Abstract

It is generally appreciated that femtosecond pump-probe techniques have the potential to provide novel and important information on elementary photophysical and photochemical processes. It has been demonstrated by several applications that time-resolved two-pulse ionization, that is, optical excitation and subsequent ionization of a molecular system with two short laser pulses, is a promising tool to observe excited state dynamics in real time.¹ In comparison to alternative real-time probing techniques such as stimulated emission or excited-state absorption with fluorescence detection, two-pulse ionization spectroscopy possesses the advantage of extreme sensitivity of signal detection. The possibility of recording, for each pulse configuration, a complete photoelectron spectrum suggests that time-resolved ionization spectroscopy may be able to yield unprecedentedly detailed information on ultrafast intramolecular processes.

© 1992 The Author(s)