Abstract

The authors introduce and describe pulse train control (PTC) of population branching in strongly coupled processes as a novel control tool for the separation of competing multiphoton processes. Control strategies are presented based on the different responses of processes with different photonicities and/or different frequency detunings to the pulse-to-pulse time delay and the pulse-to-pulse phase shift in pulse trains. The control efficiency is further enhanced by the property of pulse trains that complete population transfer can be obtained over an extended frequency range that replaces the resonance frequency of simple pulses. The possibility to freely tune the frequency assists the separation of the competing processes and reduces the number of subpulses required for full control. As a sample application, PTC of leaking multiphoton resonances is demonstrated by numerical simulations. In model systems exhibiting sizable background (intruder) state population if excited with single pulses, PTC leading to complete accumulation of population in the target state and elimination of background population is readily achieved. The analysis of the results reveals different mechanisms of control and provides clues on the mechanisms of the leaking process itself. In an alternative setup, pulse trains can be used as a phase-sensitive tool for level switching. By changing only the pulse-to-pulse phase shift of a train with otherwise unchanged parameters, population can be transferred to any of two different target states in a near-quantitative manner.

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