Vis−NIR magneto-optical crystals are the key materials in the fields of optical fiber communication, smart grids, optical fiber lasers, and so on. In this paper, the incongruentmelting Tb 3 Al 5 O 12 (TAG) single crystals with centimeter size and high quality were grown rapidly by an EFG method with the suitable design of a melt component. The effects of the sintering temperature of polycrystalline materials, the melt component, and the growth rate on the crystal quality were discussed in detail. The Verdet constants, hardness, thermal expansion coefficients, specific heat capacities, and thermal diffusivities of TAG crystal were measured. The results show that the Verdet constant of the TAG crystal is 8−30% larger than those of Tb 3 Sc 2 Al 3 O 12 (TSAG) and Tb 3 Ga 5 O 12 (TGG) crystals. Additionally, the TAG crystal also has the advantage in both thermal conductivity and hardness. Therefore, the TAG crystal has good comprehensive performance and thus has important application prospects.

Bi3+-doped iron garnet crystals (Bi:RIG) have received extensive attention for their excellent magneto-optical properties. The quality of garnet crystals has a great relationship with mismatch in the lattice and thermal expansion between crystals and seeds. Compared with TGG seeds, Sc,Ga:YIG is more suitable as the seed for growing Bi:(HoEu)IG crystals. The crystal quality and match in the lattice and thermal expansion have been discussed. The as-grown Bi:(HoEu)IG crystal has a specific Faraday rotation angle of −467° cm–1 and shows a strong magneto-optical effect.