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Waveform control of molecular dynamics close to a conical intersection
Franziska Schüppel1, Thomas Schnappinger1, Lena Bäuml1
1Department of Chemistry, LMU Munich, D-81377 Munich, Germany.
The Journal of Chemical Physics
|December 15, 2020
Summary
Carrier envelope phase control of conical intersections can steer chemical reactions. This study demonstrates optical control of branching ratios in femtosecond laser pulses, showing potential for real chemical systems like uracil.
Area of Science:
- Quantum Chemistry
- Molecular Dynamics
- Ultrafast Spectroscopy
Background:
- Conical intersections are critical points in molecular potential energy landscapes.
- They facilitate ultra-fast radiationless relaxation and influence reaction product distributions.
- Their unique properties enable optical control of chemical dynamics within femtoseconds.
Purpose of the Study:
- To explore optical control strategies using the carrier envelope phase of few-cycle infrared pulses.
- To investigate the influence of imprinted phase information on branching ratios at conical intersections.
- To assess the applicability of this control mechanism to realistic chemical systems.
Main Methods:
- Theoretical investigation of laser-matter interactions.
- Simulation of wave packet dynamics approaching conical intersections.
- Analysis of carrier envelope phase effects on electronic superposition and nuclear dynamics.
Main Results:
- Laser-induced electronic superposition before reaching the conical intersection.
- Carrier envelope phase directly influences the imprinted phase information.
- Demonstrated control over branching ratios in a model system.
- Successful transfer of control principles to uracil.
Conclusions:
- Carrier envelope phase offers a viable route for controlling chemical reactions at conical intersections.
- This method provides precise optical control in the few-femtosecond timescale.
- The findings are transferable to complex, realistic molecular systems.
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