Bonn 2025 – scientific programme
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MO: Fachverband Molekülphysik
MO 28: Ultrafast Dynamics IV
MO 28.1: Talk
Friday, March 14, 2025, 11:00–11:15, HS XVI
Generation of atomic coherence by ultrafast molecular photodissociation probed by heterodyned detected attosecond four-wave-mixing spectroscopy — •francesco montorsi1,2, patrick rupprecht3, lei xu4, niri govind4, shaul mukamel5, marco garavelli2, daniel m. neumark3, stephen r. leone3, and daniel keefer1 — 1Max-Planck-Institut für Polymerforschung, 55128 Mainz, Germany — 2Dipartimento di Chimica industriale Toso Montanari, Università di Bologna, 40136 Bologna, Italy — 3epartment of Chemistry, University of California, Berkeley, California 94720, USA — 4Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99352, United States — 5Department of Chemistry, Physics and Astronomy, University of California, Irvine, California 92697, USA
Electronic coherences (EC) in molecules can naturally form, after photoexcitation, in the vicinity of so-called conical intersections (CIs). Here, we theoretically investigate the evolution of EC generated during a photochemical process namely the bond cleavage in methyliodine. Quantum dynamics simulations show that the coherence spawned in the molecule by a CI is rapidly transferred to the atomic iodine upon dissociation. This allows the preparation of a long-lived EC, making it interesting for quantum technology applications. Finally, we propose a spectroscopic scheme based on the interference of two attosecond four-wave mixing signals which enables a background-free tomography of such EC providing crucial information about its generation at the molecular CI
Keywords: electronic coherence; attosecond four-wave-mixing; quantum dynamics; conical intersections; heterodyne detection