Changjiu Sun

Quasi-two-dimensional (quasi-2D) perovskites have attracted extraordinary attention due to their superior semiconducting properties and have emerged as one of the most promising materials for next-generation light-emitting diodes (LEDs). The outstanding optical properties originate from their structural characteristics. In particular, the inherent quantum-well structure endows them with a large exciton binding energy due to the strong dielectric- and quantum-confinement effects; the corresponding energy transfer among different n-value species thus results in high photoluminescence quantum yields (PLQYs), particularly at low excitation intensities. The review herein presents an overview of the inherent properties of quasi-2D perovskite materials, the corresponding energy transfer and spectral tunability methodologies for thin films, as well as their application in high-performance LEDs. We then summarize the challenges and potential research directions towards developing high-performance and stable quasi-2D PeLEDs. The review thus provides a systematic and timely summary for the community to deepen the understanding of quasi-2D perovskite materials and resulting LED devices.

Abstract Rapid Auger recombination represents an important challenge faced by quasi-2D perovskites, which induces resulting perovskite light-emitting diodes’ (PeLEDs) efficiency roll-off. In principle, Auger recombination rate is proportional to materials’ exciton binding energy ( E b ). Thus, Auger recombination can be suppressed by reducing the corresponding materials’ E b . Here, a polar molecule, p -fluorophenethylammonium, is employed to generate quasi-2D perovskites with reduced E b . Recombination kinetics reveal the Auger recombination rate does decrease to one-order-of magnitude lower compared to its PEA + analogues. After effective passivation, nonradiative recombination is greatly suppressed, which enables resulting films to exhibit outstanding photoluminescence quantum yields in a broad range of excitation density. We herein demonstrate the very efficient PeLEDs with a peak external quantum efficiency of 20.36%. More importantly, devices exhibit a record luminance of 82,480 cd m −2 due to the suppressed efficiency roll-off, which represent one of the brightest visible PeLEDs yet.

Abstract Serious performance decline arose for perovskite light-emitting diodes (PeLEDs) once the active area was enlarged. Here we investigate the failure mechanism of the widespread active film fabrication method; and ascribe severe phase-segregation to be the reason. We thereby introduce L-Norvaline to construct a COO − -coordinated intermediate phase with low formation enthalpy. The new intermediate phase changes the crystallization pathway, thereby suppressing the phase-segregation. Accordingly, high-quality large-area quasi-2D films with desirable properties are obtained. Based on this, we further rationally adjusted films’ recombination kinetics. We reported a series of highly-efficient green quasi-2D PeLEDs with active areas of 9.0 cm 2 . The peak EQE of 16.4% is achieved in <n > = 3, represent the most efficient large-area PeLEDs yet. Meanwhile, high brightness device with luminance up to 9.1 × 10 4 cd m −2 has achieved in <n > = 10 film.