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Photoionization time-delay in conjugated molecules arises from two factors: pathway interferences and electron correlations. Longer molecules show significantly larger delays due to interference effects, aligning with experimental findings.

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Area of Science:

  • Quantum chemistry
  • Molecular physics
  • Attosecond science

Background:

  • Photoionization time-delays offer insights into electron dynamics within molecules.
  • Linear conjugated molecules are model systems for studying electron correlation and delocalization.

Purpose of the Study:

  • To compute and analyze photoionization time-delays in linear conjugated molecules.
  • To elucidate the contributions of different electronic processes to ionization time-delays.

Main Methods:

  • Utilized the Wigner scattering approach for theoretical computation.
  • Analyzed contributions from interferences between ionization pathways and electron-electron correlations.

Main Results:

  • Identified two additive contributions to photoionization time-delays.
  • Interference between pathways scales with conjugation length, increasing time-delay.
  • Electron correlation contribution is less sensitive to conjugation length.

Conclusions:

  • The Wigner scattering approach successfully models photoionization time-delays.
  • Interference effects are dominant for longer conjugated systems, explaining experimental observations.
  • Understanding these contributions is crucial for controlling and interpreting molecular photoionization.