Department of Chemistry, School of Biological and Chemical Sciences, Queen Mary University of London, London, UK.
J Comput Chem. 2020 Apr 15;41(10):1045-1058. doi: 10.1002/jcc.26144. Epub 2020 Jan 7.
The study of photoexcitations in molecular aggregates faces the twofold problem of the increased computational cost associated with excited states and the complexity of the interactions among the constituent monomers. A mechanistic investigation of these processes requires the analysis of the intermolecular interactions, the effect of the environment, and 3D arrangements or crystal packing on the excited states. A considerable number of techniques have been tailored to navigate these obstacles; however, they are usually restricted to in-house codes and thus require a disproportionate effort to adopt by researchers approaching the field. Herein, we present the FRamewOrk for Molecular AGgregate Excitations (fromage), which implements a collection of such techniques in a Python library complemented with ready-to-use scripts. The program structure is presented and the principal features available to the user are described: geometrical analysis, exciton characterization, and a variety of ONIOM schemes. Each is illustrated by examples of diverse organic molecules in condensed phase settings. The program is available at https://github.com/Crespo-Otero-group/fromage.
分子聚集体中光激发的研究面临着与激发态相关的计算成本增加以及组成单体之间相互作用复杂性的双重问题。这些过程的机理研究需要分析分子间相互作用、环境的影响以及 3D 排列或晶体堆积对激发态的影响。已经开发了相当多的技术来克服这些障碍；然而，它们通常仅限于内部代码，因此对于接近该领域的研究人员来说，采用这些技术需要付出不成比例的努力。在这里，我们提出了用于分子聚集体激发的 FRamewOrk（fromage），它在一个 Python 库中实现了这些技术的集合，并配有现成的脚本。本文介绍了程序结构，并描述了用户可用的主要功能：几何分析、激子特征化和各种 ONIOM 方案。每个方案都通过凝聚相环境中各种有机分子的实例进行了说明。该程序可在 https://github.com/Crespo-Otero-group/fromage 获得。
