KVIK Optimiser - An Enhanced ReaxFF Force Field Training Approach


In this work, we demonstrate the superior exploration capabilities of the population-based methods over the sequential one-parameter parabolic interpolation (SOPPI) approach to optimise ReaxFF force field parameters. Evolutionary algorithms (EAs) are heuristic-based approaches using a population of concurrent models in the search space to evolve towards the global best through stochastic operations. The parallelisation of EAs scales almost linearly, and no differentiable objective function is required. These methods were tested for their search performance and convergence behaviour on different multi-dimensional, multimodal benchmark functions. The developed KVIK (Icelandic for: dynamic, in motion) optimisation framework features an extended training 1routine designed to parameterise solid-state systems efficiently. The optimisation routine was applied to train a reactive force field potential for metallic lithium and sodium and their interaction parameters. The KVIK-optimised ReaxFF potential function parameter set reproduces relative energy results from the density functional theory (DFT) reference data set within the standard deviation range established using the error estimation routine provided by the BEEF-vdW density functional. Finally, thermodynamically and kinetically driven surface growth phenomena on metallic Li- and Na-electrodes were investigated using coupled ReaxFF/Monte Carlo (MC) approaches.

Version notes

We updated the structure of the paper, removed some typos, and introduced the latest version of the force field parameter files. Further, the SI has been extended by a ReaxFF section with an overview of the used force field terms.


Supplementary material

Supporting Information
Detailed information on the implemented transition state tools for ReaxFF, extended benchmark study results, reactive force field parameters for Li-Li, Na-Na, Li-Na, and Mg-Mg, and their comparison with literature known ReaxFF parameter sets are given in the supplementary material.