Best‐Practice DFT Protocols for Basic Molecular Computational Chemistry**

2022/09/14 by Markus Bursch, Jan‐Michael Mewes, Andreas Hansen +1 · 26 citations
Chemistry · Engineering · Physics and Astronomy · #Advanced Chemical Physics Studies #Chemical Reactions and Mechanisms #Molecular Junctions and Nanostructures

paper · doi:10.1002/anie.202205735

openalex publication_date 2022/09/14 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/31

Abstract

Nowadays, many chemical investigations are supported by routine calculations of molecular structures, reaction energies, barrier heights, and spectroscopic properties. The lion's share of these quantum-chemical calculations applies density functional theory (DFT) evaluated in atomic-orbital basis sets. This work provides best-practice guidance on the numerous methodological and technical aspects of DFT calculations in three parts: Firstly, we set the stage and introduce a step-by-step decision tree to choose a computational protocol that models the experiment as closely as possible. Secondly, we present a recommendation matrix to guide the choice of functional and basis set depending on the task at hand. A particular focus is on achieving an optimal balance between accuracy, robustness, and efficiency through multi-level approaches. Finally, we discuss selected representative examples to illustrate the recommended protocols and the effect of methodological choices.

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