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Bulletin of the American Physical Society

Probing Time-Dependent Electron Interactions in Double-Rydberg Wavepackets

X. Zhang, R. R. Jones

Published May 19, 2006• 0 citations
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A technique for generating Rydberg wavepackets in preferred target states is demonstrated that exploits the mixed phase space structure of the periodically `kicked' Rydberg atom. Experimental data and classical simulations for very-high- n Rydberg atoms are presented that show that application of a train of equispaced, unidirectional half-cycle pulses can lead to localization of the final wavepacket in classical stable islands. The product wavepackets are examined using a delayed half-cycle probe pulse. It is demonstrated that the motion of the wavepackets is either quasiperiodic or random depending on whether or not the initial state of the atom overlaps a stable island.
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 (/spl sim/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 (Rb/sub 2/) and the distribution of atomic fragments into excited states spanning >10 000 cm/sup -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.