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Rare‐earth iron garnets (REIG) have recently become the materials platform of choice for spintronic studies on ferrimagnetic insulators. However, thus far the materials studied have mainly been REIG with a single rare earth species such as thulium, yttrium, or terbium iron garnets. In this study, magnetometry, ferromagnetic resonance, and magneto‐optical Kerr effect imaging is used to explore the continuous variation of magnetic properties as a function of composition for Y_xTm_3−xiron garnet (Y_xTm_3−xIG) thin films grown by pulsed laser deposition on gadolinium gallium garnet substrates. It is reported that the tunability of the magnetic anisotropy energy, with full control achieved over the type of anisotropy (from perpendicular, to isotropic, to an in‐plane easy axis) on the same substrate. In addition, a nonmonotonic composition‐dependent anisotropy term is reported, which is ascribed to growth‐induced anisotropy similar to what is reported in garnet thin films grown by liquid‐phase epitaxy. Ferromagnetic resonance shows linear variation of the damping and the g‐factor across the composition range, consistent with prior theoretical work. Domain imaging reveals differences in reversal modes, remanant states, and domain sizes in Y_xTm_3−xiron‐garnet thin films as a function of anisotropy.

 

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.

 

Abstract Single-phase multiferroic materials that allow the coexistence of ferroelectric and magnetic ordering above room temperature are highly desirable, motivating an ongoing search for mechanisms for unconventional ferroelectricity in magnetic oxides. Here, we report an antisite defect mechanism for room temperature ferroelectricity in epitaxial thin films of yttrium orthoferrite, YFeO 3 , a perovskite-structured canted antiferromagnet. A combination of piezoresponse force microscopy, atomically resolved elemental mapping with aberration corrected scanning transmission electron microscopy and density functional theory calculations reveals that the presence of Y Fe antisite defects facilitates a non-centrosymmetric distortion promoting ferroelectricity. This mechanism is predicted to work analogously for other rare earth orthoferrites, with a dependence of the polarization on the radius of the rare earth cation. Our work uncovers the distinctive role of antisite defects in providing a mechanism for ferroelectricity in a range of magnetic orthoferrites and further augments the functionality of this family of complex oxides for multiferroic applications.