Homogeneous crystallization in four-dimensional Lennard-Jones liquids

Area of Science:

• Physics
• Materials Science
• Computational Chemistry

Background:

• Crystallization in supercooled liquids is a fundamental process in materials science.
• The effect of spatial dimension (d) on crystallization is a key area of research, with geometrical frustration hypothesized to suppress crystallization as d increases.
• Previous studies often focused on systems with short-ranged interactions or lower dimensions.

Purpose of the Study:

• To investigate homogeneous crystallization in high-dimensional (d>3) liquids with realistic dynamics.
• To determine the role of long-ranged attractive interactions in high-dimensional crystallization.
• To test the hypothesis that increasing geometrical frustration suppresses crystallization with increasing spatial dimension.

Main Methods:

• Simulated supercooled four-dimensional (4D) Lennard-Jones (LJ) liquids at zero pressure and temperatures 0.59
• Simulated Weeks-Chandler-Andersen (WCA) liquids under identical conditions to isolate the effect of attractive interactions.
• Analysis of crystallization kinetics and local-bond-order distributions.

Main Results:

• Homogeneous crystallization was observed in 4D LJ liquids within ~2x10^4 tau.
• WCA liquids (lacking long-ranged attraction) did not crystallize even after 2.5x10^5 tau.
• The overlap between liquid and crystalline phases was smaller for LJ than WCA systems in 4D, contrasting the 3D trend.

Conclusions:

• Long-ranged attractive interactions significantly accelerate crystallization in 4D liquids.
• The hypothesis that increasing geometrical frustration suppresses crystallization with dimension is only generally valid for systems without attractive forces.
• This study highlights the importance of interparticle interactions in high-dimensional crystallization phenomena.