Advancing hierarchical equations of motion for efficient evaluation of coherent two-dimensional spectroscopy

TL;DR

This paper introduces an improved hierarchical equations of motion method with a mixed Heisenberg-Schrodinger scheme and numerical filtering, enabling efficient simulation of coherent two-dimensional spectroscopy in excitonic systems.

Contribution

It develops a novel mixed Heisenberg-Schrodinger approach with block-matrix implementation and filtering, enhancing the efficiency of quantum dissipative dynamics simulations.

Findings

Analyzed effects of transfer coupling and bi-exciton interaction on spectroscopy.

Demonstrated improved computational efficiency for excitonic dimer models.

Validated the method's capability to simulate complex nonlinear optical responses.

Abstract

To advance hierarchial equations of motion as a standard theory for quantum dissipative dynamics, we put forward a mixed Heisenberg--Schrodinger scheme with block-matrix implementation on efficient evaluation of nonlinear optical response function. The new approach is also integrated with optimized hierarchical theory and numerical filtering algorithm. Different configurations of coherent two-dimensional spectroscopy of model excitonic dimer systems are investigated, with focus on the effects of intermolecular transfer coupling and bi-exciton interaction.