Advancing Hierarchical Equations of Motion for E±cient Evaluation of Coherent Two-dimensional Spectroscopy

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