The development of a time-resolved coherent anti-Stokes Raman scattering (CARS) variant
for use as a probe of excited electronic state Raman-active modes following excitation with
an ultrafast pump pulse is detailed. Application of this technique involves a combination of
broadband fs-time scale pulses and a narrowband pulse of ps duration that allows
multiplexed detection of the CARS signal, permitting direct observation of molecular Raman
frequencies and intensities with time resolution dictated by the broadband pulses. Thus, this …