Five substituted gadolinium gallium garnet crystals with different Ca2+/Mg2+/Zr4+ stoichiometric ratio concentrations (Zr4+: 13.0, 15.0, 15.3, 16.3, 19.5 at.%, as well as increasing Ca2+ and Mg2+ concentrations in proportion) were grown by Czochralski technique. Their structure, defect, thermal and optical properties were comparatively studied and analyzed. The lattice parameters are achieved to be 12.47–12.54 Å which are 0.7–1.2 % larger than that of Gd3Ga5O12. A linear equation with Zr4+ concentration is fitted to adjust the lattice parameter for demand. X-ray rocking curves with narrow FWHMs of 1.67′, 1.97′, 1.75′, 2.12′, 2.99′, respectively, indicating high crystalline quality when the Zr4+ concentration is below 16.3 at.%. The dislocation densities are 62, 47, 63, 315 and 3184 cm−2, suggesting the value increases rapidly when the Zr4+ concentration exceeds 16.3 at.% due to large lattice distortion. The thermal expansion coefficients are about 8.55 × 10−6 to 8.72 × 10−6 K−1, respectively. All the transmittances are above 80 % from visible to infrared wavelengths, and Sellmeier coefficients of refraction index equation were fitted, which is benefit for CaMgZr:GGG as substrate and optics application. The above results suggest that a more suitable substrate can be obtained for the series YIG magnetic-optic thin films by optimizing the Ca2+/Mg2+/Zr4+ concentrations.
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