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| Naji, M. |
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| Azevedo, Nuno Monteiro |
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Hamming-Green, Ruben
University of Groningen
in Cooperation with on an Cooperation-Score of 37%
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article
Structural modulation in potassium birnessite single crystals
Abstract
<p>We report on the growth of single-crystal potassium birnessite (K<sub>0.31</sub>MnO<sub>2</sub>·0.41H<sub>2</sub>O) and present both the average and local structural characterization of this frustrated magnetic system. Single crystals were obtained employing a flux growth method with a KNO<sub>3</sub>/B<sub>2</sub>O<sub>3</sub>flux at 700 °C. Single-crystal X-ray diffraction revealed an average orthorhombic symmetry, with space groupCmcm. A combination of high angle annular dark field scanning transmission electron microscopy (HAADF-STEM) with atomic resolution energy dispersive X-ray spectroscopy (EDS) demonstrated the layered structure of potassium birnessite with manganese-containing planes well separated by layers of potassium atoms. MnO<sub>6</sub>octahedra and the K/H<sub>2</sub>O planes were clearly imagedviaintegrated differential phase contrast (iDPC) STEM. Furthermore, iDPC-STEM also revealed the existence of local domains with alternating contrast of the manganese oxide planes, most likely originating from charge ordering of Mn<sup>3+</sup>and Mn<sup>4+</sup>along thec-axis. These charge-ordered domains are clearly correlated with a reduction in thec-lattice parameter compared to the rest of the matrix. The insight gained from this work allows for a better understanding of the correlation between structure and magnetic properties.</p>