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Published on: November 11, 2013
Nonadiabatic quantum dynamics and laser control of Br2 in solid argon
A Accardi1, A Borowski, O Kühn
1Institut für Chemie und Biochemie, Freie Universität Berlin, Takustrasse 3, D-14195 Berlin, Germany.
The Journal of Physical Chemistry. A
|May 15, 2009
Summary
This study introduces a model for Br(2) predissociation dynamics in argon crystals, showing matrix cage compression aids nonadiabatic transitions. Vibrational preexcitation offers an alternative predissociation pathway by shifting the Franck-Condon window.
Area of Science:
- * Physical Chemistry
- * Quantum Dynamics
- * Spectroscopy
Background:
- * Bromine dimer (Br2) exhibits complex predissociation dynamics.
- * Lattice environments significantly influence molecular excited states.
- * Understanding nonadiabatic transitions is crucial in condensed phases.
Purpose of the Study:
- * To model the B- to C-state predissociation of Br2 in an argon crystal.
- * To investigate the role of matrix cage compression in nonadiabatic transitions.
- * To explore vibrational preexcitation as a method to control predissociation.
Main Methods:
- * Development of a five-dimensional reaction surface-vibronic coupling model.
- * Simulation of quantum dynamics initiated by Franck-Condon vertical excitation.
- * Application of optimal control theory for vibrational preexcitation.
Main Results:
- * Matrix cage compression enhances nonadiabatic transitions.
- * Vibrational preexcitation enables predissociation without significant matrix compression.
- * A pump-dump mechanism involving the repulsive C state can achieve vibrational preexcitation.
Conclusions:
- * The vibronic coupling model accurately describes Br2 predissociation in argon.
- * Matrix environment plays a critical role in controlling excited-state dynamics.
- * Vibrational control offers a pathway to tune molecular dissociation processes.
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