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Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization
Published on: August 6, 2018
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Strong and Long Makes Short: Strong-Pump Strong-Probe Spectroscopy
Maxim F Gelin1, Dassia Egorova2, Wolfgang Domcke1
1†Department of Chemistry, Technische Universität München, D-85747 Garching, Germany.
The Journal of Physical Chemistry Letters
|August 22, 2015
Summary
We introduce a novel strong-pump strong-probe (SPSP) spectroscopy technique. This method achieves high temporal resolution for ultrafast molecular dynamics, overcoming limitations of traditional methods.
Area of Science:
- Physical Chemistry
- Spectroscopy
- Quantum Dynamics
Background:
- Traditional pump-probe spectroscopy is limited by pulse durations for resolving ultrafast molecular processes.
- Investigating rapid electronic and vibrational dynamics requires advanced spectroscopic techniques.
Purpose of the Study:
- To introduce and validate a new time-domain spectroscopic technique, strong-pump strong-probe (SPSP) spectroscopy.
- To demonstrate the capability of SPSP for resolving ultrafast dynamics beyond the pulse duration limit.
Main Methods:
- Development of the strong-pump strong-probe (SPSP) technique.
- Numerical simulations of SPSP signals using a multilevel vibronic model.
- Analysis of simulated signals for electronic and vibrational coherences.
Main Results:
- SPSP signals exhibit electronic and vibrational beatings on timescales shorter than pulse durations.
- The technique's temporal resolution is independent of the pump and probe pulse lengths.
- Simulations confirm the feasibility of resolving ultrafast molecular events.
Conclusions:
- SPSP spectroscopy offers enhanced temporal resolution for studying molecular dynamics.
- This technique can probe processes previously inaccessible to conventional pump-probe methods.
- SPSP spectroscopy holds promise for real-time investigations of complex molecular systems.
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