Mathematical Modeling and performance analysis of Zr-Based chalcogenide perovskites with kesterite and zinc based charge transport layers

Lead-based components in perovskite solar cells (PSCs) raise environmental and health concerns, promoting research interest in lead-free alternatives. This study introduces four novel architectures for a lead-free PSC using CaZrS3 as the absorber layer, with a unique nip heterostructure incorporating kesterite (CBTS, CMTS, CNTS, CZTS) as hole transport layers (HTLs) and zinc oxide (IGZO) as electron transport Layer (ETL). The device configuration (FTO/IGZO/CaZrS3/HTL/Se) was initially simulated using the SCAPS-1D under standard AM 1.5G illumination without optimization. Pre-optimization results showed promising power conversion efficiencies (PCE) of 22.26 %, 18.55 %, 20.94 %, and 18.43 % for CBTS, CMTS, CNTS, and CZTS respectively, marking the highest recorded performances for CaZrS3-based cells to date. Subsequent optimization of the ETL and HTLs thickness and doping, along with the absorber layer, further enhanced the PCEs to 25.26 %, 19.01 %, 22.72 %, and 19.03 % respectively. Detailed analyses of the energy alignment of charge transport layers (CTL) with CaZrS3 were conducted to elucidate the operational principles of these configurations. Furthermore, with this unique device architecture this study is the first to explore the impacts of layer thickness, doping levels, defect density, interface defects, temperature and electrode variation on device performance. Among all configurations simulated, the FTO/IGZO/CaZrS3/CBTS/Se structure demonstrated exceptional performance, achieving a Jsc of 15.24 mA/cm2, Voc of 1.61 V, FF of 91.50 %, and a PCE of 22.56 %. These theoretical findings offer valuable insights for the fabrication of highly efficient and environmentally friendly PSC, potentially guiding future experimental research.