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Unlike ionic or small covalent molecules, polymers do not form crystalline solids due to the diffusion limitations of their long-chain structures. However, polymers contain microscopic crystalline domains separated by amorphous domains.
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Compositional fluctuations and polymorph selection in crystallization of model soft colloids.

Abhilasha Kumari1, Gadha Ramesh2, Debasish Koner3

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Controlling material properties relies on understanding polymorph selection. This study reveals how tuning thermodynamic conditions influences crystal phase transitions, enabling targeted material design.

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Area of Science:

  • Materials Science
  • Physical Chemistry
  • Computational Chemistry

Background:

  • Polymorph selection is crucial for designing targeted materials.
  • Controlling crystallization pathways is a significant challenge in materials science.

Purpose of the Study:

  • Investigate the control of polymorph selection in atomic and molecular systems.
  • Explore the mechanisms underlying polymorph selection by tuning thermodynamic parameters.

Main Methods:

  • Utilized Monte Carlo simulations on Gaussian core and hard-core Yukawa colloidal systems.
  • Employed supervised machine learning with topological data analysis (persistent homology) for structural analysis.

Main Results:

  • Demonstrated control over polymorph selection by modifying the free energy landscape, shifting dominance from face-centered cubic (FCC) to body-centered cubic (BCC) phases.
  • Observed an intermediate regime with selective or competitive nucleation of both phases, leading to critical composition fluctuations.
  • Identified an interpenetrating arrangement of FCC- and BCC-like particles near the fluid-BCC-FCC triple point, deviating from typical two-step nucleation.

Conclusions:

  • Insights into controlling crystallization pathways can aid in obtaining desired functional materials.
  • Machine learning approach effectively identifies polymorph selection signatures in metastable fluids.