Time resolved femtosecond dynamics of carbon disulfide (CS2) molecules using Degenerate Four-Wave Mixing

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.