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Structural complexity driven by liquid-liquid crystal phase separation of smectics.

Christopher A Browne1, Yuma Morimitsu1, Na Kyung Kim1

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Liquid-liquid crystal phase separation (LLCPS) creates diverse droplet structures. Solvent swelling and cooling path critically influence the formation of complex filamentous networks from smectic condensates.

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Area of Science:

  • Materials Science
  • Soft Matter Physics
  • Chemical Engineering

Background:

  • Phase separation in complex fluids can yield droplets with internal liquid crystalline order.
  • Droplet geometry is influenced by the elasticity of the internal liquid crystalline mesophase, forming structures like filaments and tactoids.
  • Previous work showed filamentous networks arise from liquid-liquid crystal phase separation (LLCPS) via slow cooling.

Purpose of the Study:

  • Investigate how mesogen, solvent, and concentration affect network structures formed by LLCPS.
  • Elucidate the role of solvent swelling and phase separation pathways on network morphology.
  • Understand conditions necessary for forming networked structures in liquid crystal systems.

Main Methods:

  • Utilized X-ray scattering to analyze the structure of smectic condensates.
  • Systematically varied mesogen, solvent, and concentration in phase-separated systems.
  • Observed droplet and network formation under controlled cooling conditions.

Main Results:

  • Solvent swelling of smectic layers reduced the bend modulus, leading to more complex network geometries.
  • Higher smectic layer swelling correlated with increased geometric complexity, requiring greater layer bending.
  • Filament and network formation was path-dependent, occurring only when the smectic phase formed directly from the isotropic phase.

Conclusions:

  • The choice of solvent and concentration significantly impacts the structural diversity of droplets formed by LLCPS.
  • Solvent-induced changes in material properties (e.g., bend modulus) are key to controlling network morphology.
  • Path-dependence, specifically the direct formation of the smectic phase from the isotropic phase, is crucial for network assembly.