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The electronic valence state of Mn in Pb(Zr0.2Ti0.8)O3/La0.8Sr0.2MnO3multiferroic heterostructures is probed by near edge x-ray absorptionspectroscopy as a function of the ferroelectric polarization. We observe atemperature independent shift in the absorption edge of Mn associated with achange in valency induced by charge carrier modulation in the La0.8Sr0.2MnO3,demonstrating the electronic origin of the magnetoelectric effect.Spectroscopic, magnetic, and electric characterization shows that the largemagnetoelectric response originates from a modified interfacial spinconfiguration, opening a new pathway to the electronic control of spin incomplex oxide materials.

Origin of the magnetoelectric coupling effect in Pb(Zr0.2Ti0.8)O3/La0.8Sr0.2MnO3 multiferroic heterostructures