Abstract
The magnetism of the A-site-ordered perovskite $\mathrm{LaM}{\mathrm{n}}_{3}{\mathrm{V}}_{4}{\mathrm{O}}_{12}$ is studied comprehensively by means of neutron powder diffraction experiments and theoretical calculations. Magnetic neutron diffraction results show that a rhombohedral 60\ifmmode^\circ\else\textdegree\fi{} spin structure emerges on the cubic lattice below a 44-K N\'eel transition. Ab initio electronic structure calculations confirm that high-spin ${\mathrm{Mn}}^{2+}$ moments are localized while V $3d$-band states are itinerant, and that the noncollinear 60\ifmmode^\circ\else\textdegree\fi{} spin structure is more stable than collinear ferromagnetic or G-type antiferromagnetic alternatives. Effective Heisenberg model calculations reveal that the appearance of such a nontrivial spin structure can be attributed to significant next-nearest-neighbor and third-nearest-neighbor magnetic interactions.
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