Experimental evidence of a change of exchange anisotropy sign with temperature in Zn-substituted Cu₂OSeO₃

We report small-angle neutron scattering from the conical state in a single crystal of Zn-substituted Cu2OSeO3. Using a 3D vector-field magnet to reorient the conical wave vector, our measurements show that the magnitude of the conical wave vector changes as a function of crystallographic direction. These changes are explained using the anisotropic exchange interaction (AEI) within the continuum model, whose magnitude in free-energy transitions from a maxima to a minima along the < 111 > and < 100 > crystallographic directions respectively. We further find that the AEI free-energy constant undergoes a change of sign from positive to negative with decreasing temperature. Unlike in the related compound FeGe, where similar behavior of the AEI induces a reorientation of the helical wave vector, we show that the zero field helical wave vector in (Cu0.98Zn0.02)(2)OSeO3 remains along the < 100 > directions at all temperatures due to the competing fourth-order magnetocrystalline anisotropy becoming dominant at lower temperatures.