Coherent control of nonresonant two-photon excitation in molecules

We extend coherent control schemes of nonresonant two-photon excitation from the atomic case to the molecular case. In particular, we study the two-photon excitation process induced by a set of laser sub-pulses both in a higher dissociating state and a bound state by solving the time-dependent Schr\"odinger equation. Our results show that for two-photon excitation to a higher dissociating state previous control schemes, validated for the atomic case before, do fail due to the coupling electronic and nuclear motion. For bound states we show that by controlling the time delay and the carrier-to-envelope phase difference between two consecutive Gaussian pulses we can either maximize or minimize the two-photon excitation process to a desired bound state.