Production and probing of atomic wavepackets with ultrafast laser pulses: Applications to atomic and molecular dynamics

We demonstrate that atomic wavepackets can serve as sensitive detectors for investigating atomic and molecular dynamics. In concert with parametric four-wave mixing, the interference between coherent superpositions of atomic excited states produced by ultrafast (∼150 fs) pump and probe pulses provides a new and powerful tool with which fundamental processes, such as molecular dissociation and Rydberg-Rydberg atomic collisions, can be observed with the extraordinary sensitivity afforded by a coherent nonlinear optical process. Experiments are described in which the dissociation of an electronically excited molecule (Rb²) and the distribution of atomic fragments into excited states spanning > 10 000 cm^-1 are observed. Also, resonant collisions between Rb atoms in the 7s and 5d states are detected by monitoring the shift in the frequency of an atomic wavepacket induced by the dipole-dipole interaction.