Liquid-phase epitaxy (LPE) is one of the best techniques for the preparation of single crystal garnet films. However, the specific Faraday rotation angle of Yttrium iron garnet (YIG) is small, and its easy magnetization axis is parallel to the film surface. The YIG requires a large external saturation field, which cannot meet the development needs of magneto-optical devices. It is found that Bi-substituted YIG(Bi:YIG) film has a larger specific Faraday angle. By adjusting the easy magnetization axis of Bi: YIG perpendicular to the film surface, the saturation magnetization of Bi: YIG can be reduced, so that it can work under a small external magnetic field. This meets the development needs of miniaturization and energy saving of magneto-optical device. The saturation magnetization of garnet film can be effectively reduced by substituting Ga<sup>3+</sup> for YIG crystal, mainly for Fe<sup>3+</sup> at the 24d position of its tetrahedron. And the lattice constants of Gd<sub>3</sub>Ga<sub>5</sub>O<sub>12</sub> (GGG) and YIG are 1.2383 nm and 1.2376 nm, respectively. However, the radius of Bi<sup>3+</sup> (10.8 nm) is larger than that of Y<sup>3+</sup> (9.0 nm), the lattice mismatch of garnet film increases with the incorporation of Bi<sup>3+</sup>. In order to neutralize the lattice expansion caused by Bi<sup>3+</sup>, Tm<sup>3+</sup> (8.69 nm) with a radius smaller than that of Y<sup>3+</sup> (9.0 nm) is selected. Based on the theoretical analysis of the magnetocrystalline anisotropy of garnet film, (BiTm)<sub>3</sub>(GaFe)<sub>5</sub>O<sub>12</sub> mono-crystalline films with different growth temperatures and different thickness values are grown by LPE on GGG (111) substrates. The experimental results show that when the thickness of epitaxial film is greater than 1 μm, the influence of shape anisotropy on magnetocrystalline anisotropy can be ignored. With the increase of growth temperature, the substitution number of Bi<sup>3+</sup> ions decreases gradually, the lattice constant of epitaxial film decreases gradually, and the lattice mismatch first decreases and then increases. Then, the state of compressive stress gradually changes into that of tensile stress. Compared with growth-induced anisotropy, the stress-induced anisotropy is dominant in the change of magnetocrystalline anisotropy. The Verdet constant of (BiTm)<sub>3</sub>(GaFe)<sub>5</sub>O<sub>12</sub> film is 11.8 × 10<sup>4</sup> rad/Tm@1064 nm. The results show that the prepared (BiTm)<sub>3</sub>(GaFe)<sub>5</sub>O<sub>12</sub> mono-crystalline films have great development potential in magneto-optical devices.
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