Pump-dump control and the related transient absorption spectroscopies

We combine theories of optimal pump-dump control and the related transient probe absorption spectroscopy in order to elucidate the relation between these two optical processes and the possibility of experimental realization. In the weak response regime, we identify the globally optimal pair of pump-dump control fields, and further propose a second-order difference detection scheme to monitor the wave packets dynamics that is jointly controlled by both the pump and dump fields. The globally optimal solution serves also as the initial input for the iterative search for the optimal control fields in the strong response regime. We use a model I2 molecule to demonstrate numerically the pump-dump control and the detection of a highly vibrationally excited wave packet focusing dynamics on the ground X surface in both the weak and strong response regimes. The I2B surface serves as the intermediate to assist the pump-dump control and the optical detection processes. Demonstrated in the strong response regime are the optimal pair of pump-dump molecular-π pulses that invert nearly total population onto the predefined target region within a half period of vibration motion.