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Spontaneous Crystallization in Systems of Binary Hard Sphere Colloids.

Praveen K Bommineni1, Marco Klement1, Michael Engel1

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Binary hard sphere crystals, previously unconfirmed by simulations, have now been successfully grown. This study analyzes crystallization kinetics and presents phase diagrams for binary crystal stability.

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Area of Science:

  • Computational physics and chemistry
  • Materials science
  • Statistical mechanics

Background:

  • Computer simulations are crucial for understanding fluid-to-solid phase transitions in hard sphere systems.
  • Despite theoretical predictions and experimental evidence for binary hard sphere crystals, simulations have historically failed to confirm their stability.

Purpose of the Study:

  • To report the direct simulation of binary hard sphere crystal growth from a fluid.
  • To analyze the kinetics of crystallization for specific binary crystal structures.
  • To map the stability regions of these binary crystals using packing fraction and size ratio.

Main Methods:

  • Event-driven molecular dynamics simulations were employed to model the hard sphere system.
  • Simulations were conducted both with and without swap moves to accelerate diffusion and observe crystallization.
  • Analysis focused on particle kinetics during crystal growth and the construction of state diagrams.

Main Results:

  • Successfully simulated the growth of binary hard sphere crystals isostructural to Laves phases, AlB2, and NaZn13 directly from the fluid.
  • Observed a transition in the crystallization process from nucleation and growth to spinodal decomposition within the fluid-solid coexistence regime.
  • Generated packing fraction-size ratio state diagrams illustrating the stability regions of the studied binary crystals.

Conclusions:

  • This work overcomes previous simulation limitations, confirming the stability of binary hard sphere crystals.
  • The findings provide new insights into crystallization dynamics and the phase behavior of binary hard sphere systems.
  • The presented state diagrams are valuable for predicting and understanding binary crystal formation.