Liu Zengkui, Brian Dominikus, Sun Xiang
Shanghai Frontiers Science Center of Artificial Intelligence and Deep Learning, NYU Shanghai, 567 West Yangsi Road, Shanghai 200124, China.
Division of Arts and Sciences, NYU Shanghai, 567 West Yangsi Road, Shanghai 200124, China.
J Chem Phys. 2024 Aug 14;161(6). doi: 10.1063/5.0224524.
In this work, we introduce PyCTRAMER, a comprehensive Python package designed for calculating charge transfer (CT) rate constants in disordered condensed-phase systems at finite temperatures, such as organic photovoltaic (OPV) materials. PyCTRAMER is a restructured and enriched version of the CTRAMER (Charge-Transfer RAtes from Molecular dynamics, Electronic structure, and Rate theory) package [Tinnin et al. J. Chem. Phys. 154, 214108 (2021)], enabling the computation of the Marcus CT rate constant and the six levels of the linearized semiclassical approximations of Fermi's golden rule (FGR) rate constant. It supports various types of intramolecular and intermolecular CT transitions from the excitonic states to CT state. Integrating quantum chemistry calculations, all-atom molecular dynamics (MD) simulations, spin-boson model construction, and rate constant calculations, PyCTRAMER offers an automatic workflow for handling photoinduced CT processes in explicit solvent environments and interfacial CT in amorphous donor/acceptor blends. The package also provides versatile tools for individual workflow steps, including electronic state analysis, state-specific force field construction, MD simulations, and spin-boson model construction from energy trajectories. We demonstrate the software's capabilities through two examples, highlighting both intramolecular and intermolecular CT processes in prototypical OPV systems.
在这项工作中，我们介绍了PyCTRAMER，这是一个全面的Python软件包，旨在计算有限温度下无序凝聚相系统中的电荷转移（CT）速率常数，例如有机光伏（OPV）材料。PyCTRAMER是CTRAMER（基于分子动力学、电子结构和速率理论的电荷转移速率）软件包[Tinnin等人，《化学物理杂志》154, 214108 (2021)]的重构和丰富版本，能够计算马库斯CT速率常数以及费米黄金规则（FGR）速率常数的六级线性化半经典近似值。它支持从激子态到CT态的各种类型的分子内和分子间CT跃迁。PyCTRAMER集成了量子化学计算、全原子分子动力学（MD）模拟、自旋玻色子模型构建和速率常数计算，提供了一个自动工作流程，用于处理明确溶剂环境中的光致CT过程以及非晶态供体/受体共混物中的界面CT。该软件包还为各个工作流程步骤提供了通用工具，包括电子态分析、特定态力场构建、MD模拟以及从能量轨迹构建自旋玻色子模型。我们通过两个示例展示了该软件的功能，突出了典型OPV系统中的分子内和分子间CT过程。
