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

We present experiments demonstrating an enhancement of resonant two-photon transition rate in 87Rb utilizing spectral phase manipulation of the excitation frequency comb. By selectively removing certain comb teeth, the resonant two-photon transition rate can be improved, and reach a factor of more than 1.8. The femtosecond pulse-train excitation of two-photon transition is investigated theoretically based on general multiphoton transitions and the results are compared with the experiments. The theory presented here gives a clear insight of physical mechanism of this quantum coherent control and indicates that it is simple, effective and universal for nonlinear interactions between frequency combs and matters.