Optoelectronic properties and performance optimization for photovoltaic applications of R3m-RbGeX$_3$ (X = Cl, Br, I) perovskites: A combined DFT and SCAPS-1D study

Abstract: In pursuit of an all-inorganic non-toxic perovskite solar cell (PSC) with enhanced performance, we have investigated the rhombohedral phase of the germanium-based rubidium halide perovskites RbGeX$_3$ (X = Cl, Br, I). The structural analysis followed by an in-depth study of the electronic and optical properties of these materials is performed within the framework of density functional theory (DFT). A detailed investigation of the electronic properties is carried out by examining the band structure and partial density of states (PDOS). PBE and TB-mBJ exchange-correlation functionals are used with and without the spin-orbit coupling (SOC), thereby obtaining accurate predictions of the band gaps. The key optical properties such as the real and imaginary parts of the dielectric function, absorption coefficient and refractive index are studied using PBE functional and compared among the three halides. RbGeI$_3$ exhibits the lowest band gap of 0.96 eV with the TB-mBJ + SOC functional, along with the most favorable optical properties, hence, it was identified as the most suitable candidate for the absorber layer (AL) of the PSC. SCAPS-1D simulation is performed using various input parameters for the AL such as the band gap, the effective densities of states for the conduction and valence bands and the electron and hole mobilities extracted from the DFT calculation. Performance optimization is done by exploring the impact of different inorganic hole transport layers (HTLs) and electron transport layers (ETLs). The impact of different layer thicknesses, doping densities, defect densities at the AL, ETL/AL, and AL/HTL interfaces, various back contacts, and the influence of series and shunt resistance on the overall device performance are studied. The optimized all-inorganic device demonstrated a remarkable power conversion efficiency (PCE) of $25.76\%$ with a fill factor (FF) of $79.81\%$.