REAXFF Reactive Force Field for Disulfide Mechanochemistry, Fitted to Multireference ab Initio Data

J Muller and B Hartke, JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 12, 3913-3925 (2016).

DOI: 10.1021/acs.jctc.6b00461

Mechanochemistry, in particular in the form of single-molecule atomic force microscopy experiments, is difficult to model theoretically, for two reasons: Covalent bond breaking is not captured accurately by single-determinant, single-reference quantum chemistry methods, and experimental times of milliseconds or longer are hard to simulate with any approach. Reactive force fields have the potential to alleviate both problems, as demonstrated in this work: Using non deterministic global parameter optimization by evolutionary algorithms, we have fitted a REAXFF force field to high-level multireference ab initio data for disulfides. The resulting force field can be used to reliably model large, multifunctional mechanochemistry units with disulfide bonds as designed breaking points. Explorative calculations show that a significant part of the time scale gap between AFM experiments and dynamical simulations can be bridged with this approach.

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