A parameter-free prediction of simulated crystal nucleation times in the Lennard-Jones system: From the steady-state nucleation to the transient time regime

Abstract

Large scale simulations of crystal nucleation from the liquid are performed using the Lennard-Jones potential to determine the time required for nucleation. By considering both transient and finite-size effects, we for the first time successfully predict the nucleation time without any parameter fitting in the Lennard-Jones system. All necessary parameters are derived from separate, equilibrium simulations. At small undercoolings, large system size effects are observed. The required system size is not only determined by the size of the critical nuclei, but also the characteristic spacing between them. Two distinct nucleation regions are predicted by theory and observed by the simulations, which are dominated by the transient time and the steady-state nucleation time, respectively.