Graded Heterojunction Engineering for Hole-Conductor-Free Perovskite Solar Cells with High Hole Extraction Efficiency...

Despite great progress in the photovoltaic conversion efficiency (PCE) of inorganic-organic hybrid perovskite solar cells (PSCs), the large-scale application of PSCs still faces serious challenges due to the poor-stability and high-cost of the spiro-OMeTAD hole transport layer (HTL). It is of great fundamental importance to rationally address the issues of hole extraction and transfer arising from HTL-free PSCs. Herein, a brand-new PSC architecture is designed by introducing multigraded-heterojunction (GHJ) inorganic perovskite CsPbBr_x I_3-x layers as an efficient HTL. The grade adjustment can be achieved by precisely tuning the halide proportion and distribution in the CsPbBr_x I_3-x film to reach an optimal energy alignment of the valance and conduction band between MAPbI₃ and CsPbBr_x I_3-x . The CsPbBr_x I_3-x GHJ as an efficient HTL can induce an electric field where a valance/conduction band edge is leveraged to bend at the heterojunction interface, boosting the interfacial electron-hole splitting and photoelectron extraction. The GHJ architecture enhances the hole extraction and conduction efficiency from the MAPbI₃ to the counter electrode, decreases the recombination loss during the hole transfer, and benefits in increasing the open-circuit voltage. The optimized HTL-free PCS based on the GHJ architecture demonstrates an outstanding thermal stability and a significantly improved PCE of 11.33%, nearly 40% increase compared with 8.16% for pure HTL-free devices.