Reaction streams in overall gas-phase chemical reactions.

The phase space data produced in molecular dynamics (MD) simulations of many-atom systems contain complete classical descriptions of the processes determined by the force field for the specific initial conditions. The usefulness of the simulation results comes from gleaning physically meaningful information from the mass of phase space points. This is especially difficult in the case of chemical reactions in bulk phases. Determining the major pathways from reactants to products directly from MD simulation results and without assuming a given mechanism is particularly challenging. We propose the reaction stream method based on the cluster representation for gases to identify, directly from MD simulations, the sequences of isolated reactions that are responsible for progress of the overall chemistry in complex reactions. The goal is to obviate the need for pre-convinced mechanisms to characterize the overall chemistry. To illustrate the applicability of the reaction stream method, we identify the dominant reaction pathways for the dissociation of H₂O₂ in MD simulations with the ReaxFF force field. The significance of rare reaction pathways to predict the progress of the evolving chemistry is also studied. [ABSTRACT FROM AUTHOR]