Full molecular dynamics simulations of molecular liquids for single-beam spectrally controlled two-dimensional Raman spectroscopy

Single-beam spectrally controlled (SBSC) two-dimensional (2D) Raman spectroscopy is a unique 2D vibrational measurement technique utilizing trains of short pulses that are generated from single broadband pulse by shaping. This approach overcomes the difficulty in dealing with small-signal extraction and avoids complicated low-order cascading effects, thus providing new possibility for measuring intramolecular intermolecular modes molecular liquids using fifth-order spectroscopy. Recently, quantitatively investigating mode–mode coupling mechanism, Hurwitz et al. [Opt. Express 28, 3803 (2020)] have developed design this to separate contributions fifth- third-order polarizations, which often overlapped original single-beam measurements. Here, we describe method simulating these measurements on basis second-order response function approach. We carry out full dynamics simulations carbon tetrachloride liquid water an equilibrium–nonequilibrium hybrid algorithm, aim explaining key features SBSC spectroscopic theoretical point view. The predicted signal profiles intensities provide valuable information can be applied experiments, allowing them carried more efficiently.