4
MO 19.3: Poster
Donnerstag, 12. März 2020, 17:00–19:00, Empore Lichthof
Role of coherence for photoelectron circular dichroism after multi-photon excitation in randomly oriented chiral molecules — •Alexander Blech1, R. Esteban Goetz1, Timur A. Isaev2, Behnam Nikoobakht2, Robert Berger2, Loren Greenman3, and Christiane P. Koch1 — 1Universität Kassel, Deutschland — 2Philipps-Universität Marburg, Deutschland — 3Kansas State University, Manhattan KS, USA
Photoelectron circular dichroism (PECD) refers to the forward/backward asymmetry in the photoelectron angular distribution with respect to the propagation axis of circularly polarized light. Our existing model for PECD in resonantly enhanced multi-photon ionisation of randomly oriented chiral molecules is based on perturbation theory for the light-matter interaction and on ab initio calculations for the multi-photon absorption, giving semi-quantitative agreement with experimental data for fenchone and camphor.
Here we present an extended model that explicitly takes into account the coherence between non-resonant multi-photon excitation and one-photon ionisation as well as the chirality of the photoelectron continuum by solving the scattering problem for the photoelectron. Our new theoretical description allows us to distinguish the contributions of intermediate and final states to PECD. This will be a first step towards refining our quantum optimal control approach in order to determine the ultimate strength of the chiral response.