Optical control of the quantum-state distribution of vibrational wave packets using trains of phase-locked pulses

An intuitive scheme for controlling the quantum state composition of one- coordinate molecular wave packets is developed. The accumulated phase difference between the various components of the molecular wave packet is determined, and then a sequence of phase- locked optical pulses is employed to selectively enhance or depopulate specific vibrational states, or sets of vibrational states. The quantum state composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multi- pulse response of the time- dependent vibrational state populations.