We analyze the fundamental process of crystallization of silicon nanoclusters by means of molecular dynamics simulations, complemented by magnetron-sputter inert gas condensation, which was used to synthesize polycrystalline silicon nanoclusters with good size control. We utilize two well-established Si interatomic potentials: the Stillinger-Weber and the Tersoff III. Both the simulations and experiments show that upon cooling down by an Ar gas thermal bath, initially liquid, free-standing Si nanocluster can grow multiple crystal nuclei, which drive their transition into polycrystalline solid nanoclusters. The simulations allow detailed analysis of the mechanism, and show that the crystallization temperature is size-dependent and that the probability of crystalline phase nucleation depends on the highest temperature the cluster reaches during the initial condensation and the cooling rate after it.
|Physical Review B - Condensed Matter and Materials Physics
|Published - 15 Jan 2015