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

Lee S, Teich EG, Engel M, Glotzer SC (2019)

Publication Type: Journal article

Publication year: 2019

Journal

Proceedings of the National Academy of Sciences of the United States of America National Academy of Sciences

Book Volume: 116

Pages Range: 14843-14851

Journal Issue: 30

DOI: 10.1073/pnas.1905929116

Abstract

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. Our results establish the existence of complex crystallization pathways in entropic systems and reveal prenucleation motifs of various dimensions.

Authors with CRIS profile

Michael Engel Professur für Modellierung von Selbstorganisationsprozessen

Involved external institutions

University of Michigan US United States (USA) (US)

How to cite

APA:

Lee, S., Teich, E.G., Engel, M., & Glotzer, S.C. (2019). Entropic colloidal crystallization pathways via fluid–fluid transitions and multidimensional prenucleation motifs. Proceedings of the National Academy of Sciences of the United States of America, 116(30), 14843-14851. https://doi.org/10.1073/pnas.1905929116

MLA:

Lee, Sangmin, et al. "Entropic colloidal crystallization pathways via fluid–fluid transitions and multidimensional prenucleation motifs." Proceedings of the National Academy of Sciences of the United States of America 116.30 (2019): 14843-14851.

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