Learn on the fly:: A hybrid classical and quantum-mechanical molecular dynamics simulation -: art. no. 175503

We describe and test a novel molecular dynamics method which combines quantum-mechanical embedding and classical force model optimization into a unified scheme free of the boundary region, and the transferability problems which these techniques, taken separately, involve. The scheme is based on the idea of augmenting a unique, simple parametrized force model by incorporating in it, at run time, the quantum-mechanical information necessary to ensure accurate trajectories. The scheme is tested on a number of silicon systems composed of up to similar to200 000 atoms.