在高效稳定的2D/3D钙钛矿太阳能电池中实现接近辐射极限的准费米能级分裂：详细平衡模型

Abstract Three-dimensional (3D) perovskite solar cells (PSCs) are renowned for their high-power conversion efficiencies (PCEs), yet they face challenges related to performance and stability. This study introduces a new Dion-Jacobson (DJ) 2D-3D lead-free perovskite solar cell (PSC) design with an optimized hole transport layer, reaching a power conversion efficiency (PCE) of 17.32 %. The enhanced performance is primarily attributed to the incorporation of a suitable hole transport layer (HTL), with a slight additional boost from the quantum confinement effect in the 2D DJ perovskite, which also contributes to improved stability. Together, these factors contribute to increased short-circuit current density ( J SC ) and open-circuit voltage ( V OC ). Notably, our optimized device exhibits a Quasi-Fermi level splitting ( QFLS ) of 1.15 eV and a photoluminescence quantum yield ( PLQY ) of 7.08 × 10 -2 , compared to 0.95 eV and 3.07 × 10 -5 for conventional 3D PSCs . Capacitance measurements indicate that PTAA as an HTL achieves the highest capacitance at 19.5 nF/cm 2 , while NiO provides superior overall efficiency. Mott-Schottky analysis further reveals that the device with NiO HTL exhibits the highest built-in potential and optimal performance at voltages exceeding 1 V. These findings highlight the effectiveness of combining DJ 2D perovskites with appropriate HTL materials to enhance both the performance and stability of lead-free PSCs , paving the way for future advancements in sustainable solar energy technologies.