Accelerated lignocellulosic molecule adsorption structure determination

Abstract: Here, we present a study combining Bayesian optimisation structural inference with the machine learning interatomic potential NequIP to accelerate and enable the study of the adsorption of the conformationally flexible lignocellulosic molecules $\beta$-D-xylose and 1,4-$\beta$-D-xylotetraose on a copper surface. The number of structure evaluations needed to map out the relevant potential energy surfaces are reduced by Bayesian optimisation, while NequIP minimises the time spent on each evaluation, ultimately resulting in cost-efficient and reliable sampling of large systems and configurational spaces. Although the applicability of Bayesian optimisation for the conformational analysis of the more flexible xylotetraose molecule is restricted by the sample complexity bottleneck, the latter can be effectively bypassed with external conformer search tools, such as the Conformer-Rotamer Ensemble Sampling Tool, facilitating the subsequent lower dimensional global minimum adsorption structure determination. Finally, we demonstrate the applicability of the described approach to find adsorption structures practically equivalent to the density functional theory counterparts at a fraction of the computational cost.