Quasi-two-dimensional (quasi-2D) perovskite-based light-emitting diodes (PeLEDs) have attracted intensive attention due to their high quantum yields, tunable emission wavelengths, and solution-processing capability, showing great potential in next-generation display and lighting applications. However, further performance enhancement in PeLEDs is severely limited by the uncontrolled transfer of charge carriers under bias, leading to crowding of interfacial carriers and severe efficiency roll-off. Herein, we insert an ultra-thin dielectric buffer layer of lithium fluoride (LiF) into the electron transport layer (ETL) to regulate the transfer dynamics of electrons and passivate the interfacial defects simultaneously. The dielectric LiF interlayer can effectively reduce the efficiency roll-off in PeLEDs by improving the charge balance through preventing the overwhelming injection of electrons. Moreover, the fluoride anions from LiF can passivate the surface defects of the perovskite film, enhancing the radiative recombination. As a result, the LiF interlayer-assisted quasi-2D PeLED presents an outstanding external quantum efficiency (EQE) of 24.03% and a maximum brightness of 30 845 cd m−2. The operational stability of the device is also extended, with a half-lifetime (T50) of 71.28 min (at an initial luminance of 1 000 cd m−2), which is 7.4-fold longer than that for the control device.Graphical
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