Strain Release and Defect Passivation in Formamidinium-Dominated Perovskite via a Novel in-Plane Thermal Gradient Assisted Crystallization Strategy.

It is essential to release annealing induced strain during the crystallization process to realize efficient and stable perovskite solar cells (PSCs), which does not seem achievable using the conventional annealing process. Here we report a novel and facile thermal gradient assisted crystallization strategy by simply introducing a slant angle between the preheated hot plate and the substrate. A distinct crystallization sequence resulted along the in-plane direction pointing from the hot side to the cool side, which effectively reduced the crystallization rate, controlled the perovskite grain growth, and released the in-plane tensile strain. Moreover, this strategy enabled uniform strain distribution in the vertical direction and assisted in reducing the defects and aligning the energy bands. The corresponding device demonstrated champion power conversion efficiencies (PCEs) of 23.70% and 21.04% on the rigid and flexible substrates, respectively. These highly stable rigid devices retained 97% of the initial PCE after 1097 h of storage and more than 80% of the initial PCE after 1000 h of continuous operation at the maximum power point. This novel strategy opens a simple and effective avenue to improve the quality of perovskite films and photovoltaic devices via strain modulation and defect passivation.