Strong-pump strong-probe spectroscopy: effects of higher excited electronic states.

The present paper is devoted to the simulation of (integral and dispersed) pump-probe signals in the nonperturbative regime for a series of material systems with multiple electronic states and excited-state absorption. We show that strong-pump strong-probe spectroscopy permits the probing of vibrational wavepackets in high-lying and/or short-lived excited electronic states with a time resolution which is not limited by the pulse durations. The field strength can be regarded as an additional experimentally controllable parameter, which can be tuned to maximize the spectroscopic information for a given material system.