Abstract

We have investigated magnetic and electrical properties in a multiferroic Mn0.93Co0.07W0.93O4-δ single crystal grown using the flux method, in which spiral spin orderings are known to be stabilized and thus magnetically induced electric polarization develops consistent with the spin current model. Upon temperature being lowered, two successive magnetic transitions appeared at \(T_{\text{N1}} = 13.0\) and \(T_{\text{N2}} = 12.2\) K. While there was no development of ferroelectric polarization \(P\) below \(T_{\text{N1}}\), a dominant \(P\) along the \(a\)-axis (\(P_{a}\)) and a small \(P\) along the \(b\)-axis (\(P_{b}\)) clearly developed below \(T_{\text{N2}}\), suggesting the stabilization of a spiral order with its basal plane close to the \(ac\)-plane. The magnetization measurements also support the existence of the spiral order with \(ac\)-basal plane below \(T_{\text{N2}}\) by exhibiting the largest spin susceptibility along the \(b\)-axis and the smaller ones along the \(a\)- and \(c\)-axes. Upon further lowering temperature below \(T^{*} = 10.1\) K, \(P_{a}\) starts to decrease significantly accompanied by a small increase of \(P_{b}\) while the magnetic susceptibility along the \(c\)-axis gradually becomes the largest and concomitantly shows a saturation. We have also found that the magnitude of \(P_{a}\) or \(P_{b}\) can be controlled smoothly at low temperatures as a function of magnetic field less than 9 T. These findings show that the magnitude and direction of the electric polarization vector in Mn0.93Co0.07W0.93O4-δ can be varied as a function of temperature and magnetic field via the changes in the properties of the associated spiral phases.

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