Solvent-induced polarization dynamics and coherent two-dimensional spectroscopy: Dissipaton equation of motion approach

Abstract

This work exploits the dissipaton equation of motion (DEOM) approach to study the solvent-induced non-Condon polarization dynamics and its two-dimensional coherent spectroscopy for model excitonic systems. DEOM is a second quantization generation of the celebrated hierarchical equations of motion theory, with the capability of accurate evaluation for both reduced system and hybrid bath dynamics. The underlying dissipaton algebra includes the generalized Wick’s theorem and DEOM-space techniques for hybrid bath dynamics. Methods discussed also involve an efficient derivative–resum level truncation scheme that preserves the prescription invariance, and the mixed Heisenberg–Schrödinger picture approach for efficient simulation of nonlinear response functions. Our model simulations show clearly the correlated system-and-bath interference and the resulting Fano entanglement spectroscopy profiles.