Efficiency Gain of 9.22% by Dual Hole-Transport Layer Engineering for High-Performance 2D/3D Perovskite Solar Cells: SCAPS-1D Numerical Study
摘要
Two-/three-dimensional (2D/3D) perovskite solar cells combine strong light absorption with excellent charge transport; however, their device performance remains highly sensitive to interfacial recombination and imperfect energy level alignment. In this work, we evaluate a dual-hole-transport-layer (HTL) strategy for this kind of perovskite stack based on MAPbI3 and a thin PEA2PbI4 2D capping layer using SCAPS-1D. A broad screening of organic and inorganic dual HTLs is conducted, with emphasis on HTL ordering and its impact on band alignment and carrier extraction. The simulations show that HTL ordering is decisive, and that placing an inorganic HTL adjacent to the perovskite while keeping Spiro-OMeTAD as the outer HTL can reduce interfacial losses and increase the fill factor and current density. Among the tested combinations and optimization strategies, the CuO/Spiro-OMeTAD bilayer provides the highest simulated performance, reaching peak power conversion efficiency of 29.97% under the chosen model parameters. Analysis of the 2D/3D interface defect density (Nt) of the optimal dual-HTL (CuO/Spiro-OMeTAD) device in terms of open-circuit voltage (Voc) sensitivity, thermodynamic efficiency limits, and recombination kinetics reveals a defect-tolerant regime of Nt ≤ 1012 cm−2, with a critical threshold of Nt = 1015 cm−2, identified as the practical limit to prevent significant Voc degradation. These results establish practical design rules for dual-HTL selection and thickness optimization in 2D/3D perovskite devices.
Graphical Abstract