Reactive Car-Parrinello dynamics

M. Iannuzzi, A. Laio and M. Parrinello

Centro Svizzero di Calcolo Scientifico (CSCS), CH-6928 Manno

and Physical Chemistry, ETH, Hönggerberg HCI, CH-8093 Zurich, Switzerland

Ab-initio molecular dynamics is ideally suited for studying chemical processes that take place in the condensed phase. However, the short time scale of ab-initio simulations (~10ps) allows none but the fastest chemical reactions to occur spontaneously in ab-initio molecular dynamics runs. Here we present a new method that combines the ideas of the extended Lagrangean approach with coarse-grained non-Markovian metadynamics. With this new method it becomes possible to observe complex chemical reactions in short ab-initio molecular dynamics simulations and to overcome very large energy barriers.