Preparation of single-layer manganese oxide nanosheets (monosheets) comprised of edge-shared MnO(6) octahedra has relied on multistep processing involving a high-temperature solid-state synthesis of bulk templates, and ion-exchange and exfoliation reactions in solutions, requiring high cost and long processing time. Here we demonstrate the first single-step approach to directly access the MnO(2) monosheets, by the chemical oxidation of Mn(2+) ions in the presence of tetramethylammonium cations in an aqueous solution. Of importance is that this template-free reaction readily proceeds within a day at room temperature. The ability of the MnO(2) monosheets to self-assemble allows aggregation, to form layered structures with potassium cations and cationic tetrathiafulvalene analogues as intercalants. Furthermore, Langmuir-Blodgett (LB) films composed of the MnO(2) monosheets were successfully fabricated by the LB deposition method, in which about one layer of the monosheets was deposited for each process.

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