Simple position and orientation preconditioning scheme for minimum energy path calculations

Minimum-energy path (MEP) calculations, such as those typified by the nudged elastic band method, require input of reactant and product molecular configurations at initialization. In the case of reactions involving more than one molecule, generating initial reactant and product configurations requires careful consideration of the relative position and orientations of the reactive molecules in order to ensure that the resulting MEP calculation proceeds without converging on an alternative reaction-path, and without requiring excessive numbers of optimization iterations; as such, this initial system set-up is most commonly performed by hand, with an expert user arranging reactive molecules in space to ensure that the following MEP calculation runs smoothly. In this Article, we introduce a simple preconditioning scheme which replaces this labor-intensive, human-knowledge-based step with an automated deterministic computational scheme. In our approach, initial reactant and product configurations are generated such that steric hindrance between reactive molecules is minimized in the reactant and product configurations, while also simultaneously requiring minimal structural differences between the reactants and products. The method is demonstrated using a benchmark test-set of >3400 organic molecular reactions, where comparison of the reactant/product configurations generated using our approach compare very well to initial configurations which were generated on an ad hoc basis.

Automated summary

This article introduces a simple preconditioning scheme to replace the labor-intensive, human-knowledge-based step of setting up initial reactant and product configurations with an automated deterministic computational scheme. The method minimizes steric hindrance between reactive molecules and minimizes structural differences between reactants and products, providing an efficient way for MEP calculations.