2D THz-THz-Raman Simulations in Liquid Bromoform

Low frequency excitations in the condensed phase play a crucial role in processes such as solvation, dynamics of bio-molecules and liquid phase chemistry. Two dimensional Terahertz-Raman methods measure the 3rd order non-linear response of mater to a sequence of three laser pulses (Raman-THz-THz, THz-Raman-THz or THz-THz-Raman) and provide means to study the origin of anharmonicity and coupling between these thermally excited, low frequency modes. We have developed theoretical techniques to model the non-linear responses using a range of methods that involve different levels of approximations, including methods based on all-atom simulation and reduced density matrix modeling. We employ these methods to analyze recently measured THz-THz-Raman response in liquid bromoform.