Spray-coated lead-free CsSnBr3 all-inorganic perovskites for efficient solar cells: A combined experimental and theoretical approach
摘要
Lead-based halide perovskite solar cells have demonstrated outstanding power conversion efficiencies; however, lead toxicity and challenges associated with large-area fabrication hinder their commercial deployment. In this study, a novel all-inorganic, lead-free n-i-p perovskite solar cell architecture FTO/TiO2/CsSnBr3/CuSCN/carbon, is systematically investigated through a combination of numerical simulations and experimental validation, with the CsSnBr3 layer deposited using a one-step spray-coating technique. Numerical optimization identifies optimal TiO2 and CuSCN thicknesses of 30 nm and 150 nm, respectively. The effects of absorber thickness and total defect density are analyzed, revealing an optimal CsSnBr3 thickness of 700 nm with a defect density of 1014 cm−3. Interface defect analysis shows that the absorber/HTL interface exhibits lower defect tolerance than the absorber/ETL interface. Charge generation and recombination dynamics are examined to elucidate the device operating mechanisms, with the optimized simulated device achieving a power conversion efficiency of 16.03%. Experimentally, the optical, structural, morphological and chemical properties of pristine and annealed CsSnBr3 films are systematically characterized. Annealing at 120 °C enhances visible light absorption, improves crystallinity and crystallite size, and results in a uniform, pinhole-free morphology, while X-ray photoelectron spectroscopy confirms the expected oxidation states of Cs, Sn, and Br. The fabricated device achieves a power conversion efficiency of 1.09%, with an open-circuit voltage of 0.40 V, a short-circuit current density of 4.01 mA cm−2, and a fill factor of 68% under 1-sun illumination, retaining approximately 95% photocurrent stability over 80 s. These results highlight the promise of CsSnBr3-based lead-free perovskite solar cells for sustainable photovoltaic applications.