This study explores the morphological, optical, structural, mechanical, and radiation-shielding properties of borosilicate glass–ceramic samples modified with titanium oxide and various ratios of barium oxide. The morphology of the glass–ceramic system was investigated using scanning electron microscopy (SEM). The mechanical properties, Raman spectroscopy, Fourier transform infrared (FTIR) spectroscopy, and X-ray diffraction (XRD) were used to identify the fabricated sample structures. The optical properties were calculated to define the refractive index and band gap (Eg). The shielding properties were obtained by Monte Carlo simulation (MC) and compared with XCOM software data. Glass samples were converted to glass–ceramic samples at 800 °C for 6 h, and the GC25 and GC30 samples were converted to completely crystalline phases as illustrated by the XRD, FTIR, and Raman results, unlike the GC15 and GC20 samples. The XRD results showed the trigonal structure of BaB2TiO6 with the R-3 space group for the GC25 and GC30 samples and the tetragonal phase of TiO2 with the P42/mnm space group for the GC15 and GC20 samples. The sharp FTIR and Raman spectrum peaks affirm the crystal phase for G25 and G30 samples. The parent glass of the GC20 sample showed the highest mechanical moduli (Young's, bulk, shear, and longitudinal) and Poisson ratio. Concurrently, the addition of BaO instead of B2O3 caused a gradual reduction in the packing factor, dissociation energy, and microhardness. The Phy-X program was used to theoretically assess the shielding properties. The obtained results showed the highest compatibility between the Monte Carlo N-particle (MCNP) and XCOM software results, and the GC30 sample displayed the highest shielding properties due to adding BaO instead of B2O3. The crystalline phase and shielding features of the samples were improved by increasing the BaO ratio, indicating that the current samples are suitable for radiation-shielding applications.
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