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Study of the Effect of Gallium Replacement by Thallium in CuGa(1-x)TlxS2 Structure by First-Principles Calculations on CASTEP

A natural extension of the zinc-blende compounds from which they crystallographically derive, chalcopyrites are of great interest to the scientific community. Indeed, this family of compounds has many applications, from optoelectronics to diiodes electroluminescence. In order to improve their properties, the current study employs first-principles calculations using the CASTEP software to investigate the effect of gallium substitutional by thallium atoms (TlGa) in the CuGaS2 (CGS) chalcopyrite structure. The effect, including structural, electrical and optical properties was studied. Several representatives semiconductors CuGa(1-x)TlxS2 were studied, x represents the atomic ratio of Thallium taken from 0 to 40. Properties, convergence of the cutoff energy and the K-mesh were carried out based on first-principles calculations of density functional theory (DFT). The optimized cutoff energy and the optimized K-mesh was found to be 420 eV, 6 6 3 respectively. The results show that, TlGa doping induced intermediate band (IB), which can be ascribed to donors’ states. That results in a shift of the conduction band minimum (CBM) of CGS towards lower energies. When increasing Tl atomic ratio, the band gap energy decreases from 0.758 (x=0) to 0.172 eV (x=0.40). From optical properties study, CuGa0.78Tl0.22S2, CuGa0.67Tl0.33S2, CuGa0.60Tl0.40S2 showed high absorption coefficient in visible light range, at ca. 1.5 eV. These results suggest that the substitution of Ga by Tl can significantly impact the optical and electrical properties of compounds may have potential applications in photovoltaic, photocatalytic and optoelectronic devices.

First-principles Calculations, Doping, Chalcopyrite Structure, Intermediate Band, Band Gap Energy, Absorption Coefficient

Sangare Kassoum, Diomande Sékou, Bede Affoué Lucie. (2023). Study of the Effect of Gallium Replacement by Thallium in CuGa(1-x)TlxS2 Structure by First-Principles Calculations on CASTEP. International Journal of Materials Science and Applications, 12(5), 67-74.

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