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

Area of Science:

• Computational Chemistry
• Materials Science
• Nanotechnology

Background:

• Mechanochemistry, particularly single-molecule atomic force microscopy (AFM), faces theoretical modeling challenges.
• Accurate simulation of covalent bond breaking and long experimental timescales (milliseconds+) is difficult with standard quantum chemistry methods.

Purpose of the Study:

• To develop a reliable computational approach for mechanochemistry simulations.
• To address limitations in modeling covalent bond dynamics and experimental time scales in mechanochemical processes.

Main Methods:

• Fitting a reaxFF reactive force field using evolutionary algorithms and high-level multireference ab initio data for disulfides.
• Utilizing nondeterministic global parameter optimization for force field development.
• Applying the developed force field to model large, multifunctional mechanochemistry units.

Main Results:

• The fitted reaxFF force field accurately models mechanochemistry involving disulfide bonds as breaking points.
• The approach successfully bridges the time scale gap between AFM experiments and dynamical simulations.
• Demonstrated reliability in modeling complex mechanochemical systems.

Conclusions:

• Reactive force fields, optimized with advanced computational techniques, offer a viable solution for mechanochemistry modeling.
• This method enhances the ability to simulate and understand complex chemical reactions under mechanical force.
• The developed force field provides a powerful tool for designing and predicting the behavior of mechanochemical systems.