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Area of Science:

  • Materials Science
  • Colloid Science
  • Nanotechnology

Background:

  • Nanoparticle (NP) mixtures with grafted DNA offer tunable selectivity.
  • Nonadditive mixing, where component volumes don't sum, is rare in NP systems.
  • Systematic studies on nonadditive NP mixtures are lacking.

Purpose of the Study:

  • Investigate nonadditive mixing in patchy nanoparticle systems.
  • Explore the relationship between phase behavior and nonadditivity.
  • Design NP-NP interactions for controlled self-assembly.

Main Methods:

  • Calculated nanoparticle-nanoparticle potential of mean force (PMF).
  • Quantified nonadditivity using a nonadditive parameter.
  • Simulated self-assembly of one-patch and two-patch NP mixtures.

Main Results:

  • One-patch NPs primarily formed lamellar morphologies.
  • Two-patch NP mixtures exhibited rich phase behavior (gyroid, cylinder, honeycomb, layered crystal).
  • Phase behavior depended on patch-patch angle and degree of nonadditivity.

Conclusions:

  • Tunable protrusion in patchy NPs enables controlled nonadditivity.
  • Minimum positive nonadditivity and multivalent interactions are crucial for network mesophases.
  • This work provides a framework for designing complex NP self-assembly.