Mixed quantum-classical treatment of vibrational decoherence.
The mixed quantum-classical method based on the Bohmian formulation of quantum mechanics [J. Chem. Phys. 113, 9369 (2000)]] is applied to study the process of vibrational decoherence of I2 in a dense helium environment. Specifically, the revival of vibrational wave packets, detectable by pump-probe spectroscopy, is a quantum phenomena which depends sensitively on the coherence between the vibrational levels excited by the pump pulse. The time-dependent pump-probe revival signal is a very sensitive way of detecting vibrational dephasing induced by an environment. The very good agreement between previous experimental signals and calculations presented in ths work confirms the theoretical approach and provides a promising basis for the prediction and interpretation of future experiments exploiting quantum revivals as a probe of decoherence.
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Laboratoire Collisions, Agrégats, Réactivité, Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes, Université Paul Sabatier, 31062 Toulouse, France.