Selective preparation of the zeroth-order vibrational states in the HOD molecule by ultrashort infrared laser pulses

An approach for controlling the molecular dynamics competing against intramolecular vibrational-energy redistribution and selective preparation of the zeroth-order vibrational states on a picosecond time scale is developed and demonstrated for the HOD molecule. The zeroth-order states of a local OH bond are prepared selectively and demonstrate the coherent oscillatory behaviour after the end of the laser excitation. Coherent in-phase and out-of-phase oscillations are demonstrated by two single zeroth-order states efficiently coupled to each other. Quasi-periodic in-phase and out-of-phase oscillations occur if a single zeroth-order state is coupled to several other zeroth-order states. The frequency of these oscillations depends on the laser field which prepares the state. The laser control scheme includes superposition of properly optimized infrared laser pulses of a subpicosecond duration.