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Probing Electronic Symmetry Reduction during Charge Migration via Time-Resolved X-Ray Diffraction.

Jean Christophe Tremblay1, Ambre Blanc1, Pascal Krause2

  • 1CNRS-Université de Lorraine, LPCT, 57070, Metz, France.

Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry
|September 27, 2022
PubMed
Summary

Ultrafast charge migration in LiCN molecules was controlled using laser pulses. Time-resolved X-ray diffraction revealed transient symmetry reduction during this process.

Keywords:
current densityelectron dynamicssymmetry Breakingtime-resolved x-ray diffraction

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Area of Science:

  • Physical Chemistry
  • Quantum Dynamics
  • Molecular Spectroscopy

Background:

  • Ultrafast charge migration is a fundamental process in molecular systems following photoexcitation.
  • Understanding charge dynamics is crucial for controlling chemical reactions and developing new materials.
  • Lithium cyanide (LiCN) offers a unique system for studying charge migration due to its orientational control and accessible electronic states.

Purpose of the Study:

  • To investigate ultrafast charge migration in oriented LiCN molecules after symmetry-breaking excitation.
  • To explore the control of charge migration pathways using tailored ultrashort laser pulses.
  • To analyze the information encoded in time-resolved X-ray diffraction (TRXRD) signals regarding transient symmetry changes.

Main Methods:

  • Simulations employing hybrid time-dependent density functional theory/configuration interaction (TD-DFT/CI).
  • Calculation of time-resolved electronic current densities.
  • Simulation of time-resolved X-ray diffraction (TRXRD) signals.

Main Results:

  • Demonstrated control over the symmetry of induced charge migration by selecting specific laser polarizations.
  • Observed that TRXRD signals encode transient symmetry reduction at intermediate time scales.
  • Identified LiCN as a suitable model system for probing charge migration dynamics.

Conclusions:

  • Laser polarization can steer ultrafast charge migration pathways in molecules.
  • TRXRD is a powerful technique for observing symmetry dynamics in real-time.
  • This work provides insights into controlling electron dynamics for potential applications in molecular electronics and photochemistry.