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Solid solutions Ga 1−x Ge x V 4 S 8  (x = 0−1) were synthesized by solid-state reactions and characterized by temperature-dependent X-ray powder diffraction and static magnetic susceptibility measurements. The compounds crystallize in the cubic GaMo 4 S 8 -type structure (space group F43m), built up by heterocubane-like [V 4 S 4 ] (5−x)+  cubes and [Ga 1−x Ge x S 4 ] (5−x)−  tetrahedra arranged in a NaCllike manner. The successive substitution of Ga 3+  by Ge 4+  increases the electron count in the molecular orbitals (MO’s) of the V4-cluster gradually from seven to eight. We observe an almost linear increase of the magnetic moments, connected with a transition from ferromagnetic to antiferromagnetic ordering around x ≈ 0.5. Remarkably, low-temperature structural phase transitions as known from the ternary compounds were also detected in the solid solutions. The gallium-rich compounds (0 ≤ x &lt; 0.5) undergo rhombohedral distortions like GaV 4 S 8  (space group R3m), whereas distortions to orthorhombic symmetry (space group Imm2) as known from GeV 4 S 8  occur in the germanium-rich part of the solid solutions (0.5 ≤ x ≤ 1)

Low-temperature Crystal Structures and Magnetic Properties of the V 4 -Cluster Compounds Ga 1-x Ge x V 4 S 8