Preparation and resolution of molecular states by coherent sequences of phase-locked ultrashort laser pulses

J Chem Phys. 2004 Aug 1;121(5):2117-24. doi: 10.1063/1.1767513.

Abstract

We study the application of nonlinear wave packet interferometry to the preparation and resolution of the overlaps of nonstationary nuclear wave functions evolving in an excited electronic state of a diatomic molecule. It is shown that possible experiments with two phase-locked ultrashort pulsepairs can be used to determine a specific vibrational wave packet state in terms of coherent states of the ground electronic state. We apply this scheme to an idealized molecule with harmonic potential energy surfaces and to the X <-- B transition states of the iodine molecule. Our results indicate that this scheme is very promising as a potential tool to quantum control.