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We study in detail coherent phase control of femtosecond resonance-mediated(2+1) three-photon absorption and its dependence on the spectral bandwidth ofthe excitation pulse. The regime is the weak-field regime of third perturbativeorder. The corresponding interference mechanism involves a group ofthree-photon excitation pathways that are on resonance with the intermediatestate and a group of three-photon excitation pathways that are near resonantwith it. The model system of the study is atomic sodium (Na), for whichexperimental and numerical-theoretical results are obtained. Prominent amongthe results is our finding that with simple proper pulse shaping an increase inthe excitation bandwidth leads to a corresponding increase in the enhancementof the three-photon absorption over the absorption induced by the (unshaped)transform-limited pulse. For example, here, a 40-nm bandwidth leads to anorder-of-magnitude enhancement over the transform-limited absorption.

Pulse-Bandwidth Dependence of Coherent Phase Control of Resonance-Mediated (2+1) Three-Photon Absorption