Decoding recombination dynamics in perovskite solar cells: an in-depth critical review

Abstract

The remarkable optoelectronic properties of metal halide perovskites (MHPs) have established them as highly promising photovoltaic absorber materials, propelling the rapid advancement of perovskite solar cells (PSCs) that outperform many traditional alternatives in terms of power conversion efficiency (PCE). However, despite their advancements, PSC devices encounter significant non-radiative recombination losses, encompassing trap-assisted (Shockley–Read–Hall) recombination in bulk and interfaces of PSCs, which restricts their open-circuit voltage (V_OC) and overall PCE, dragging it below the Shockley–Queisser (SQ) limit. The ongoing debate regarding the role of grain boundary (GB) recombination, whether it primarily manifests as bulk or surface recombination, has spurred extensive research aimed at elucidating these mechanisms. This review provides a critical comprehensive analysis of the thermodynamic correlations related to V_OC losses, bridging the gap between the theoretical SQ limit and practical device performance. Subsequently, it delves into recent findings that aim to decipher the multifaced nature and origin of radiative and non-radiative recombination-induced losses within the device stack, assessing their impacts on overall performance. Furthermore, this review emphasizes the application of advanced machine learning techniques to discern dominant recombination mechanisms in PSCs. Finally, it summarizes the notable advanced strategies to mitigate undesirable non-radiative recombination losses, which pave the way to the thermodynamic efficiency limit.