Entropic colloidal crystallization pathways via fluid–fluid transitions and multidimensional prenucleation motifs

Lee, Sangmin; Teich, Erin G.; Engel, Michael; Glotzer, Sharon C.

doi:10.1073/pnas.1905929116

Title: Entropic colloidal crystallization pathways via fluid–fluid transitions and multidimensional prenucleation motifs

Journal Article · Mon Jul 08 00:00:00 EDT 2019 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1905929116· OSTI ID:1610454

^[1]; Teich, Erin G. ^[1]; Engel, Michael ^[2]; Glotzer, Sharon C. ^[1]

Univ. of Michigan, Ann Arbor, MI (United States)
Univ. of Michigan, Ann Arbor, MI (United States); Friedrich-Alexander Univ. Erlangen-Nurnberg (Germany)

Complex crystallization pathways are common in protein crystallization, tetrahedrally coordinated systems, and biomineralization, where single or multiple precursors temporarily appear before the formation of the crystal. The emergence of precursors is often explained by a unique property of the system, such as short-range attraction, directional bonding, or ion association. But, structural characteristics of the prenucleation phases found in multistep crystallization remain unclear, and models are needed for testing and expanding the understanding of fluid-to-solid ordering pathways. Here, we report 3 instances of 2-step crystallization of hard-particle fluids. Crystallization in these systems proceeds via a high-density precursor fluid phase with prenucleation motifs in the form of clusters, fibers and layers, and networks, respectively. The density and diffusivity change across the fluid–fluid phase transition increases with motif dimension. We observe crystal nucleation to be catalyzed by the interface between the 2 fluid phases. The crystals that form are complex, including, notably, a crystal with 432 particles in the cubic unit cell. Finally, our results establish the existence of complex crystallization pathways in entropic systems and reveal prenucleation motifs of various dimensions.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Energy Science (CBES); Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); DGE 1256260; ACI-1053575

Grant/Contract Number:: SC0000989; DMR 1409620

OSTI ID:: 1610454

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Vol. 116, Issue 30; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 34 works

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