MoP${}_3$SiO${}_{11}$: a $4d^3$ honeycomb antiferromagnet with disconnected octahedra

Abstract

We report the crystal structure and magnetic behavior of the $4d^3$ spin-$\frac{3}{2}$ silicophosphate MoP${}_3$SiO${}_{11}$ studied by high-resolution synchrotron x-ray diffraction, neutron diffraction, thermodynamic measurements, and ab initio band-structure calculations. Our data revise the crystallographic symmetry of this compound and establish its rhombohedral space group ($R\bar{3}c$) along with the geometrically perfect honeycomb lattice of the Mo${}^{3+}$ ions residing in disconnected MoO${}_6$ octahedra. Long-range antiferromagnetic order with the propagation vector $\mathbf{k}=0$ observed below $T_N=6.8$ K is a combined effect of the nearest-neighbor in-plane exchange coupling $J\simeq 2.6$ K, easy-plane single-ion anisotropy $D\simeq 2.2$ K, and a weak interlayer coupling $J_c\simeq 0.8$ K. The 12% reduction in the ordered magnetic moment of the Mo${}^{3+}$ ions and the magnon gap of $\Delta \simeq 7$ K induced by the single-ion anisotropy further illustrate the impact of spin-orbit coupling on the magnetism. Our analysis puts forward single-ion anisotropy as an important ingredient of $4d^3$ honeycomb antiferromagnets despite their nominally quenched orbital moment.

published version

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Cited by in corpus (2)

• Magnetism and field-induced effects in the S = 5/2 honeycomb lattice antiferromagnet FeP3SiO11
• Theoretical analysis of single-ion anisotropy in $d^3$ Mott insulators