Proceedings of 13th Conference on Hybrid and Organic Photovoltaics (HOPV21)
Publication date: 11th May 2021
Introducing molecular additives into perovskite precursors has become one of the most effective and prevailing strategies to improve the performance of metal halide perovskite optoelectronic devices, which recently has boosted the external quantum efficiency (EQE) of perovskite light-emitting diodes (PeLEDs) to above ~20%1,2. The performance enhancement results from suppressed non-radiative recombination which is generally believed to be associated with defect passivation – surface dangling bonds in perovskites are said to be healed by additional coordination or ionic bonding with the additives, leading to the annihilation of trap states. Accordingly, a wide range of passivating molecular additives have been investigated for PeLEDs, especially those containing Lewis base moieties such as amino- and carboxyl-functionalized molecules However, a general and puzzling observation that can hardly be rationalized by passivation alone is that most of the molecular additives enabling high-efficiency perovskite light-PeLEDs are chelating (multidentate) molecules, while their respective monodentate counterparts receive limited attention. Here, we reveal the largely ignored yet critical role of the chelate effect on governing crystallization dynamics of perovskite emitters and mitigating trap-mediated non-radiative losses. Specifically, we discover that the chelate effect enhances lead-additive coordination affinity, enabling the formation of thermodynamically stable intermediate phases and inhibition of halide coordination-driven perovskite nucleation. The retarded perovskite nucleation and crystal growth are key to high crystal quality and thus efficient electroluminescence. Our work elucidates the full effects of molecular additives on PeLEDs by uncovering the chelate effect as an important feature within perovskite crystallization, as well as opening new prospects for the rationalized screening of highly effective molecular additives.
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