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Sub-7-femtosecond conical-intersection dynamics probed at the carbon K-edge. 2021

Kristina S Zinchenko, and Fernando Ardana-Lamas, and Issaka Seidu, and Simon P Neville, and Joscelyn van der Veen, and Valentina Utrio Lanfaloni, and Michael S Schuurman, and Hans Jakob Wörner
Laboratorium für Physikalische Chemie, ETH Zürich, 8093 Zürich, Switzerland.

Conical intersections allow electronically excited molecules to return to their electronic ground state. Here, we observe the fastest electronic relaxation dynamics measured to date by extending attosecond transient-absorption spectroscopy (ATAS) to the carbon K-edge. We selectively launch wave packets in the two lowest electronic states (D0 and D1) of C2H4 + The electronic D1 → D0 relaxation takes place with a short time constant of 6.8 ± 0.2 femtoseconds. The electronic-state switching is directly visualized in ATAS owing to a spectral separation of the D1 and D0 bands caused by electron correlation. Multidimensional structural dynamics of the molecule are simultaneously observed. Our results demonstrate the capability to resolve the fastest electronic and structural dynamics in the broad class of organic molecules. They show that electronic relaxation in the prototypical organic chromophore can take place within less than a single vibrational period.

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