Support Vector Regression-Based Monte Carlo Simulation of Flexible Water Clusters.

Molecular simulations based on classical force fields are computationally efficient but lack accuracy due to the empirical formulation of non-bonded interactions. Quantum mechanical (QM) methods, albeit accurate, have inhibitory computational costs for large molecules and clusters. Hence, to overcome the bottleneck, machine learning (ML)-based methods have been employed in the recent years. We had earlier reported a combined scheme of many-body expansion (MBE) and ML to predict the interaction energies of rigid water clusters. In this work, we proceed toward building a flexible water model using the ML-MBE scheme. This ML-MBE scheme has an error of <1% for interaction energy prediction in comparison to the parent QM method for flexible water decamers. Machine learning-based Monte Carlo simulations (MLMC) are performed with this water model, and the structural properties of these configurations are compared with those obtained from ab initio molecular dynamics (AIMD) and the TIP3P classical force field. The radial distribution functions, tetrahedral order parameters, and number of hydrogen bonds in AIMD and MLMC have a similar qualitative and quantitative trend, whereas the classical force fields show a significant deviation.