In a mixed-valence polyoxometalate, electrons are usually delocalized within the cluster anion because of low level of inter-cluster interaction. Herein, we report the structure and electrical properties of a single crystal in which mixed-valence polyoxometalates were electrically wired by cationic π-molecules of tetrathiafulvalene substituted with pyridinium. Electron-transport characteristics are suggested to represent electron hopping through strong interactions between cluster and cationic π-molecules. Down to the wire: In a mixed-valence polyoxometalate (POM), electrons are usually delocalized within the metal cluster anion because of a low degree of inter-cluster interaction. If the mixed-valence POMs are electrically linked together by wires of cationic π molecules of tetrathiafulvalene substituted with pyridinium, electron transport can occur by electron hopping as a result of the strong interactions between cluster and cationic π molecules.
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