Single-crystal growth, crystallography, magnetic susceptibility, heat capacity, and thermal expansion of the antiferromagneticS=1chain compoundCaV2O4

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The compound CaV{sub 2}O{sub 4} contains V{sup +3} cations with spin S=1 and has an orthorhombic structure at room temperature containing zigzag chains of V atoms running along the c axis. We have grown single crystals of CaV{sub 2}O{sub 4} and report crystallography, static magnetization, magnetic susceptibility x, ac magnetic susceptibility, heat capacity C{sub p}, and thermal expansion measurements in the temperature T range of 1.8--350 K on the single crystals and on polycrystalline samples. An orthorhombic-to-monoclinic structural distortion and a long-range antiferromagnetic (AF) transition were found at sample-dependent temperatures T{sub S}{approx}108--145 K and T{sub 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 V{sub 2}O{sub 3} impurity 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 x(T) shows a broad maximum at {approx}300 K associated with short-range AF ordering and the anisotropy of x above T{sub N} is small. The anisotropic x(T{yields}0) data below T{sub N} show that the (average) easy axis of the AF magnetic structure is the b axis. The C{sub p}(T) data indicatemore » strong short-range AF ordering above T{sub N}, consistent with the x(T) data. We fitted our x data by a J{sub 1}-J{sub 2} S=1 Heisenberg chain model, where J{sub 1}(J{sub 2}) is the (next)-nearest-neighbor exchange interaction. We find J{sub 1}{approx}230 K and surprisingly, J{sub 2}/J{sub 1}{approx}0 (or J{sub 1}/J{sub 2}{approx}0). The interaction J{sub {perpendicular}} between these S=1 chains leading to long-range AF ordering at T{sub N} is estimated to be J{sub {perpendicular}}/J{sub 1}{approx_equal}0.04.« less