Parametrization of Nonbonded Force Field Terms for Metal–Organic Frameworks Using Machine Learning Approach

The enormous structural and chemical diversity of metal–organic frameworks (MOFs) forces researchers to actively use simulation techniques as often as experiments. MOFs are widely known for their outstanding adsorption properties, so a precise description of the host–guest interactions is essential for high-throughput screening aimed at ranking the most promising candidates. However, highly accurate ab initio calculations cannot be routinely applied to model thousands of structures due to the demanding computational costs. Furthermore, methods based on force field (FF) parametrization suffer from low transferability. To resolve this accuracy–efficiency dilemma, we applied a machine learning (ML) approach: extreme gradient boosting. The trained models reproduced the atom-in-material quantities, including partial charges, polarizabilities, dispersion coefficients, quantum Drude oscillator, and electron cloud parameters, with accuracy similar to the reference data set. The aforementioned FF precursors make it possible to thoroughly describe noncovalent interactions typical for MOF–adsorbate systems: electrostatic, dispersion, polarization, and short-range repulsion. The presented approach can also readily facilitate hybrid atomistic simulation/ML workflows.