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Nonclassical Nucleation in a Solid-Solid Transition of Confined Hard Spheres.

Weikai Qi1,2, Yi Peng3, Yilong Han3

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Area of Science:

  • Condensed matter physics
  • Materials science
  • Statistical mechanics

Background:

  • Phase transitions in confined systems are crucial for understanding material properties.
  • Colloidal systems offer a model for studying fundamental physical phenomena.
  • Understanding nucleation mechanisms is key to controlling material self-assembly.

Purpose of the Study:

  • To investigate the solid-solid phase transition of colloidal hard spheres confined between planar walls.
  • To elucidate the nucleation mechanism governing the transition from a five-layer square (5□) solid to a four-layer triangular (4△) solid.
  • To analyze the role of liquid phases and wall interactions in the transition process.

Main Methods:

  • Molecular dynamics (MD) simulations to model particle interactions and dynamics.
  • Monte Carlo (MC) simulations to explore phase space and calculate free energies.
  • Free-energy calculations to determine the transition pathway and barrier height.

Main Results:

  • The solid-solid transition occurs via a nonclassical nucleation mechanism.
  • A precritical liquid cluster forms first, followed by the growth of the stable 4△ solid phase within the liquid.
  • The critical nucleus comprises a 4△ solid cluster wetted by a metastable liquid, growing at the walls.
  • Critical nucleus size increases with supersaturation, contradicting classical nucleation theory.
  • The △-solid-like cluster exhibits both face-centered-cubic (FCC) and hexagonal-close-packed (HCP) ordering.

Conclusions:

  • The transition is a one-step process with a single free-energy barrier.
  • Wall interactions significantly influence the nucleation and growth of solid phases.
  • The observed nucleation mechanism deviates from classical theories, highlighting the complexity of confined phase transitions.