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Probing Electronic Symmetry Reduction during Charge Migration via Time-Resolved X-Ray Diffraction
Journal
ChemPhysChem
ISSN
14394235
Date Issued
2023-01-17
Author(s)
Tremblay, Jean Christophe
Blanc, Ambre
Krause, Pascal
Giri, Sucharita
Dixit, Gopal
Abstract
The present work focuses on probing ultrafast charge migration after symmetry-breaking excitation using ultrashort laser pulses. LiCN is chosen as prototypical system because it can be oriented in the laboratory frame and it possesses optically-accessible charge transfer states at low energies. The charge migration is simulated within the hybrid time-dependent density functional theory/configuration interaction framework. Time-resolved electronic current densities and simulated time-resolved x-ray diffraction signals are used to unravel the mechanism of charge migration. Our simulations demonstrate that specific choices of laser polarization lead to a control over the symmetry of the induced charge migration. Moreover, time-resolved x-ray diffraction signals are shown to encode transient symmetry reduction at intermediate times.
Subjects