A new experimental method for ultrafast time-resolved pump-probe Raman
spectroscopy by use of temporally incoherent light is proposed. It is
predicted that the temporal resolution of this pump-probe Raman exper
iment is not determined by the duration of pump and probe pulses but b
y the cross-correlation time between pump and probe lights. This idea
is experimentally examined for Raman scattering from electronically ex
cited trans-stilbene in n-hexane solution. In accordance with the pred
iction, the picosecond decay of the Raman band at 1560 cm-1 arising fr
om the stilbene molecules in the S1 state is observed by use of nanose
cond pump and probe pulses, while no decay is observed for the Raman b
ands of the solvent.