A critical look at methods for calculating charge transfer couplings fast and accurately

TL;DR

This paper critically reviews methods for calculating charge transfer couplings, focusing on Density Functional Theory and related approaches, assessing their regimes, strengths, weaknesses, and providing practical guidance for the FDE-ET method.

Contribution

It offers a comprehensive critical assessment of charge transfer coupling methods and introduces a practical protocol for the FDE-ET approach.

Findings

Assessment of regimes suitable for different methods

Identification of strengths and weaknesses of each method

Provision of a practical protocol for FDE-ET calculations

Abstract

We present here a short and subjective review of methods for calculating charge transfer couplings. Although we mostly focus on Density Functional Theory, we discuss a small subset of semiempirical methods as well as the adiabatic-to-diabatic transformation methods typically coupled with wavefunction-based electronic structure calculations. In this work, we will present the reader with a critical assessment of the regimes that can be modeled by the various methods their strengths and weaknesses. In order to give a feeling about the practical aspects of the calculations, we also provide the reader with a practical protocol for running coupling calculations with the recently developed FDE-ET method.