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Electrostatic Superlattices Beyond 1:1 Stoichiometry
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DOI：10.1002/adfm.77545.png)
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Abstract
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Exotic nanoparticle superstructures can be accessed by harnessing nanoparticle softness and charge regulation, features often viewed as obstacles to structural control. Here, we show that regulated charge mismatch in polymer-grafted nanoparticles enables the assembly of high-stoichiometry cubic superlattices. By co-tuning grafting density, particle size, and bulk composition, we realize ionic-lattice analogues, such as CaF2 CaF2${\rm CaF}_2$ and Th3P Th3P${\rm Th}_3{\rm P}$4 4$_4$, as well as single-component A3 A3${\rm A}_3$ and A7 A7${\rm A}_7$ superlattices without atomic counterparts. The A3 A3${\rm A}_3$ superlattice has recently been identified theoretically as a photonic band-gap lattice. These phases emerge from a 1:1 “parent” lattice when local charge neutrality cannot be satisfied, driving either progressive interstitial filling or reorganization into a larger basis. For instance, the systematic occupation of ZnS tetrahedral sites yields CaF2 CaF2${\rm CaF}_2$, while ligand-swapping symmetry breaking converts CsCl into Th3 Th3${\rm Th}_3$P4 P4${\rm P}_4$. Upon heating, the assemblies exhibit reversible lattice contraction and pronounced negative thermal expansion. Furthermore, the energetic penalty for defects increases with nanoparticle size, facilitating the scalable production of high-quality, open superlattices for photonic applications.
Keywords:
gold nanoparticles
ionic crystal analogs
nanoparticle self-assembly
photonic superlattices
small-angle x-ray scattering
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