Abstract

Isotropic and anisotropic magnetic behavior of the frustrated spin chain compound ββ-TeVO4_4 is reported. Three magnetic transitions observed in zero magnetic field are tracked in fields applied along different crystallographic directions using magnetization, heat capacity, and magnetostriction measurements. Qualitatively different temperature-field diagrams are obtained below 10 T for the field applied along aa or bb and along cc, respectively. In contrast, a nearly isotropic high-field phase emerges above 18 T and persists up to the saturation that occurs around 22.5 T. Upon cooling in low fields, the transitions at TN1T_{\rm N1} and TN2T_{\rm N2} toward the spin-density-wave and stripe phases are of the second order, whereas the transition at TN3T_{\rm N3} toward the helical state is of the first order and entails a lattice component. Our microscopic analysis identifies frustrated J1−J2J_1-J_2 spin chains with a sizable antiferromagnetic interchain coupling in the bcbc plane and ferromagnetic couplings along the aa direction. The competition between these ferromagnetic interchain couplings and the helical order within the chain underlies the incommensurate order along the aa-direction, as observed experimentally. Although a helical state is triggered by the competition between J1J_1 and J2J_2 within the chain, the plane of the helix is not uniquely defined because of competing magnetic anisotropies. Using high-resolution synchrotron diffraction and 125^{125}Te nuclear magnetic resonance, we also demonstrate that the crystal structure of ββ-TeVO4_4 does not change down to 10 K, and the orbital state of V4+^{4+} is preserved.

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