Dimensionality-Controlled Surface Passivation for Enhancing Performance and Stability of Perovskite Solar Cells via Triethylenetetramine Vapor

Perovskite solar cells (PSCs) have achieved unprecedented progress in terms of enhancement of power conversion efficiency (PCE). Nevertheless, device stability is still an obstacle to the commercialization of this emerging photovoltaic technology. Though strategies such as compositional management and ligand engineering have been reported to tackle this critical issue, these methods often have drawbacks such as compromised device performance. Herein, we propose an approach combining material dimensionality control and interfacial passivation by a post-device treatment via triethylenetetramine (TETA) vapor to enhance both efficiency and stability of Cs0.05FA0.79MA0.16PbI2.5Br0.5-based PSCs. Results of X-ray diffraction and scanning electron microscopy show the formation of low-dimensional perovskites at the interface between the perovskite film and the hole transporting layer after the TETA vapor treatment. Measurements of the energy level alignment and electrochemical properties by ultraviolet photoelectron spectroscopy and impedance spectra confirm the reduced density of trap states and improved interfacial charge transport. Consequently, TETA-based treatment significantly enhances both efficiency (from 17.07 to 18.03%) and stability (PCE retention from 73.4 to 88.9%) of the PSCs under >65% relative humidity for 1000 h compared to the controlled device without TETA treatment. Furthermore, the TETA vapor also shows an advantageous effect of dramatically improving the performance of PSC devices, which initially had poor performance (from 6.8 to 10.5%) through surface defect passivation.