Coherent quantum control of two-photon transitions by a femtosecond laser pulse

Coherent quantum control(1-3) has attracted interest as a means to influence the outcome of a quantum-mechanical interaction. In principle, the quantum system can be steered towards a desired state by its interaction with light. For example, in photoinduced transitions between atomic energy levels, quantum interference effects can lead to enhancement or cancellation of the total transition probability. The interference depends on the spectral phase distribution of the incident beam; as this phase distribution can be tuned, the outcome of the interaction can in principle be controlled. Here we demonstrate that a femtosecond laser pulse can be tailored, using ultrashort pulse-shaping(4-7) techniques, to control two-photon transitions in caesium. By varying the spectral phases of the pulse components, we observe the predicted cancellation of the transitions due to destructive quantum interference; the power spectrum and energy of these 'dark pulses' are unchanged. We also show that the pulse shape can be modified extensively without affecting the two-photon transition probability.