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

Journal article


Publication Details

Author(s): Lee S, Teich EG, Engel M, Glotzer SC
Journal: Proceedings of the National Academy of Sciences of the United States of America
Publication year: 2019
Volume: 116
Journal issue: 30
Pages range: 14843-14851
ISSN: 0027-8424
eISSN: 1091-6490


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.


FAU Authors / FAU Editors

Engel, Michael Prof. Dr.
Juniorprofessur für Modellierung von Selbstorganisationsprozessen


External institutions with authors

University of Michigan


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://dx.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.

BibTeX: 

Last updated on 2019-07-08 at 10:38