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Self-assembly of binary space-tessellating compounds.

Mihir R Khadilkar1, Fernando A Escobedo

  • 1Department of Physics, Cornell University, Ithaca, New York 14853, USA.

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|November 28, 2012
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Binary mixtures of polyhedral nanoparticles do not spontaneously form predicted tessellated structures due to high energy barriers. Introducing attractive forces helps overcome these barriers, guiding self-assembly towards ordered materials.

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Area of Science:

  • Materials Science
  • Colloidal Science
  • Computational Chemistry

Background:

  • Self-assembly of polyhedral nanoparticles is key for novel material engineering.
  • Studying binary mixtures of tessellating particles is crucial for understanding complex structures.

Purpose of the Study:

  • Investigate the self-assembly behavior of three binary tessellating mixtures: cuboctahedra + octahedra, octahedra + tetrahedra, and truncated cubes + octahedra.
  • Determine phase behavior driven by entropic forces (hard-core interactions).
  • Explore methods to overcome kinetic barriers for spontaneous ordering.

Main Methods:

  • Monte Carlo simulations to determine phase behavior.
  • Interfacial simulations to assess metastability.
  • Polybead models to study the effect of enthalpic interactions.

Main Results:

  • None of the studied mixtures spontaneously ordered into tessellated structures under entropic conditions.
  • Mixtures 1 and 2 formed metastable glassy states.
  • Mixture 3 demixed into disordered and unusual ordered phases.
  • Favorable enthalpic interactions were shown to overcome free-energy barriers for nucleation.

Conclusions:

  • Self-assembly of binary tessellating polyhedral particles is kinetically hindered by large free-energy barriers.
  • Overcoming these barriers requires specific enthalpic interactions, not just entropy.
  • Results provide insights into the "chemistry" of polyhedral compounds and their self-assembly pathways.