Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 47, Pages 21183-21189Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202009941
Keywords
nanoparticle self-assembly; nanoscale surface chemistry; orientational order; plastic crystals; uniform metacrystals
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Funding
- Ministry of Education, Singapore, under Tier 1 grant [RG11/18]
- Ministry of Education, Singapore, under Tier 2 grant [MOE2016-T2-1-043]
- Max Planck Institute-Nanyang Technological University Joint Lab
- Nanyang Technological University, Singapore
- Singapore Ministry of Education
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In nanoparticle self-assembly, the current lack of strategy to modulate orientational order creates challenges in isolating large-area plastic crystals. Here, we achieve two orientationally distinct supercrystals using one nanoparticle shape, including plastic crystals and uniform metacrystals. Our approach integrates multi-faceted Archimedean polyhedra with molecular-level surface polymeric interactions to tune nanoparticle orientational order during self-assembly. Experiments and simulations show that coiled surface polymer chains limit interparticle interactions, creating various geometrical configurations among Archimedean polyhedra to form plastic crystals. In contrast, brush-like polymer chains enable molecular interdigitation between neighboring particles, favoring consistent particle configurations and result in uniform metacrystals. Our strategy enhances supercrystal diversity for polyhedra comprising multiple nondegenerate facets.
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