Quantum control of four-level diamond-configuration quantum system Jaewook Ahn (KAIST) Two-photon transition pathways of a four-level atomic system in a diamond con?guration is investigated. 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 as a sum of all possible resonant and nonresonant two-photon transition probability amplitudes via 5P1/2 and 5P3/2. Second-order perturbation theory predicts a spectral phase-code solution for an "optimal" laser pulse that induces the maximal constructive interference of the transition probability amplitudes. Experiments carried out with spectrally phase-coded laser pulses show good agreement with the theoretical prediction.