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Abstract Complex oxides offer rich magnetic and electronic behavior intimately tied to the composition and arrangement of cations within the structure. Rare earth iron garnet films exhibit an anisotropy along the growth direction which has long been theorized to originate from the ordering of different cations on the same crystallographic site. Here, we directly demonstrate the three-dimensional ordering of rare earth ions in pulsed laser deposited (Eu_xTm_1-x)₃Fe₅O₁₂garnet thin films using both atomically-resolved elemental mapping to visualize cation ordering and X-ray diffraction to detect the resulting order superlattice reflection. We quantify the resulting ordering-induced ‘magnetotaxial’ anisotropy as a function of Eu:Tm ratio using transport measurements, showing an overwhelmingly dominant contribution from magnetotaxial anisotropy that reaches 30 kJ m⁻³for garnets with x = 0.5. Control of cation ordering on inequivalent sites provides a strategy to control matter on the atomic level and to engineer the magnetic properties of complex oxides. 

Cerium-substituted yttrium iron garnet (Ce:YIG, Ce0.9Y2.1Fe5O12) was epitaxially grown on a (111)-oriented yttrium aluminum garnet (YAG) substrate using radio frequency ion beam sputtering. Magnetic hysteresis loops, transmissivity spectra, and magnetooptical (MO) responses, including Faraday rotation and Faraday ellipticity, were measured. The structural properties of the grown Ce:YIG were characterized using the x-ray rocking curve, reciprocal space map, pole figure, and x-ray reflectivity. X-ray photoelectron spectrometry revealed a dominant Ce3+ state in the grown Ce:YIG, but the transmission electron microscopy images showed columnar growth of Ce:YIG. This study demonstrates integration of epitaxial Ce:YIG on YAG, marking a significant step toward the fusion of MO garnets and laser crystals. 

Abstract Ferrimagnetic oxide thin films are important material platforms for spintronic devices. Films grown on low symmetry orientations such as (110) exhibit complex anisotropy landscapes that can provide insight into novel phenomena such as spin‐torque auto‐oscillation and spin superfluidity. Using spin‐Hall magnetoresistance measurements, the in‐plane (IP) and out‐of‐plane (OOP) uniaxial anisotropy energies are determined for a thickness series (5–50 nm) of europium iron garnet (EuIG) and thulium iron garnet (TmIG) films epitaxially grown on a gadolinium gallium substrate with (110) orientation and capped with Pt. Pt/EuIG/GGG exhibits an (001) easy plane of magnetization perpendicular to the substrate, whereas Pt/TmIG/GGG exhibits an (001) hard plane of magnetization perpendicular to the substrate with an IP easy axis. Both IP and OOP surface anisotropy energies comparable in magnitude to the bulk anisotropy are observed. The temperature dependence of the surface anisotropies is consistent with first‐order predictions of a simplified Néel surface anisotropy model. By taking advantage of the thickness and temperature dependence demonstrated in these ferrimagnetic oxides grown on the low symmetry (110) orientations, the complex anisotropy landscapes can be tuned to act as a platform to explore rich spin textures and dynamics. 

Abstract Oxygen coordination and vacancy ordering play an important role in dictating the functionality of complex oxides. In this work, an unconventional layering of oxygen ions in a mixed conductor SrCo_1‐xFe_xO_3‐δ(SCFO) thin film grown epitaxially on SrTiO₃(STO) is reported. Scanning transmission electron microscopy (STEM) reveals alternating layers of oxygen deficiency along the growth direction, with the oxygen‐rich layer correlated with the neighboring Co,Fe‐site intensity, and contraction of the Sr–Sr distance. Density functional theory (DFT) calculations and STEM image simulations support the emergence of periodic (Co,Fe)O₆and (Co,Fe)O₄/(Co,Fe)O₅layers, an ordering that is also sensitive to the Co:Fe ratio. 

Abstract This work characterizes the structural, magnetic, and ferroelectric properties of epitaxial LuFeO₃orthoferrite thin films with different Lu/Fe ratios. LuFeO₃thin films are grown by pulsed laser deposition on SrTiO₃substrates with Lu/Fe ratio ranging from 0.6 to 1.5. LuFeO₃is antiferromagnetic with a weak canted moment perpendicular to the film plane. Piezoresponse force microscopy imaging and switching spectroscopy reveal room temperature ferroelectricity in Lu‐rich and Fe‐rich films, whereas the stoichiometric film shows little polarization. Ferroelectricity in Lu‐rich films is present for a range of deposition conditions and crystallographic orientations. Positive‐up‐negative‐down ferroelectric measurements on a Lu‐rich film yield ≈13 µC cm⁻²of switchable polarization, although the film also shows electrical leakage. The ferroelectric response is attributed to antisite defects analogous to that of Y‐rich YFeO₃, yielding multiferroicity via defect engineering in a rare earth orthoferrite. 

Abstract Ferrimagnetic iron garnets enable magnetic and magneto‐optical functionality in silicon photonics and electronics. However, garnets require high‐temperature processing for crystallization which can degrade other devices on the wafer. Here bismuth‐substituted yttrium and terbium iron garnet (Bi‐YIG and Bi‐TbIG) films are demonstrated with good magneto‐optical performance and perpendicular magnetic anisotropy (PMA) crystallized by a microheater built on a Si chip or by rapid thermal annealing. The Bi‐TbIG film crystallizes on Si at 873 K without a seed layer and exhibits good magneto‐optical properties with Faraday rotation (FR) of −1700 deg cm⁻¹. The Bi‐YIG film also crystallizes on Si and fused SiO₂at 873 K without a seed layer. Rapidly cooled films exhibit PMA due to the tensile stress caused by the thermal expansion mismatch with the substrates, increasing the magnetoelastic anisotropy by 4 kJ m⁻³versus slow‐cooled films. Annealing in the air for 15 s using the microheater yields fully crystallized Bi‐TbIG on the Si chip. 

Abstract 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. 

Abstract Films of polycrystalline terbium iron garnet (TbIG), cerium‐substituted TbIG (CeTbIG), and bismuth‐substituted TbIG (BiTbIG) are grown on Si substrates by pulsed laser deposition. The films grow under tensile strain due to thermal mismatch with the Si substrate, resulting in a dominant magnetoelastic anisotropy which, combined with shape anisotropy, leads to in‐plane magnetization. TbIG has a compensation temperature of 253 K which is reduced by substitution of Ce and Bi. The Faraday rotation at 1550 nm of the TbIG, Ce_0.36TbIG, and Bi_0.03TbIG films is 5400 ± 600° cm⁻¹, 4500 ± 100° cm^–1, and 6200 ± 300° cm⁻¹, respectively, while Ce_0.36TbIG and Bi_0.03TbIG exhibit lower optical absorption than TbIG, attributed to a reduction in Fe²⁺and Tb⁴⁺absorption pathways. The high Faraday rotation of the films, and in particular the high magneto‐optical figure of merit of the Bi_0.03TbIG of 720° dB⁻¹at 1550 nm, make these polycrystalline films valuable for applications in integrated photonics.