Kavli Affiliate: David T. Limmer
| Summary:
Nanocrystals (NCs) serve as versatile building blocks for the creation of functional materials, with NC self-assembly offering opportunities to enable novel material properties. Here, we demonstrate that PbS NCs functionalized with strongly negatively charged metal chalcogenide complex (MCC) ligands, such as $Sn_2S_6^4-$ and $AsS_4^3-$, can self-assemble into all-inorganic superlattices with both long-range superlattice translational and atomic-lattice orientational order. Structural characterizations reveal that the NCs adopt unexpected edge-to-edge alignment, and numerical simulation clarifies that orientational order is thermodynamically stabilized by many-body ion correlations originating from the dense electrolyte. Furthermore, we show that the superlattices of $Sn_2S_6^4-$-functionalized PbS NCs can be fully disassembled back into the colloidal state, which is highly unusual for orientationally attached superlattices with atomic-lattice alignment. The reversible oriented attachment of NCs, enabling their dynamic assembly and disassembly into effectively single-crystalline superstructures, offers a pathway toward designing reconfigurable materials with adaptive and controllable electronic and optoelectronic properties.
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