Disentangling the origin of degradation in perovskite solar cells via optical imaging and Bayesian inference

Abstract

Machine learning and computational inference, coupled with experimental data, promise to significantly accelerate our rate of learning in most scientific disciplines. In this study, we develop tools that connect microscopic observations to macroscopic device behaviour, a capability that is essential for accelerating the design of durable energy materials. To this end, we introduce a novel approach that integrates photoluminescence imaging with drift diffusion simulations to understand operation and degradation in fully fabricated perovskite solar cells. By employing Bayesian inference, we generate "inferred maps" of parameters that govern recombination processes present in devices. We track these parameter maps while the devices are aged (70 {\deg}C, full spectrum sunlight) to analyse their temporal evolution during degradation. Notably, our approach allows us to distinguish between degradation occurring at the hole or electron transporting layer interface, or within the bulk. Our analysis reveals pronounced spatially non-uniform degradation, with significant macroscopic heterogeneity observed in the optoelectronic parameter maps. We pinpoint the greatest degradation observed in specific regions to stem from the perovskite/transport layer interfaces. Finally, we demonstrate that an amino-silane molecular passivation treatment suppresses this degradation, highlighting its specific role in enhancing device stability. Our approach offers valuable insights for future device fabrication and is a clear exemplification of how advanced Bayesian inference can significantly increase the value of experimental data.