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Tuning Stoichiometry to Promote Formation of Binary Colloidal Superlattices

R. Allen LaCour, Timothy C. Moore, and Sharon C. Glotzer
Phys. Rev. Lett. 128, 188001 – Published 2 May 2022
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Abstract

The self-assembly of binary nanoparticle superlattices from colloidal mixtures is a promising method for the fabrication of complex colloidal cocrystal structures. However, binary mixtures often form amorphous or metastable phases instead of the thermodynamically stable phase. Here we show that in binary mixtures of differently sized spherical particles, an excess of the smaller component can promote—and, in some cases, may be necessary for—the self-assembly of a binary cocrystal. Using computer simulations, we identify two mechanisms responsible for this phenomenon. First, excess small particles act like plasticizers and enable systems to reach a greater supersaturation before kinetic arrest occurs. Second, they can disfavor competing structures that may interfere with the growth of the target structure. We find the phase behavior of simulated mixtures of nearly hard spheres closely matches published experimental results. We demonstrate the generality of our findings for mixtures of particles of arbitrary shape by presenting a binary mixture of hard shapes that only self-assembles with an excess of the smaller component.

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  • Received 11 December 2021
  • Revised 27 March 2022
  • Accepted 31 March 2022

DOI:https://doi.org/10.1103/PhysRevLett.128.188001

© 2022 American Physical Society

Physics Subject Headings (PhySH)

Polymers & Soft Matter

Authors & Affiliations

R. Allen LaCour, Timothy C. Moore, and Sharon C. Glotzer*

  • Department of Chemical Engineering, The University of Michigan, Ann Arbor, Michigan 48109, USA Biointerfaces Institute, The University of Michigan, Ann Arbor, Michigan 48109, USA

  • *sglotzer@umich.edu

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Issue

Vol. 128, Iss. 18 — 6 May 2022

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