Inelastic Deformation in Methylammonium Lead Iodide Perovskite and Mitigation by Additives during Thermal Cycling

Metal halide perovskite thin films are promising materials for next-generation photovoltaic applications, but the thermomechanical instabilities of these materials are critical barriers to device longevity. In this study, we measure the evolution of stresses in methylammonium lead iodide (MAPbI3) films thermally cycled from 25 to 105 °C using a multibeam optical stress sensor (MOSS) system. We demonstrate that these films undergo residual stress buildup due to inelastic deformation as well as a simple mitigation strategy by incorporating low concentrations of 5-aminovaleric acid hydrochloride (5-AVACl) as an additive. Adding 5-AVACl increases the tensile stresses measured at room temperature but beneficially decreases the biaxial modulus from 9.60 ± 0.44 GPa to 7.95 ± 0.55 GPa, resulting in greater accommodation of thermal stresses. The hysteresis loop is ∼63% smaller with the inclusion of 5-AVACl, and the stress relaxation at 50 °C decreases from 86.46 to 51.49 MPa. The larger stress relaxation in pristine MAPbI3 is correlated with grain boundary opening after five cycles, while the inclusion of 5-AVACl mitigates this degradation. Our findings underscore the importance of studying the dynamic response of perovskite films during thermal cycling and lay the foundation for further exploration into the mechanisms governing the thermomechanical behavior of perovskite thin films.