Classical density functional theory: an ideal tool to study heterogeneous crystal nucleation.

Area of Science:

• Computational Physics
• Materials Science
• Chemical Physics

Background:

• Freezing and crystallization are fundamental processes in condensed matter physics and materials science.
• Microscopic theories are needed to accurately describe these phase transitions.
• Density functional theory (DFT) offers a robust framework for such investigations.

Purpose of the Study:

• To review the application of static and dynamical density functional theory (DFT) to freezing and crystallization.
• To summarize DFT's utility in calculating equilibrium phase diagrams.
• To explore DFT's role in heterogeneous crystal nucleation and growth, and its relation to phase field crystal models.

Main Methods:

• Static density functional theory for equilibrium phase diagram calculations.
• Dynamical density functional theory for systems with overdamped Brownian dynamics.
• Detailed analysis of heterogeneous nucleation, including a 2D dipolar system example.

Main Results:

• DFT effectively predicts equilibrium phase diagrams.
• Dynamical DFT accurately models crystallization processes governed by Brownian motion.
• Heterogeneous nucleation and crystal growth are well-described by DFT, particularly at imposed nucleation sites.

Conclusions:

• Density functional theory is a versatile and powerful tool for studying freezing and crystallization phenomena.
• Both static and dynamical DFT approaches provide valuable insights into phase behavior and crystal formation.
• The connection between dynamical DFT and phase field crystal models offers further avenues for research.