Controlled Self-Assembly of Gold Nanotetrahedra into Quasicrystals and Complex Periodic Supracrystals

Wang, Yi; Chen, Jun; Li, Ruipeng; Götz, Alexander; Drobek, Dominik; Przybilla, Thomas; Hübner, Sabine; Pelz, Philipp; Yang, Lin; Apeleo Zubiri, Benjamin; Spiecker, Erdmann; Engel, Michael; Ye, Xingchen

doi:10.1021/jacs.3c05299

Title: Controlled Self-Assembly of Gold Nanotetrahedra into Quasicrystals and Complex Periodic Supracrystals

Journal Article · 03 August 2023 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.3c05299 · OSTI ID:2432562

^[1];

^[1]; Li, Ruipeng ^[2]; Götz, Alexander ^[3]; Drobek, Dominik ^[3]; Przybilla, Thomas ^[3]; Hübner, Sabine ^[3]; Pelz, Philipp ^[3]; Yang, Lin ^[2]; Apeleo Zubiri, Benjamin ^[3];

^[3];

^[1]

Indiana Univ., Bloomington, IN (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Friedrich-Alexander University Erlangen-Nuremberg, Erlangen (Germany)

The self-assembly of shape-anisotropic nanocrystals into large-scale structures is a versatile and scalable approach to creating multifunctional materials. The tetrahedral geometry is ubiquitous in natural and manmade materials, yet regular tetrahedra present a formidable challenge in understanding their self-assembly behavior as they do not tile space. Here, we report diverse supracrystals from gold nanotetrahedra including the quasicrystal (QC) and the dimer packing predicted more than a decade ago and hitherto unknown phases. We solve the complex three-dimensional (3D) structure of the QC by a combination of electron microscopy, tomography, and synchrotron X-ray scattering. Nanotetrahedron vertex sharpness, surface ligands, and assembly conditions work in concert to regulate supracrystal structure. We also discover that the surface curvature of supracrystals can induce structural changes of the QC tiling and eventually, for small supracrystals with high curvature, stabilize a hexagonal approximant. Finally, our findings bridge the gap between computational design and experimental realization of soft matter assemblies and demonstrate the importance of accurate control over nanocrystal attributes and the assembly conditions to realize increasingly complex nanopolyhedron supracrystals.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: National Institute of General Medical Sciences (NIGMS); National Institutes of Health (NIH); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: SC0012704

OSTI ID:: 2432562

Report Number(s):: BNL--225938-2024-JAAM

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 32 Vol. 145; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: Controlled Self-Assembly of Gold Nanotetrahedra into Quasicrystals and Complex Periodic Supracrystals

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