Cascaded free-induction decay four-wave mixing Original Research Article

We report the observation of cascaded optical free-induction decay four-wave mixing (FID-FWM) signal. This process can take place when nonlinear optical measurements are carried out with pulses that are orders of magnitude shorter than the dephasing time of the sample. Experimental observations and theoretical calculations show that the coherent emission from the first laser pulse participates as a time-delayed local electric field to yield the cascaded signal. We arrive at this conclusion based on pulse sequences of degenerate noncollinear femtosecond pulses for which three-pulse FWM is forbidden. Further confirmation was obtained from experiments where the time delay between two pulses were used to form ground or excited state populations, the signal reflected the corresponding ground or excited state dynamics. Although FID is long lived, the femtosecond resolution was found to be maintained in our measurements on gas phase molecular iodine. This is because the FID is modulated in the femtosecond time scale by the molecular dynamics of the system; its intensity and modulation were confirmed using femtosecond time-gated up-conversion measurements.