A novel method for analyzing energy relaxation in condensed phases using nonequilibrium molecular dynamics simulations: Application to the energy relaxation of intermolecular motions in liquid water

We present a novel method to investigate energy relaxation processes in condensed phases using nonequilibrium molecular dynamics simulations. This method can reveal details of the time evolution of energy relaxation like two-color third-order IR spectroscopy. Nonetheless, the computational cost of this method is significantly lower than that of third-order response functions. We apply this method to the energy relaxation of intermolecular motions in liquid water. We show that the intermolecular energy relaxation in water is characterized by four energy transfer processes. The structural changes of the liquid associated with the energy relaxation are also analyzed by the nonequilibrium molecular dynamics technique. (C) 2011 American Institute of Physics. [doi:10.1063/1.3587105]