The Role of Water in the Reversible Optoelectronic Degradation of Hybrid Perovskites at Low Pressure

There is no doubt about the potential offered by the low-cost fabrication and high efficiency of hybrid organic inorganic perovskite solar cells. However, the service lifetimes of these devices must be increased from months to years to capitalize on their potential. The archetypal hybrid perovskite for solar cells, methylammonium lead iodide (CH3NH3PbI3, abbreviated MAPI), readily degrades in ambient atmosphere under standard operating conditions. Understanding the origin and effects of this degradation can pave the way to better engineer photovoltaic devices and the perovskite material itself. Herein we present the effects of varying pressure on the electrical performance of MAPI solar cells. Solar cell parameters, especially open circuit voltage, are significantly affected by the total ambient pressure and present an unexpected reversible behavior upon pressure cycling. We complement photoluminescence studies as a function of ambient atmosphere and temperature with first principles density functional theory (DFT) calculations. The results suggest that the reversible intercalation of water in MAPI is a necessary component underlying this behavior.