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Attosecond Dynamics of Molecular Electronic Ring Currents.

Kai-Jun Yuan1, Chuan-Cun Shu2, Daoyi Dong2

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Researchers tracked ultrafast charge migration in molecules using circularly polarized UV and X-ray pulses. This method reveals electronic coherence dynamics and circular charge migration on an attosecond timescale.

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Area of Science:

  • Physical Chemistry
  • Quantum Dynamics
  • Attosecond Science

Background:

  • Ultrafast charge migration is crucial for understanding photoinduced chemical reactions.
  • Observing these quantum dynamics necessitates high spatial and temporal resolution.
  • Current methods face challenges in achieving attosecond resolution for charge migration.

Purpose of the Study:

  • To demonstrate a method for tracking electronic coherence dynamics in molecules.
  • To probe ultrafast circular charge migration induced by UV pulses.
  • To achieve attosecond temporal resolution for observing quantum coherence.

Main Methods:

  • Utilized a circularly polarized ultraviolet (UV) pulse to induce electronic coherence.
  • Employed a time-delayed, circularly polarized attosecond X-ray pulse as a probe.
  • Analyzed X-ray probe spectra to retrieve time-resolved charge migration information.

Main Results:

  • Successfully tracked electronic coherence dynamics on an attosecond timescale.
  • Observed instantaneous circular charge migration information encoded in X-ray spectra.
  • Demonstrated a strong dependence of electronic coherence on UV pulse helicity.

Conclusions:

  • The proposed X-ray probing technique provides attosecond resolution for charge migration.
  • This method allows real-time access to electronic quantum coherence dynamics.
  • Offers a direct approach to control photophysical and photochemical reactions.