Interface Regulation by an Ultrathin Wide-Bandgap Halide for Stable and Efficient Inverted Perovskite Solar Cells

The nonradiative recombination between hole transport layers (HTLs) and perovskites generally leads to obvious energy losses. The trap states at the HTL/perovskite interface directly influence the improvement of the power conversion efficiency (PCE) and stability. Interface regulation is a simple and commonly used method to decrease nonradiative recombination in inverted perovskite solar cells (PSCs). Here, a wide-bandgap halide was used to regulate the PTAA/MAPbI₃ interface, in which n-hexyltrimethylammonium bromide (HTAB) was used to modify the upper surface of poly[bis(4-phenyl)-(2,4,6-trimethylphenyl)amine] (PTAA). Upon introduction of the HTAB layer, the contact between PTAA and MAPbI₃ is strengthened, the defect state density in PSCs is reduced, the MAPbI₃ crystallinity is improved, and the nonradiative recombination loss is suppressed. The device with HTAB delivers the highest PCE of 21.01% with negligible hysteresis, which is significantly higher than that of the control device (17.71%), and it maintains approximately 87% of its initial PCE for 1000 h without encapsulation in air with a relative humidity of 25 ± 5%. This work reveals an effective way of using a wide-bandgap halide to regulate the PTAA/MAPbI₃ interface to simultaneously promote the PCE and stability of PSCs.