Abstract
Phase dependence in nonlinear optical processes reveals an intriguing interplay between the phase coherence of a short laser pulse and the laser-induced quantum wave-packet dynamics, which cannot be observed in the linear response regime. In this paper, the intra-pulse quantum coherence is demonstrated with three examples: molecular π pulses for total inversion of electron population, unexpected chirp dependence in multi-photon absorption yield, and active control of decoherence for quantum computation. These results demonstrate that quantum coherence is a unique method in the dynamic control of molecular systems, which cannot be achieved otherwise.
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