Highly Efficient and Stable Perovskite Solar Cells via Modification of Energy Levels at the Perovskite/Carbon Electrode Interface

Perovskite solar cells (PSCs) have attracted great attention in the past few years due to their rapid increase in efficiency and low‐cost fabrication. However, instability against thermal stress and humidity is a big issue hindering their commercialization and practical applications. Here, by combining thermally stable formamidinium–cesium‐based perovskite and a moisture‐resistant carbon electrode, successful fabrication of stable PSCs is reported, which maintain on average 77% of the initial value after being aged for 192 h under conditions of 85 °C and 85% relative humidity (the “double 85” aging condition) without encapsulation. However, the mismatch of energy levels at the interface between the perovskite and the carbon electrode limits charge collection and leads to poor device performance. To address this issue, a thin‐layer of poly(ethylene oxide) (PEO) is introduced to achieve improved interfacial energy level alignment, which is verified by ultraviolet photoemission spectroscopy measurements. Indeed as a result, power conversion efficiency increases from 12.2% to 14.9% after suitable energy level modification by intentionally introducing a thin layer of PEO at the perovskite/carbon interface. A thin layer of polyethylene oxide (PEO) is introduced to modify the energy level alignment at the interface between an FA0.8Cs0.2PbI2.64Br0.36 perovskite and a carbon electrode. The PEO‐modified perovskite cell shows 22% increase in power conversion efficiency and enhanced stability keeping 77% of the initial value after being aged for 192 h under the conditions of 85 °C and 85% humidity without encapsulation.