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Strong-field-induced wave packet dynamics in carbon dioxide molecule
Artem Rudenko1, Varun Makhija2, Aram Vajdi3
1J.R Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, Kansas 66506, USA. rudenko@phys.ksu.edu and Max-Planck-Institut für Kernphysik, 69117 Heidelberg, Germany.
Faraday Discussions
|October 7, 2016
Summary
Strong-field excitation of carbon dioxide (CO2) reveals vibrational dynamics in both ionic and neutral states. Rotational motion causes coherent electronic wave packet decay in ions within 10 ps.
Area of Science:
- Physical Chemistry
- Quantum Dynamics
- Molecular Spectroscopy
Background:
- Understanding molecular dynamics under strong laser fields is crucial for controlling chemical reactions.
- Carbon dioxide (CO2) is a fundamental molecule for studying electronic and nuclear wave packet evolution.
Purpose of the Study:
- To investigate the temporal evolution of electronic and nuclear wave packets in CO2 following strong-field excitation.
- To elucidate the mechanisms of vibrational excitation in both neutral and ionic CO2 states.
- To explore the influence of rotational motion on electronic wave packet dynamics.
Main Methods:
- Momentum-resolved ion spectroscopy.
- Channel-selective Fourier analysis.
- Pump-probe spectroscopy with varying pulse durations (8 fs and 35 fs).
Main Results:
- Observed signatures of vibrational dynamics in both ionic and neutral CO2 states.
- Identified far-off-resonance two-photon Raman scattering as the likely mechanism for vibrational excitation in neutral CO2.
- Found evidence of electronic and vibrational excitations in ionic states, involving ground and first excited electronic states.
- Demonstrated complete decay of coherent electronic wave packets in ions within 10 ps due to rotational coupling.
Conclusions:
- The study provides insights into the complex interplay of electronic, nuclear, and rotational dynamics in CO2 under strong laser fields.
- The use of shorter pulses revealed neutral state contributions not observed previously.
- Rotational motion significantly impacts the coherence of electronic wave packets in ionic CO2.
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