  Degenerate Four-Wave Mixing (DFWM) technique has been widely used for the
characterization of novel materials exhibiting third-order nonlinearity. From
the many geometries available for achieving this process, folded Box-CARS
(Coherent Anti-Stokes Raman Spectroscopy) geometry is widely used for their
high spatial resolution and easily achievable phase-matching. CS2 molecules are
widely studied using this technique because of their high third-order
nonlinearity. The nonlinear response of CS2 molecules has been reported as 2
ps. We report the time dynamics study of CS2 molecules at a timescale of <500
fs using 515 nm wavelength source with 1 MHz repetition rate. The results
showed that the study at this timescale (< response time of CS2 molecules)
could predict the re-orientational dynamics of CS2 which has not been reported
so far. The results are interpreted with the aid of graphical illustrations and
comparison of experimentally observed results with theoretically simulated
results.
