Impact of Amine Additives on Perovskite Precursor Aging: A Case Study of Light-Emitting Diodes

Amines are widely employed as additives for improving the performance of metal halide perovskite optoelectronic devices. However, amines are well-known for their high chemical reactivity, the impact of which has yet to receive enough attention from the perovskite light-emitting diode community. Here, by investigating an unusual positive aging effect of CH3NH3I/CsI/PbI2 precursor solutions as an example, we reveal that amines gradually undergo N-formylation in perovskite precursors over time. This reaction is initialized by hydrolysis of dimethylformamide in the acidic chemical environment. Further investigations suggest that the reaction products collectively impact perovskite crystallization and eventually lead to significantly enhanced external quantum efficiency values, increasing from similar to 2% for fresh solutions to greater than or similar to 12% for aged ones. While this case study provides a positive aging effect, a negative aging effect is possible in other perovksite systems. Our findings pave the way for more reliable and reproducible device fabrication and call for further attention to underlying chemical reactions within the perovskite inks once amine additives are included. Funding Agencies|ERCEuropean Research Council (ERC)European Commission [717026]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [SFO-Mat-LiU 2009-00971]; National Natural Science Foundation of ChinaNational Natural Science Foundation of China (NSFC) [51472164, 62005126]; 1000 Talents Program for Young Scientists of China; Shenzhen Peacock Plan [KQTD2016053112042971]; Educational Commission of Guangdong Province [2015KGJHZ006]; Research Foundation-Flanders (FWO)FWO [12Y7221N]