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We explore and describe the roles of inter-molecular vibrations employing aBrownian oscillator (BO) model with linear-linear (LL) and square-linear (SL)system-bath interactions, which we use to analyze two-dimensional (2D)THz-Raman spectra obtained by means of molecular dynamics (MD) simulations. Inaddition to linear absorption (1D IR), we calculated 2D Raman-THz-THz,THz-Raman-THz, and THz-THz-Raman signals for liquid formamide, water, andmethanol using an equilibrium non-equilibrium hybrid MD simulation. Thecalculated 1D IR and 2D THz-Raman signals are compared with results obtainedfrom the LL+SL BO model applied through use of hierarchal Fokker-Planckequations with non-perturbative and non-Markovian noise. We find that all ofthe qualitative features of the 2D profiles of the signals obtained from the MDsimulations are reproduced with the LL+SL BO model, indicating that this modelcaptures the essential features of the inter-molecular motion. We analyze thefitted 2D profiles in terms of anharmonicity, nonlinear polarizability, anddephasing time. The origins of the echo peaks of the librational motion and theelongated peaks parallel to the probe direction are elucidated using opticalLiouville paths.

Analysis of 2D THz-Raman spectroscopy using a non-Markovian Brownian oscillator model with nonlinear system-bath interactions