Triphenylamine-based interlayer with carboxyl anchoring group for tuning of charge collection interface in stabilized p-i-n perovskite solar cells and modules

A novel triphenylamine-based hole transport material (HTM) with a carboxyl anchoring group (TPATC) was developed for tuning the interface between nanocrystalline NiO and double cation CsCH3(NH2)2PbI3-xClx absorber in p-i-n device architectures. We present a unique comprehensive confinement study of PSCs with TPATC as the self-assembled HTM, including analysis of numerical defect parameters, phase composition evolution, and up-scaling capabilities. Our investigation shows that the ultrathin TPATC interlayer effectively passivates traps, increases work-function of HTL by about ~0.2 eV, and enhances the charge carrier extraction efficiency. Advanced transient spectroscopy measurements revealed that modification of the NiO surface with TPATC in perovskite solar cells (PSCs) reduces the concentration of ionic defects by an order of magnitude. Interface engineering with TPATC allowed to reach power conversion efficiency of 20.58% for small area devices (0.15 cm2) under standard AM 1.5 G conditions. Using TPATC interlayer also provided stabilized performance of PSCs under operation conditions and improved sustainability of the perovskite absorber to decomposition. After continuous light-soaking (1000 h, ISOS-L-2 protocol), NiO/TPATC devices showed a slight decrease of 2% in maximum power. In contrast, NiO PSCs demonstrated decrease in power output (>20%) after 400 h. We explored the potential of TPATC to modify interfaces in large-area perovskite solar modules (PSM, active area-64.8 cm2, 12 sub-cells). By applying slot-die-coated TPATC, the PCE at AM 1.5 G conditions increased from 13.22% for NiO PSM to 15.64% for NiO/TPATC ones. This study provides new insights into the interface engineering for p-i-n perovskite solar cells, behavior of the ionic defects and their contribution to the long-term stability.