Owing to the enlarged exciton binding energy and the ability to confine charge carriers compared to their three-dimensional (3D) counterparts, research on quasi-two-dimensional (quasi-2D) perovskite materials and the correlative application in light-emitting diodes (LEDs) has attracted considerable attention. However, high density of defects, exciton emission trapping, and unbalanced charge injection are still the main intractable obstacles to their further development and practical application. Herein, we report an efficient multifunctional interlayer, lithium fluoride (LiF), to boost the performance of green-emitting quasi-2D perovskite LEDs (PeLEDs) by simultaneously overcoming the aforementioned issues. The introduced LiF interlayer not only eliminates the defects at perovskite grain boundaries and the surface by reinforcing the chemical bonds with uncoordinated lead ions but also restrains the emission of perovskite from quenching triggered by the electron transport layer and reduces excess electron injections to effectively balance carriers in the device. As a result, the resulting green quasi-2D PeLED shows a maximum external quantum efficiency of 16.35%, which is the best value obtained for quasi-2D perovskite-based LEDs reported so far, with simultaneous improvement in the operating lifetime of the device.
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