Phase effects in a quantum control experiment on the two-photon transition 4s <--<-- 3s of atomic sodium are studied. In our experiment, we combine the generation of phase-locked interferometrically generated pulses with pulse-shaping techniques to study in detail the interplay of optical and quantum-mechanical phases. Subtle differences in the physical realization of the pulse sequences produce large difference in the control objective-the 4s population. The control mechanisms of more complex pulse sequences generated by periodic and discontinuous phase-modulation functions are investigated systematically and analyzed on the basis of quantum-mechanical interference.
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