Abstract
In recent years, chalcogenide perovskites have emerged as promising candidates with favorable structural, electrical, and optical properties for photovoltaic applications. This paper explores the structural, electronic, and optical characteristics of ABSe(3) perovskites (where A = Li, Na, K, Rb, Cs; B = Si, Ge, Sn) in their triclinic crystallographic phases using density functional theory. The stability of these materials is ensured by calculating formation energies, tolerance factors (T(f)), and phonon dispersion. The E(form) values of all ABSe(3) are negative, suggesting favorable thermodynamic stability. The T(f) values range between 0.82 and 1.1, which is consistent with stable perovskites. The phonon dispersion analysis of the chalcogenide perovskites revealed no imaginary frequencies in any of the vibrational modes, confirming their stability. The electronic band structures and corresponding density of states are computed to unveil the semiconducting nature of the studied compounds. These perovskites are promising for high-performance solar cells due to their indirect bandgaps (E(g), 1.10-2.33 eV) and a small difference between these indirect and direct gaps (0.149-0.493 eV). The E(g) values increase as the ionic radii of A-site elements increase (Li < Na < K < Rb < Cs). At the B-site, Si-based chalcogenides have the largest E(g) values, followed by Sn-based and then Ge-based materials. Furthermore, optical properties such as the real part and imaginary part of the dielectric function, refractive index extinction coefficient, optical conductivity, absorption coefficient, reflectivity, and energy loss are predicted within the energy range of 0-50 eV. Several ABSe(3) materials, particularly LiGeSe(3) and NaGeSe(3), demonstrated optical properties comparable to both traditional and emerging materials, suggesting their potential for effective use in solar cells.