The role of molecular and resonance phases in the coherent control of chemical reactions
Abstract
Coherent control of the photoionization and photodissociation of HI and the photoionization of H2S were obtained in the region of the 5d(π, δ) resonance of HI. Interference between one- and three-photon excitation paths caused modulation of the HI+, I+, and H2S+ signals. Phase lags between the different modulated signals, measured as a function of excitation energy, revealed the roles played by molecular and resonance phases. A theory of the phase lag arising from a set of overlapping rotational resonances was developed and used to interpret the observations.