Time‐ and frequency‐resolved optical signals provide insights into the properties of light‐harvesting molecular complexes, including excitation energies, dipole strengths and orientations, as well as in the exciton energy flow through the complex. The hierarchical equations of motion (HEOM) provide a unifying theory, which allows one to study the combined effects of system‐environment dissipation and non‐Markovian memory without making restrictive assumptions about weak or strong couplings or separability of vibrational and electronic degrees of freedom. With increasing system size the exact solution of the open quantum system dynamics requires memory and compute resources beyond a single compute node. To overcome this barrier, we developed a scalable variant of HEOM. Our distributed memory HEOM, DM‐HEOM, is a universal tool for open quantum system dynamics. It is used to accurately compute all experimentally accessible time‐ and frequency‐resolved processes in light‐harvesting molecular complexes with arbitrary system‐environment couplings for a wide range of temperatures and complex sizes. © 2018 Wiley Periodicals, Inc.

中文翻译：

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使用分布式内存 HEOM (DM-HEOM) 高效计算开放量子系统动力学和时间分辨光谱

时间和频率分辨光信号提供了对光捕获分子复合物特性的洞察，包括激发能、偶极子强度和取向，以及通过复合物的激子能量流。分层运动方程 (HEOM) 提供了一种统一理论，它允许人们研究系统-环境耗散和非马尔可夫记忆的组合效应，而无需对弱耦合或强耦合或振动和电子自由度的可分离性做出限制性假设。随着系统规模的增加，开放量子系统动力学的精确解决方案需要超出单个计算节点的内存和计算资源。为了克服这个障碍，我们开发了一个可扩展的 HEOM 变体。我们的分布式内存 HEOM、DM-HEOM、是开放量子系统动力学的通用工具。它用于准确计算具有任意系统-环境耦合的光捕获分子复合物中所有可通过实验获得的时间和频率分辨过程，适用于各种温度和复杂尺寸。© 2018 Wiley Periodicals, Inc.