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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.

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This summary is machine-generated.

Researchers developed a new method to observe charge migration in molecules using infrared multi-photon ionization and X-ray lasers. This technique allows for the selective triggering and probing of electron coherence dynamics, advancing attosecond molecular science.

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Area of Science:

  • Attosecond molecular science
  • Quantum dynamics
  • Electron coherence

Background:

  • Correlation-driven charge migration is a key phenomenon in attosecond molecular science.
  • Despite theoretical interest, unambiguous experimental observation of quantum beating in charge migration remains challenging.

Purpose of the Study:

  • To present a method for selectively triggering and probing correlation-driven charge migration dynamics.
  • To investigate molecules exhibiting long-lived electron coherence.

Main Methods:

  • Selective triggering of charge migration using infrared multi-photon ionization.
  • Probing dynamics with the spatial resolution of X-ray free-electron lasers.
  • Utilizing real-time time-dependent density-functional theory (RT-TDDFT) to model the dynamics.

Main Results:

  • Demonstrated a promising experimental scheme to study charge migration.
  • Showed that RT-TDDFT can accurately describe correlation-driven charge migration in molecules with specific electronic structures.
  • Identified hole mixing involving the highest occupied molecular orbital as a key factor.

Conclusions:

  • The proposed method offers a pathway to experimentally observe elusive quantum beating in charge migration.
  • RT-TDDFT is a viable tool for simulating these complex electronic dynamics.
  • Advances in attosecond science are crucial for understanding fundamental molecular processes.