Dzyaloshinskii-Moriya nature of ferroelectric ordering in magnetoelectric Gd$_{1-x}$Y$_{x}$MnO$_{3}$ system


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This work reports on magnetic, dielectric, thermodynamic and magnetoelectric properties of Gd$_{1-x}$Y$_{x}$MnO$_{3}$, with 0 leq x leq 0.4, with emphasis on the (x, T) phase diagram, towards unraveling the role of the driving mechanisms in stabilizing both magnetic and ferroelectric orderings. The (x, T) phase diagram reflects the effect of lattice distortions induced by the substitution of $Gd^{3+}$ ion by smaller $Y^{3+}$ ion, which gradually unbalances the antiferromagnetic against the ferromagnetic exchange interactions, enabling the emergence of ferroelectricity for higher concentrations of yttrium. For $x leq 0.1$, the paramagnetic phase is followed by a presumably incommensurate collinear antiferromagnetic phase, then a weak ferromagnetic canted A-type antiferromagnetic ordering is established at lower temperatures.For $0.2 leq x leq 0.4$, a different phase sequence is obtained. The canted A-type antiferromagnetic arrangement is no more stable, and instead a pure antiferromagnetic ordering is stabilized below T$_{lock}$ $approx$ 14 - 17 K, with an improper ferroelectric character. From these results, a cycloid modulated spin arrangement at low temperatures is proposed, accordingly to the inverse Dzyaloshinskii Moriya model. Anomalous temperature dependence of the dipolar relaxation energy and magnetization evidence for structural and magnetic changes occurring at $T* approx 22 - 28 K$, for $0.1 leq x leq 0.4$.

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