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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.

Magnetic insulators, such as the rare‐earth iron garnets, are promising materials for energy‐efficient spintronic memory and logic devices, and their anisotropy, magnetization, and other properties can be tuned over a wide range through selection of the rare‐earth ion. Films are typically grown as epitaxial single crystals on garnet substrates, but integration of these materials with conventional electronic devices requires growth on Si. The growth, magnetic, and spin transport properties of polycrystalline films of dysprosium iron garnet (DyIG) with perpendicular magnetic anisotropy (PMA) on Si substrates and as single crystal films on garnet substrates are reported. PMA originates from magnetoelastic anisotropy and is obtained by controlling the strain state of the film through lattice mismatch or thermal expansion mismatch with the substrates. DyIG/Si exhibits large grain sizes and bulk‐like magnetization and compensation temperature. Polarized neutron reflectometry demonstrates a small interfacial nonmagnetic region near the substrate. Spin Hall magnetoresistance measurements conducted on a Pt/DyIG/Si heterostructure demonstrate a large interfacial spin mixing conductance between the Pt and DyIG comparable to other garnet/Pt heterostructures.