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Updated: May 28, 2026

Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids
Published on: May 27, 2020
Optimized hierarchical equations of motion theory for Drude dissipation and efficient implementation to nonlinear
Jin-Jin Ding1, Jian Xu, Jie Hu
1Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China.
Abstract:
Hierarchical equations of motion theory for Drude dissipation is optimized, with a convenient convergence criterion proposed in advance of numerical propagations. The theoretical construction is on the basis of a Padé spectrum decomposition that has been qualified to be the best sum-over-poles scheme for quantum distribution function. The resulting hierarchical dynamics under the a priori convergence criterion are exemplified with a benchmark spin-boson system, and also the transient absorption and related coherent two-dimensional spectroscopy of a model exciton dimer system. We combine the present theory with several advanced techniques such as the block hierarchical dynamics in mixed Heisenberg-Schrödinger picture and the on-the-fly filtering algorithm for the efficient evaluation of third-order optical response functions.
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