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Yttrium iron garnet (YIG) and barium titanate (BTO) were co-deposited on (001)-orientated gadolinium gallium garnet substrates by pulsed laser deposition with composition determined by the ratio of laser shots ablating each target. With increasing shot ratios of YIG/BTO = 2.5/1, 4/1, 20/1, and 30/1, the majority phase in the film changes from textured polycrystalline perovskite to epitaxial garnet. Cross-sectional STEM characterization of the YIG-rich films reveals three distinct sublayers: the bottom layer is a coherent epitaxial garnet layer with higher unit cell volume than that of YIG; the second layer is garnet exhibiting crystalline defects and misorientation; and the upper layer is amorphous. Highly defective regions within the second layer are richer in Ba, suggesting that the microstructure is promoted by the insolubility of Ba in YIG. Temperature-dependent magnetization measurements fitted to a super-exchange dilution model indicate the presence of nonmagnetic Ti and vacancies in both octahedral and tetrahedral sites.

Voltage-tuning of magnetic anisotropy is demonstrated in ferrimagnetic insulating rare earth iron garnets on a piezoelectric substrate, (011)-oriented PMN-PT. A 42 nm thick yttrium-substituted dysprosium iron garnet (YDyIG) film is grown via pulsed laser deposition followed by a rapid thermal anneal to crystallize the garnet into ≈5  μm diameter grains. The annealed polycrystalline film is magnetically isotropic in the film plane with total anisotropy dominated by shape and magnetoelastic contributions. Application of an electric field perpendicular to the substrate breaks the in-plane easy axis along [01[Formula: see text]] and an intermediate axis along [100]. The results are explained in terms of the piezoelectric remanent strain caused by poling the substrate, which is transferred to the YDyIG and modulates the magnetoelastic anisotropy.

We use density functional theory (DFT) calculations to show that oxygen vacancies (vO) and mobility induce noncentrosymmetric polar structures in SrTi1−x−yFexCoyO3−δ (STFC, x=y=0.125) with δ={0.125,0.25}, enhance the saturation magnetization, and give rise to large changes in the electric polarization |ΔP|. We present an intuitive set of rules to describe the properties of STFC, which are based on the interplay between (Co/Fe)-vO defects, magnetic cation coordination, and topological vacancy disorder. STFC structures consist of layered crystals with sheets of linearly organized O4,5,6-coordinated Fe–Co pairs, sandwiched with layers of O5-coordinated Ti. (Co/Fe)-vO defects are the source of crystal distortions, cation off-centering and bending of the oxygen octahedra which, considering the charge redistribution mediated by vO and the cations’ electronegativity and valence states, triggers an effective electric polarization. Oxygen migration for δ=0.125 leads to |ΔP|>∼10 µC/cm2 due to quantum-of-polarization differences between δ=0.125 structures. Increasing the oxygen deficiency to δ=0.25 yields |ΔP|, the O migration of which resolved polarization for δ=0.25 is >∼3 µC/cm2. Magnetism is dominated by the Fe,Co spin states for δ=0.125, and there is a contribution from Ti magnetic moments (∼1 μB) for δ=0.25. Magnetic and electric order parameters change for variations of δ or oxygen migration for a given oxygenmore »deficiency. Our results capture characteristics observed in the end members of the series SrTi(Co,Fe)O3, and suggest the existence of a broader set of rules for oxygen-deficient multiferroic oxides.« less