Hierarchical Equations of Motion in Matrix Product States: Formalism and Applications for Charge Transport.

IF 5.5 1区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Chemical Theory and Computation Pub Date : 2025-10-16 DOI:10.1021/acs.jctc.5c01385

Hengrui Yang,Zirui Sheng,Liqi Zhou,Zhigang Shuai

引用次数: 0

Abstract

We present a Hierarchical Equations of Motion (HEOM) approach in the Matrix Product State (MPS) formalism to simulate carrier transport in molecular aggregates described by an electron-phonon Hamiltonian with bosonic dissipation. Transport properties are evaluated through time-dependent population analysis and mobility calculations. The method's validity is rigorously established through benchmarking against conventional HEOM. Comparative analysis with Thermo-Field Dynamics combined with MPS (TFD + MPS) reveals fundamental similarities and differences in their effective Hamiltonians and demonstrates the superior accuracy and computational efficiency of our HEOM + MPS framework. For single-electron systems, we introduce state-vector space configurations that enhance performance beyond traditional Fock space approaches. Results confirm that our method provides a robust, nearly exact, and efficient numerical quantum dynamic approach for carrier transport in dissipative bosonic environments.

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矩阵积态的层次运动方程：形式主义及其在电荷输运中的应用。

我们提出了一种矩阵积态（MPS）形式下的层次运动方程（HEOM）方法来模拟分子聚集体中载流子的输运，该输运由具有玻色子耗散的电子-声子哈密顿量描述。通过随时间变化的人口分析和流动性计算来评估运输特性。通过对传统HEOM的基准测试，严格验证了该方法的有效性。与热场动力学结合MPS （TFD + MPS）的比较分析揭示了它们有效哈密顿量的基本异同，并证明了我们的HEOM + MPS框架具有优越的精度和计算效率。对于单电子系统，我们引入了超越传统Fock空间方法的状态向量空间配置，以提高性能。结果证实，我们的方法为耗散玻色子环境中的载流子输运提供了一种鲁棒、接近精确和有效的数值量子动力学方法。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Journal of Chemical Theory and Computation 化学-物理：原子、分子和化学物理

CiteScore

9.90

自引率

16.40%

发文量

568

审稿时长

1 months

期刊介绍： The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.