A classical iterative theory based on the Langevin equation for two-dimensional nonlinear terahertz spectroscopy

Abstract

A classical iterative theory based on the Langevin equation is presented to obtain the nonlinear response of a system and simulate two-dimensional (2D) nonlinear terahertz (THz) spectroscopy (2DTS). Compared with the widely used method of calculating the multi-time correlation function or the Poison brackets, we start from the classical Langevin equation and use an iterative method to obtain any order of nonlinear response. The anharmonic potential (AHP) and nonlinear coordinates dependence of the dipole moment (NDM) are two types of nonlinear sources introduced here. Results are derived for general three-pulse processes with nonlinear sources, AHP or NDM, separately and with the combination of both. Only the simulative 2DTS results for the single mode case with impulsive incident THz fields are presented.