Suchergebnisse

One of the most critical challenges in perovskite light-emitting diodes (PeLEDs) lies in poor operational stability. Although field dependent ion migration is believed to play an important role in the operation of perovskite optoelectronic devices, a complete understanding of how it affects the stability of PeLEDs is still missing. Here, we report a unique self-repairing behavior that the electroluminescence of moderately degraded PeLEDs can almost completely restore to their initial performance after resting. We find that the accumulated halides within the hole transport layer undergo back diffusion toward the surface of the perovskite layer during resting, repairing the vacancies and thus resulting in electroluminescence recovery. These findings indicate that one of the dominant degradation pathways in PeLEDs is the generation of halide vacancies at perovskite/hole transport layer interface during operation. We thus further passivate this key interface, which results in a high external quantum efficiency of 22.8% and obviously improved operational stability. ; Funding Agencies|ERCEuropean Research Council (ERC)European Commission [717026]; Swedish Energy Agency EnergimyndighetenSwedish Energy Agency [48758-1]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009-00971]; DFGGerman Research Foundation (DFG)European Commission [SPP 2196, 424216076]; China Scholarship CouncilChina Scholarship Council [201906830040]; Nanjing University of Aeronautics and Astronautics PhD short-term visiting scholar project [180608DF06]; Priority Academic Program Development of Jiangsu Higher Education Institutions; Swiss Federal Office of Energy (SFOE)-BFE [SI/501805-01]

Multidentate molecular additives are widely used to passivate perovskite, yet the role of chelate effect is still unclear. Here, the authors investigate a wide range of additives with different coordination number and functional moieties to establish correlation between coordination affinity and perovskite crystallisation dynamics. Molecular additives are widely utilized to minimize non-radiative recombination in metal halide perovskite emitters due to their passivation effects from chemical bonds with ionic defects. 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-emitting diodes (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 inhibiting 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 such, we open new prospects for the rationalized screening of highly effective molecular additives. ; Funding Agencies|ERC Starting GrantEuropean Research Council (ERC) [717026]; Swedish Energy Agency EnergimyndighetenSwedish Energy Agency [48758-1, 44651-1]; Swedish Research Council VRSwedish Research Council; NanoLund; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009-00971]; National Natural Science Foundation of ChinaNational Natural Science Foundation of China (NSFC) [91833303, 61974098, 62005126]; National Key Research and Development Program [2016YFA0201900]; Jiangsu High Educational Natural Science Foundation [18KJA430012]; 111 ProgramMinistry of Education, China - 111 Project; Collaborative Innovation Center of Suzhou Nano Science and Technology; Collaborative Innovation Center of Suzhou Nano Science Technology; Research Foundation - Flanders (FWO)FWO [12Y7218N, 12Y7221N, G098319N]; KU Leuven Research FundKU Leuven [C14/19/079, 201806920071, 201906830040, 201608530162, 201806460021]; China Scholarship CouncilChina Scholarship Council