The assembly of uniform nanocrystal building blocks into well ordered superstructures is a fundamental strategy for the generation of meso- and macroscale metamaterials with emergent nanoscopic functionalities1,2,3,4,5,6,7,8,9,10. The packing of spherical nanocrystals, which frequently adopt dense, face-centred-cubic or hexagonal-close-packed arrangements at thermodynamic equilibrium, has been much more widely studied than that of non-spherical, polyhedral nanocrystals, despite the fact that the latter have intriguing anisotropic properties resulting from the shapes of the building blocks11,12,13. Here we report the packing of truncated tetrahedral quantum dot nanocrystals into three distinct superstructures—one-dimensional chiral tetrahelices, two-dimensional quasicrystal-approximant superlattices and three-dimensional cluster-based body-centred-cubic single supercrystals—by controlling the assembly conditions. Using techniques in real and reciprocal spaces, we successfully characterized the superstructures from their nanocrystal translational orderings down to the atomic-orientation alignments of individual quantum dots. Our packing models showed that formation of the nanocrystal superstructures is dominated by the selective facet-to-facet contact induced by the anisotropic patchiness of the tetrahedra. This study provides information about the packing of non-spherical nanocrystals into complex superstructures, and may enhance the potential of self-assembled nanocrystal metamaterials in practical applications.
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The data supporting the findings of this study are available from the corresponding author upon reasonable request.
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O.C. acknowledges support from the Brown University Startup Fund, the Salomon Award Fund, the IMNI Seed Fund and the UAC grant from the Xerox foundation. The Cornell High Energy Synchrotron Source was supported by the NSF award DMR-1332208. This work was performed, in part, at the Center for Nanoscale Materials, a US Department of Energy Office of Science User Facility, and supported by the US Department of Energy, Office of Science, under contract number DE-AC02-06CH11357. The TEM and SEM measurements were performed at the Electron Microscopy Facility in the Institute for Molecular and Nanoscale Innovation (IMNI) at Brown University.
Nature thanks J. Fang, A. Petukhov and the other anonymous reviewer(s) for their contribution to the peer review of this work.