Abstract

Coherent control of resonant and non-resonant two-photon absorption processes was examined using a spatio-temporal pulse-shaping technique. By utilizing a combination of temporal focusing and femtosecond pulse-shaping techniques, we spatially control multiphoton absorption processes in a completely deterministic manner. Distinctive symmetry properties emerge through two-dimensional mapping of spatio-temporal data. These symmetries break down in the transition to strong fields, revealing details of strong-field effects such as power broadenings and dynamic Stark shifts. We also present demonstrations of chirp-dependent population transfer in atomic rubidium, as well as the spatial separation of resonant and non-resonant excitation pathways in atomic caesium.

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