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The compound CaV2O4 contains V^{+3} cations with spin S = 1 and has anorthorhombic structure at room temperature containing zigzag chains of V atomsrunning along the c-axis. We have grown single crystals of CaV2O4 and reportcrystallography, static magnetization, magnetic susceptibility \chi, acmagnetic susceptibility, heat capacity Cp, and thermal expansion measurementsin the temperature T range of 1.8-350 K on the single crystals and onpolycrystalline samples. An orthorhombic to monoclinic structural distortionand a long-range antiferromagnetic (AF) transition were found atsample-dependent temperatures T_S \approx 108-145 K and T_N \approx 51-76 K,respectively. In two annealed single crystals, another transition was found at\approx 200 K. In one of the crystals, this transition is mostly due to V2O3impurity phase that grows coherently in the crystals during annealing. However,in the other crystal the origin of this transition at 200 K is unknown. The\chi(T) shows a broad maximum at \approx 300 K associated with short-range AFordering and the anisotropy of \chi above T_N is small. The anisotropic \chi(T\to 0) data below T_N show that the (average) easy axis of the AF magneticstructure is the b-axis. The Cp(T) data indicate strong short-range AF orderingabove T_N, consistent with the \chi(T) data. We fitted our \chi(T) data nearroom temperature by a J1-J2 S = 1 Heisenberg chain model, where J1(J2) is the(next)-nearest-neighbor exchange interaction. We find J1 \approx 230 K, andsurprisingly, J2/J1 \approx 0 (or J1/J2 \approx 0). The interaction J_\perpbetween these S = 1 chains leading to long-range AF ordering at T_N isestimated to be J_\perp/J_1 \gtrsim 0.04.

physical review. b, condensed matter and materials physics

Single Crystal Growth, Crystallography, Magnetic Susceptibility, Heat  Capacity, and Thermal Expansion of the Antiferromagnetic S = 1 Chain Compound  CaV2O4