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Transient-Absorption Pump-Probe Spectra as Information-Rich Observables: Case Study of Fulvene.

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Summary

Conical intersections (CIs) efficiently drive molecular processes. This study shows simulated transient absorption (TA) pump-probe (PP) spectra reveal more about CI dynamics than electronic populations alone.

Keywords:
conical intersectionsdoorway window approximationsymmetrical quasiclassical/Meyer–Miller–Stock–Thosstransient absorption pump-probe spectroscopy

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Area of Science:

  • Photochemistry
  • Theoretical Chemistry
  • Spectroscopy

Background:

  • Conical intersections (CIs) are critical for ultrafast molecular processes like photodeactivation and energy transfer.
  • Femtosecond spectroscopy is a key experimental technique for studying these CI-driven dynamics.

Purpose of the Study:

  • To investigate conical intersection-mediated internal conversion in fulvene using ab initio methods.
  • To explore the utility of simulated time-resolved transient absorption (TA) pump-probe (PP) spectra for characterizing molecular dynamics.

Main Methods:

  • Comprehensive ab initio simulations of electronic population, bond lengths, and angles.
  • On-the-fly evaluation of TA pump-probe spectra using symmetrical quasiclassical/Meyer-Miller-Stock-Thoss (SQC/MMST) dynamics.
  • Application of the doorway-window representation for spectroscopic signal analysis.

Main Results:

  • Simulated TA pump-probe spectra successfully captured population dynamics and key nuclear motions, including mode-mode couplings.
  • Demonstrated that TA pump-probe signals provide richer information than electronic populations for analyzing CI-driven dynamics.
  • Highlighted the potential of theoretical TA pump-probe spectra as informative theoretical observables.

Conclusions:

  • Time-resolved TA pump-probe spectroscopy, both experimentally and theoretically, offers deeper insights into conical intersection dynamics.
  • Theoretical analysis of TA pump-probe spectra can extract detailed information on nuclear motions and couplings.
  • This approach enhances our understanding of photophysical processes mediated by conical intersections.