Controlled Self-Assembly of Gold Nanotetrahedra into Quasicrystals and Complex Periodic Supracrystals
Controlled Self-Assembly of Gold Nanotetrahedra into Quasicrystals and Complex Periodic Supracrystals
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金纳米四面体受控自组装成准晶和复杂周期超晶
DOI：
10.1021/jacs.3c05299
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发表时间：
2023
影响因子：
15
通讯作者：
Apeleo Zubiri, Benjamin
中科院分区：
文献类型：
--
作者：
Wang, Yi;Chen, Jun;Li, Ruipeng;Götz, Alexander;Drobek, Dominik;Przybilla, Thomas;Hübner, Sabine;Pelz, Philipp;Yang, Lin;Apeleo Zubiri, Benjamin
形状各向异性纳米晶体自组装成大规模结构是一种多功能和可扩展的方法来创建多功能材料。四面体几何在自然和人造材料中普遍存在，然而正四面体在理解它们的自组装行为方面提出了一个巨大的挑战，因为它们不平铺空间。在这里，我们报告不同的超晶体从金纳米四面体，包括准晶体（QC）和二聚体包装预测超过十年前和迄今未知的阶段。我们解决了复杂的三维（3D）结构的QC相结合的电子显微镜，断层扫描，和同步辐射X射线散射。纳米四面体顶点锐度、表面配体和组装条件协同工作以调节超晶体结构。我们还发现，超晶体的表面曲率可以诱导的QC平铺结构的变化，并最终，小超晶体与高曲率，稳定的六方近似。我们的研究结果弥合了软物质组装体的计算设计和实验实现之间的差距，并证明了精确控制超晶格属性和组装条件以实现日益复杂的纳米多面体超晶体的重要性。
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. 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.