Optical N-wave-mixing spectroscopy with strong and temporally well-separated pulses: The doorway-window representation

We have extended the doorway-window representation of optical pump-probe spectroscopy with weak pulses toward N-wave-mixing spectroscopy with temporally well-separated pulses of arbitrary strength. The expressions for the signals in the strong-pulse doorway-window representation are derived in the framework of the nonperturbative theory of N-wave-mixing spectroscopy. The strong- pulse doorway-window representation is complementary to the equation-of-motion phase-matching approach. The latter fully accounts for pulse-overlap effects in signals induced by weak pulses but is computationally more expensive. The performance of the doorway-window approximation for temporally well-separated strong pulses is illustrated for an electronic two-level system with an underdamped Condon-active vibrational mode.