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Attosecond transient coherent Raman spectroscopy reveals molecular quantum dynamics. The study shows these signals remain robust against environmental noise up to hundreds of femtoseconds.

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Area of Science:

  • Quantum dynamics
  • Molecular spectroscopy
  • Physical chemistry

Background:

  • Conical intersections are crucial in molecular dynamics.
  • Attosecond transient coherent Raman spectroscopy (ATCRS) probes ultrafast molecular processes.
  • Previous ATCRS studies excluded environmental quantum noise.

Purpose of the Study:

  • To investigate the impact of environmental quantum noise on ATCRS signals.
  • To determine the robustness of electronic and vibrational coherence under dephasing conditions.
  • To assess the accessibility of quantum dynamics information via ATCRS in realistic environments.

Main Methods:

  • Numerically exact hierarchy equation of motion (HEOM) approach.
  • Simulation of vibronic wave packet dynamics through a conical intersection.
  • Modeling of electronic and vibrational dephasing due to environmental noise.

Main Results:

  • Transient coherent Raman signals are robust against electronic dephasing.
  • Vibrational dephasing does not significantly obscure the signals.
  • Quantum coherent dynamics are accessible on femtosecond timescales despite noise.

Conclusions:

  • ATCRS is a viable technique for studying molecular quantum dynamics even with environmental noise.
  • The robustness of the signals allows for probing electronic and vibrational coherence over extended periods.
  • This work paves the way for experimental investigations of quantum dynamics in noisy environments.