title: Strong and Long Makes Short: Strong-Pump Strong-Probe Spectroscopy.
abstract: We propose a new time-domain spectroscopic technique that is based on strong pump and probe pulses. The strong-pump strong-probe (SPSP) technique provides temporal resolution that is not limited by the durations of the pump and probe pulses. By numerically exact simulations of SPSP signals for a multilevel vibronic model, we show that the SPSP signals exhibit electronic and vibrational beatings on time scales which are significantly shorter than the pulse durations. This suggests the possible application of SPSP spectroscopy for the real-time investigation of molecular processes that cannot be temporally resolved by pump-probe spectroscopy with weak pump and probe pulses.
authors: †Department of Chemistry, Technische Universität München, D-85747 Garching, Germany.
authors: Maxim F
authors: MF
authors: Gelin
authors: ‡Institute of Physical Chemistry, Christian-Albrechts-Universität zu Kiel, D-24098 Kiel, Germany.
authors: Dassia
authors: D
authors: Egorova
authors: †Department of Chemistry, Technische Universität München, D-85747 Garching, Germany.
authors: Wolfgang
authors: W
authors: Domcke
keywords: strong fields; time resolution; ultrafast spectroscopy