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Updated: Sep 10, 2025

Direct Imaging of Laser-driven Ultrafast Molecular Rotation
Published on: February 4, 2017
Correlation-driven charge migration triggered by infrared multi-photon ionization
Clément Guiot du Doignon1, Rajarshi Sinha-Roy1, Franck Rabilloud1
1Université Claude Bernard Lyon 1, CNRS, Institut Lumière Matière, UMR5306 F-69100 Villeurbanne France rajarshi.sinha-roy@univ-lyon1.fr victor.despre@univ-lyon1.fr.
None:
The possibility of observing correlation-driven charge migration has been a driving force behind theoretical and experimental developments in the field of attosecond molecular science since its inception. Despite significant accomplishments, the unambiguous experimental observation of this quantum beating remains elusive. In this work, we present a method to selectively trigger such dynamics in molecules predicted to exhibit long-lived electron coherence. We show that these dynamics can be selectively triggered using infrared multi-photon ionization and probed using the spacial resolution of X-ray free-electron laser, proposing a promising experimental scheme to study these pivotal dynamics. Additionally, we demonstrate that real-time time-dependent density-functional theory can describe correlation-driven charge migration resulting from a hole mixing structure involving the highest occupied molecular orbital of a molecule.
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