BaMn9[VO4]6(OH)2: A Unique Canted Antiferromagnet with a Chiral “Paddle-Wheel” Structural Feature

BaMn9[VO4]6(OH)2 was synthesized by hydrothermal methods. We evaluated the crystal structure based on the two possible space groups P213 and Pa3̅ [a = 12.8417(2) Å] using single-crystal and powder X-ray diffraction techniques. The structure contains three-dimensionally linked Mn9 units of a chiral “paddle-wheel” type. Experimental IR and Raman spectra were analyzed in terms of fundamental vanadate and hydroxide vibrational modes. The magnetic properties were investigated, and the specific heat in applied fields was studied. The dominant magnetic interactions (Mn2+, S = 5/2) are of antiferromagnetic origin, as indicated by a Curie–Weiss fit above 175 K with Θ ≈ −200 K. Canting of the spins on the geometrically frustrated triangle segment of the structural feature is considered to account for the ferrimagnetic type of long-range order at TC ≈ 18 K. We propose a model for the spin structure in the ordered regime. Dielectric constants were measured and indicate a magnetodielectric effect at TC, which is assigned to spin–lattice coupling.