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Tracking an electronic wave packet in the vicinity of a conical intersection.
Da-Long Qi1, Hong-Guang Duan2, Zhen-Rong Sun1
1State Key Laboratory of Precision Spectroscopy, School of Physics and Material Science, East China Normal University, 3663 North Zhongshan Road, 200062 Shanghai, China.
The Journal of Chemical Physics
|August 24, 2017
Summary
Vibrational coherence significantly impacts quantum efficiency near conical intersections. Maintaining coherence enhances quantum yield but increases transfer time, while damping reduces efficiency but speeds up transfer.
Area of Science:
- Physical Chemistry
- Quantum Dynamics
- Spectroscopy
Background:
- Conical intersections are critical in non-adiabatic processes.
- Vibrational coherence plays a key role in chemical reaction dynamics.
- Understanding energy transfer in excited states is crucial for photochemistry.
Purpose of the Study:
- To investigate the influence of vibrational coherence on quantum efficiency.
- To analyze the dynamics of electronic wave packets near conical intersections.
- To correlate vibrational damping with energy transfer pathways.
Main Methods:
- Time-dependent wave packet projection analysis.
- Tuning vibrational coherence by varying coupling to thermal baths.
- Monitoring quantum efficiency and transfer time constants.
Main Results:
- Maximum coherence yielded 93% quantum efficiency with longer transfer times.
- Strong damping reduced quantum efficiency to 50% but shortened transfer times.
- Damped wave packets exhibited tunneling and direct passage mechanisms.
Conclusions:
- Vibrational coherence is a decisive factor in wave packet dynamics.
- Controlling vibrational coherence can optimize quantum efficiency.
- The study provides direct evidence for coherence effects in conical intersection dynamics.
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