Systematic coarse-graining in nucleation theory

摘要: In this work, we show that the standard method to obtain nucleation rate-predictions with aid of atomistic Monte Carlo simulations leads rate predictions deviate 3 - 5 orders magnitude from recent brute-force molecular dynamics [Diemand et al., J. Chem. Phys. 139, 074309 (2013)] conducted in experimental accessible supersaturation regime for Lennard-Jones argon. We argue is due truncated state space literature mostly relies on, where number atoms a nucleus considered only relevant order parameter. here formulate nonequilibrium statistical mechanics an extended space, internal energy and momentum nuclei are additionally incorporated. model explains lack agreement between by Diemand al. space. demonstrate additional benefits using space; particular, definition temperature arises very naturally can be shown without further approximation obey fluctuation law McGraw LaViolette. addition, illustrate our theory conveniently allows extend existing theories richer sets parameters.