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Abstract

By means of the first-principles density functional theory (DFT), I2-II-IV-VI4 type Cu-based quaternary chalcogenides Cu 2 XSiS 4 (X = Ge, Sn, and Pb) have been thoroughly investigated. We report the study of Ge and Sn substitution in the divalent cation site for their potential applications in photovoltaics for the first time. The structural, electronic, optical, and mechanical properties have been calculated. The structural and thermal stability is verified by calculating the elastic constants, formation energy and total potential energy at 300 K from the ab-initio molecular dynamics (MD) simulation. The compounds under our investigation exhibited an indirect band gap in the range of 1.0--1.56 eV, suitable for energy harvesting by trapping the sunlight. The presence of absorption peaks within the visible region complements their potential in photovoltaic applications. For further validation, we have designed a model of a heterostructure (FTO/TiO2/Cu2XSiS4/CuO/Au) solar cell, and a numerical simulation has been performed by solving the Poisson equation and continuity equations to obtain the I-V characteristic by using SCAPS-1D. All the inputs needed for solar- cell simulation in SCAPS-1D have been taken from the DFT results. The corresponding Power Conversion Efficiency (PCE) is denoted by {\eta}% and their respective values for X=Ge, Sn and Pb are 23.46%, 23.29% and 22.60%, at room temperature. The Ge-based system exhibits the highest {\eta}%, owing to its band gap value in the visible range of the solar spectrum. Thus, we report that Ge-based compounds may act as a promising absorber layer in heterostructure solar-cell applications.