Freezing of a Lennard-Jones Fluid: From Nucleation to Spinodal Regime
Year: 2006
Type: article
Abstract: Using molecular dynamics, we investigate the crystal nucleation in a Lennard-Jones fluid as a function of the degree of supercooling. At moderate supercooling, a nucleation picture applies, while for deeper quenches, the phenomenon progressively acquires a spinodal character. We show that in the nucleation regime, the freezing is a two-step process. The formation of the critical nucleus is indeed preceded by the abrupt formation of a precritical crystallite from a density fluctuation in the fluid. In contrast, as the degree of supercooling is increased, crystallization proceeds in a more continuous and collective fashion and becomes more spatially diffuse, indicating that the liquid is unstable and crystallizes by a spinodal mechanism.
Source: Physical Review Letters
Institution: ETH Zurich
Language: English
Subfield: Physical and Theoretical Chemistry
Field: Chemistry
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W2033858596