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Title: Entropic formation of a thermodynamically stable colloidal quasicrystal with negligible phason strain

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3];  [4]; ORCiD logo [5]
  1. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering; Univ. of Michigan, Ann Arbor, MI (United States).
  2. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering
  3. Univ. of Michigan, Ann Arbor, MI (United States). Applied Physics Program
  4. Freidrich Alexander Univ. Erlangen-Nürnberg (FAU), Erlangen (Germany). Interdisciplinary Center for Nanostructured Films. Inst. for Multiscale Simulation
  5. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Chemical Engineering; Univ. of Michigan, Ann Arbor, MI (United States). Applied Physics Program; Univ. of Michigan, Ann Arbor, MI (United States). Biointerfaces Inst.

Quasicrystals have been discovered in a variety of materials ranging from metals to polymers. Yet, why and how they form is incompletely understood. In situ transmission electron microscopy of alloy quasicrystal formation in metals suggests an error-and-repair mechanism, whereby quasiperiodic crystals grow imperfectly with phason strain present, and only perfect themselves later into a high-quality quasicrystal with negligible phason strain. The growth mechanism has not been investigated for other types of quasicrystals, such as dendrimeric, polymeric, or colloidal quasicrystals. Soft-matter quasicrystals typically result from entropic, rather than energetic, interactions, and are not usually grown (either in laboratories or in silico) into large-volume quasicrystals. Consequently, it is unknown whether soft-matter quasicrystals form with the high degree of structural quality found in metal alloy quasicrystals. Here, we investigate the entropically driven growth of colloidal dodecagonal quasicrystals (DQCs) via computer simulation of systems of hard tetrahedra, which are simple models for anisotropic colloidal particles that form a quasicrystal. Using a pattern recognition algorithm applied to particle trajectories during DQC growth, we analyze phason strain to follow the evolution of quasiperiodic order. As in alloys, we observe high structural quality; DQCs with low phason strain crystallize directly from the melt and only require minimal further reduction of phason strain. Finally, we also observe transformation from a denser approximant to the DQC via continuous phason strain relaxation. Our results demonstrate that soft-matter quasicrystals dominated by entropy can be thermodynamically stable and grown with high structural quality––just like their alloy quasicrystal counterparts.

Research Organization:
Univ. of Michigan, Ann Arbor, MI (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
Grant/Contract Number:
SC0019118
OSTI ID:
1852847
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 7 Vol. 118; ISSN 0027-8424
Publisher:
National Academy of SciencesCopyright Statement
Country of Publication:
United States
Language:
English

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