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We present experiments demonstrating an enhancement of resonant two-photontransition rate in 87Rb utilizing spectral phase manipulation of the excitationfrequency comb. By selectively removing certain comb teeth, the resonanttwo-photon transition rate can be improved, and reach a factor of more than1.8. The femtosecond pulse-train excitation of two-photon transition isinvestigated theoretically based on general multiphoton transitions and theresults are compared with the experiments. The theory presented here gives aclear insight of physical mechanism of this quantum coherent control andindicates that it is simple, effective and universal for nonlinear interactionsbetween frequency combs and matters.

Enhancement of two-photon transition rate by selectively removing certain frequency comb teeth