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Influence of Nonadditive Mixing on Colloidal Diamond Phase Formation from Patchy Particles
Isabela Quintela Matos1, Fernando A Escobedo1
1R. F. Smith School of Chemical and Biomolecular Engineering, Cornell University, Ithaca, New York 14853, United States.
The Journal of Physical Chemistry. B
|April 14, 2023
Summary
Nonadditive mixing in nanoparticle (NP) systems enhances diamond phase formation. Molecular simulations reveal kinetic boosts for self-assembly, driven by packing density and interfacial free energy.
Area of Science:
- Colloidal science
- Materials science
- Computational chemistry
Background:
- Nanoparticle (NP) mixtures with DNA-grafted strands enable tunable NP-NP interactions.
- Nonadditive mixing, known in molecular fluids, is less studied in NP self-assembly.
- Understanding nonadditive mixing is key to designing complex NP materials.
Purpose of the Study:
- Explore nonadditive mixing effects in binary systems of tetrahedral patchy NPs.
- Investigate the self-assembly behavior of NPs interacting via DNA hybridization.
- Analyze the influence of nonadditivity on phase transitions and kinetics.
Main Methods:
- Utilized molecular simulations for a binary NP system.
- Modeled tetrahedral patchy NPs with raised patches and DNA hybridization interactions.
- Employed a coarse-grained interparticle potential to represent DNA hybridization.
Main Results:
- Patchy NPs spontaneously nucleated into the diamond phase.
- Hard NP cores suppressed competition between diamond and BCC phases.
- Higher nonadditivity showed minor phase behavior effects but kinetically enhanced diamond phase formation.
Conclusions:
- Nonadditive mixing kinetically promotes the diamond phase in NP self-assembly.
- Phase packing densities and interfacial free energy modulation explain kinetic enhancement.
- This work provides insights into designing complex self-assembled NP structures.
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