Abstract
We investigate coherent control of the two-photon transition pathways of a four-level atomic system in a diamond configuration. When an ultrashort laser pulse interacts with this system in the ground state 5S1/2 of rubidium, the two-photon transition probability amplitude of 5D3/2 is obtained by a summation of all possible resonant and nonresonant two-photon transition probability amplitudes via 5P1/2 and 5P3/2. Second-order perturbation theory predicts that the maximal constructive interference of the transition probability amplitudes occurs when the phases of eight different spectrum blocks satisfy four different phase relations. Experiments carried out with spectrally phase-coded laser pulses show good agreement with the theoretical prediction.
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