paper

Polyhedral distortions and unusual magnetic order in spinel FeMnO

arXiv:2210.15089 · doi:10.1021/acs.chemmater.2c03182

Abstract

Spinel compounds ABX consist of both tetrahedral (AX) and octahedral (BX) environments with the former forming a diamond lattice and the latter a geometrically frustrated pyrochlore lattice. Exploring the fascinating properties and their correlations with structural features is critical in understanding these materials. FeMnO has been reported to exhibit one structural transition and two successive magnetic transitions. Here, we report the polyhedral distortions and their correlations to the structural and two magnetic transitions in FeMnO by employing the high-resolution neutron powder diffraction. While a large trigonal distortion is found even in the high-temperature cubic phase, the first-order cubic-tetragonal structural transition associated with the elongation of both tetrahedra and octahedra along the axis occurs at 750 K, driven by the Jahn-Teller effect of the orbital active B-site Mn cation. A strong magnetoelastic coupling is unveiled at K as manifested by the appearance of Nèel-type collinear ferrimagnetic order, an anomaly in both tetrahedral and octahedral distortions, as well as an anomalous decrease of the lattice constant and a weak anomaly of . Upon cooling below K, it evolves to a noncollinear ferrimagnetic order with a canting of half B-site / spins in the pyrochlore lattice, which is a unique magnetic order among spinels. Such a noncollinear order induces modifications of the O-B-O bond angles in the octahedra without affecting much the bond lengths of the tetrahedra/octahedra. Our study indicates that FeMnO is a wonderful platform to unveil interesting magnetic order and to investigate their correlations to polyhedral distortions and lattice.

13 pages, 10 figures, Accepted for publication in Chemistry of Materials

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