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Ba2−xSrxZnWO6 double perovskite (DP) oxide compounds (x = 1, 1.25, 1.5, 1.75, 2) were successfully created by means of conventional solid-state techniques. The crystal structures of our series were studied using an X-ray diffractometer. The x = 1 compound has a cubic (Fm-3m) crystal structure, the 1 ≤ x ≤ 2 compounds have tetragonal (I4/m) symmetry, and the phase was transferred to monoclinic (P21/n) symmetry for the Sr2ZnWO6 (x = 2) compound. Scanning electron microscopy (SEM) was used to investigate the morphology of the series, showing that the samples had crystallized microstructures. Molecular bonds were investigated using Fourier transform infrared and Raman spectroscopies, which confirmed the double perovskite octahedral geometry for the samples in our series. Furthermore, the octahedral W–O6 anti-symmetric stretching mode was found to occur. The optical properties of the Ba2−xSrxZnWO6 series were studied using Ultraviolet–visible (UV–vis) diffuse reflectance and photoluminescence (PL) spectroscopies. The absorption edge of the samples appeared around the near-violet and visible spectra, between 336–360 nm. The band gap energy was investigated in two ways—using the absorption cutoff and Tauc plots—which increased from 3.52 to 3.7 eV with increasing substitution of Ba2+ by Sr2+. Furthermore, excitation and emission spectra were collected at room temperature. A broad band at 260–360 nm appeared in the PLE spectra for all samples, and the PL spectra of the samples had a band that spread from 320–450 nm.

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