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We report the crystal structure and magnetic behavior of the $4d^3$spin-$\frac32$ silicophosphate MoP$_3$SiO$_{11}$ studied by high-resolutionsynchrotron x-ray diffraction, neutron diffraction, thermodynamic measurements,and ab initio band-structure calculations. Our data revise the crystallographicsymmetry of this compound and establish its rhombohedral space group ($R\bar3c$) along with the geometrically perfect honeycomb lattice of the Mo$^{3+}$ions residing in disconnected MoO$_6$ octahedra. Long-range antiferromagneticorder with the propagation vector $\mathbf k=0$ observed below $T_N=6.8$ K is acombined effect of the nearest-neighbor in-plane exchange coupling $J\simeq2.6$ K, easy-plane single-ion anisotropy $D\simeq 2.2 $ K, and a weakinterlayer coupling $J_c\simeq 0.8$ K. The 12% reduction in the orderedmagnetic moment of the Mo$^{3+}$ ions and the magnon gap of $\Delta\simeq 7$ Kinduced by the single-ion anisotropy further illustrate the impact ofspin-orbit coupling on the magnetism. Our analysis puts forward single-ionanisotropy as an important ingredient of $4d^3$ honeycomb antiferromagnetsdespite their nominally quenched orbital moment.

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