From Many-Body Ab Initio to Effective Excitonic Models: A Versatile Mapping Approach Including Environmental Embedding Effects

IF 5.7 1区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Chemical Theory and Computation Pub Date : 2024-09-18 DOI:10.1021/acs.jctc.4c00756

Mauricio Rodriguez-Mayorga, Xavier Blase, Ivan Duchemin, Gabriele D’Avino

引用次数: 0

Abstract

We present an original multistate projective diabatization scheme based on Green’s function formalisms that allows the systematic mapping of many-body ab initio calculations onto effective excitonic models. This method inherits the ability of the Bethe–Salpeter equation to describe Frenkel molecular excitons and intermolecular charge-transfer states equally well, as well as the possibility for an effective description of environmental effects in a QM/MM framework. The latter is found to be a crucial element in order to obtain accurate model parameters for condensed phases and to ensure their transferability to excitonic models for extended systems. The method is presented through a series of examples illustrating its quality, robustness, and internal consistency.

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从多体 Ab Initio 到有效激子模型：包括环境嵌入效应的多功能映射方法

我们提出了一种基于格林函数形式的原创性多态投影二重化方案，它允许将多体 ab initio 计算系统地映射到有效的激子模型上。这种方法继承了 Bethe-Salpeter 方程对 Frenkel 分子激子和分子间电荷转移态进行同等描述的能力，以及在 QM/MM 框架内对环境效应进行有效描述的可能性。为了获得凝聚相的精确模型参数，并确保这些参数能够转移到扩展系统的激子模型中，我们发现后者是一个关键因素。该方法通过一系列实例展示，说明了其质量、稳健性和内部一致性。

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Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere.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.