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Register a new user^{17}O and ^{51}V NMR for the zigzag spin-1 chain compound CaV2O4
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$^{51}$V NMR studies on CaV2O4 single crystals and $^{17}$O NMR studies on $^{17}$O-enriched powder samples are reported. The temperature dependences of the $^{17}$O NMR line width and nuclear spin-lattice relaxation rate give strong evidence for a long-range antiferromagnetic transition at Tn = 78 K in the powder. Magnetic susceptibility measurements show that Tn = 69 K in the crystals. A zero-field $^{51}$V NMR signal was observed at low temperatures (f $approx$ 237 MHz at 4.2 K) in the crystals. The field swept spectra with the field in different directions suggest the presence of two antiferromagnetic substructures. Each substructure is collinear, with the easy axes of the two substructures separated by an angle of 19(1) degree, and with their average direction pointing approximately along the b-axis of the crystal structure. The two spin substructures contain equal number of spins. The temperature dependence of the ordered moment, measured up to 45 K, shows the presence of an energy gap Eg in the antiferromagnetic spin wave excitation spectrum. Antiferromagnetic spin wave theory suggests that Eg lies between 64 and 98 K.
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We present muon-spin rotation measurements on polycrystalline samples of the complete family of the antiferromagnetic (AF) $zigzag$ chain compounds, Na$_x$Ca$_{1-x}$V$_2$O$_4$. In this family, we explore the magnetic properties from the metallic NaV$_2$O$_4$ to the insulating CaV$_2$O$_4$. We find a critical $x_c(sim0.833)$ which separates the low and high Na-concentration dependent transition temperature and its magnetic ground state. In the $x<x_c$ compounds, the magnetic ordered phase is characterized by a single homogenous phase and the formation of incommensurate spin-density-wave order. Whereas in the $x>x_c$ compounds, multiple sub-phases appear with temperature and $x$. Based on the muon data obtained in zero external magnetic field, a careful dipolar field simulation was able to reproduce the muon behavior and indicates a modulated helical incommensurate spin structure of the metallic AF phase. The incommensurate modulation period obtained by the simulation agrees with that determined by neutron diffraction.
The compound CaV2O4 contains V^{+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 CaV2O4 and report crystallography, static magnetization, magnetic susceptibility chi, ac magnetic susceptibility, heat capacity Cp, 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_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 V2O3 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 chi(T) shows a broad maximum at approx 300 K associated with short-range AF ordering 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 magnetic structure is the b-axis. The Cp(T) data indicate strong short-range AF ordering above T_N, consistent with the chi(T) data. We fitted our chi(T) data near room 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, and surprisingly, J2/J1 approx 0 (or J1/J2 approx 0). The interaction J_perp between these S = 1 chains leading to long-range AF ordering at T_N is estimated to be J_perp/J_1 gtrsim 0.04.
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