Insights into the electronic structure, optical properties, and photocatalytic potential of Gd2CoCrO6 perovskite: a comprehensive theoretical and experimental investigation†

Abstract

In this study, we present a comprehensive theoretical and experimental investigation into the electronic structure, optical properties, and photocatalytic potential of Gd₂CoCrO₆ (GCCO) double perovskite. Using first-principles calculations with the generalized-gradient-approximation plus Hubbard U (GGA + U) method, we explored the effects of Coulomb interactions on the electronic properties. Our calculations revealed that GCCO exhibits a half-metallic nature, displaying metallic behavior for up-spin and semiconducting behavior for down-spin states. The optimized U_eff value of 4.2 eV accurately reproduces the direct bandgap of 2.25 eV, which aligns closely with experimental results obtained through UV-visible absorption spectroscopy and photoluminescence analysis. Additionally, time-resolved photoluminescence (TRPL) measurements indicate a mean charge carrier lifetime of 2.37 ns, suggesting effective charge separation. Mott–Schottky analysis and valence band X-ray photoelectron spectroscopy (XPS) confirm the n-type semiconducting nature of GCCO with favorable band edge positions for redox reactions. The combination of theoretical insights and experimental characterization indicates that GCCO holds significant promise as a photocatalyst for applications in renewable energy production and environmental remediation, particularly in solar-driven water splitting and pollutant degradation. Our study provides crucial insights into the electronic structure and optical properties of double perovskites like GCCO, highlighting their suitability for photocatalytic applications. Furthermore, the research paves the way for future work in the compositional engineering and defect modulation of double perovskites to optimize their photocatalytic efficiency.