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A highly luminescent Zn4L6 tetrahedron is reported with 3.8 nm perylene bisimide edges and hexadentate ZnII–imine chelate vertices. Replacing FeII and monoamines commonly utilized in subcomponent self‐assembly with ZnII and tris(2‐aminoethyl)amine provides access to a metallosupramolecular host with the rare combination of structural integrity at concentrations <10−7 mol L−1 and an exceptionally...
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