Universal Molecular Control Strategy for Scalable Fabrication of Perovskite Light-Emitting Diodes.

Despite the rapid progress in perovskite light-emitting diodes (PeLEDs), the electroluminescence performance of large-area perovskite devices lags far behind that of laboratory-size ones. Here, we report a 3.5 cm × 3.5 cm large-area PeLED with a record-high external quantum efficiency of 12.1% by creating an amphipathic molecular interface modifier of betaine citrate (BC) between the perovskite layer and the underlying hole transport layer (HTL). It is found that the surface wettability for various HTLs can be efficiently improved as a result of the coexistence of methyl and carboxyl groups in the BC molecules that makes favorable groups to selectively contact with the HTL surface and increases the surface free energy, which greatly facilitates the scalable process of solution-processed perovskite films. Moreover, the luminous performance of perovskite emitters is simultaneously enhanced through the coordination between C═O in the carboxyl groups and Pb dangling bonds.

Mixed-Dimensional MXene-Based Composite Electrodes Enable Mechanically Stable and Efficient Flexible Perovskite Light-Emitting Diodes.

Significant advancements in perovskite light-emitting diodes (PeLEDs) based on ITO glass substrates have been realized in recent years, yet the overall performance of flexible devices still lags far behind, mainly being ascribed to the high surface roughness and poor optoelectronic properties of flexible electrodes. Here, we report efficient and robust flexible PeLEDs based on a mixed-dimensional (0D-1D-2D-3D) composite electrode consisting of 0D Ag nanoparticles (AgNPs)/1D Ag nanowires (AgNWs)/2D MXene/3D poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS). Our designed MXene-based electrodes combine the advantages of facile formation of a film of low-dimensional materials and excellent optical and electrical properties of metal, inorganic, and organic semiconductors, which endow the electrodes with high electrical/thermal conductivity, flexibility, a smooth surface, and good transmittance. Consequently, the resulting flexible PeLEDs (without a light-coupling structure) demonstrate a record external quantum efficiency of 16.5%, a high luminance of close to 50000 cd/m2, a large emitting area of 8 cm2, and significantly enhanced mechanical stability.

Smoothing the energy transfer pathway in quasi-2D perovskite films using methanesulfonate leads to highly efficient light-emitting devices.

Quasi-two-dimensional (quasi-2D) Ruddlesden-Popper (RP) perovskites such as BA2Csn-1PbnBr3n+1 (BA = butylammonium, n > 1) are promising emitters, but their electroluminescence performance is limited by a severe non-radiative recombination during the energy transfer process. Here, we make use of methanesulfonate (MeS) that can interact with the spacer BA cations via strong hydrogen bonding interaction to reconstruct the quasi-2D perovskite structure, which increases the energy acceptor-to-donor ratio and enhances the energy transfer in perovskite films, thus improving the light emission efficiency. MeS additives also lower the defect density in RP perovskites, which is due to the elimination of uncoordinated Pb2+ by the electron-rich Lewis base MeS and the weakened adsorbate blocking effect. As a result, green light-emitting diodes fabricated using these quasi-2D RP perovskite films reach current efficiency of 63 cd A-1 and 20.5% external quantum efficiency, which are the best reported performance for devices based on quasi-2D perovskites so far.

Boosting the Efficiency of NiOx-Based Perovskite Light-Emitting Diodes by Interface Engineering.

Nickel oxide (NiOx) is a promising hole-transporting material for perovskite light-emitting diodes (PeLEDs) because of its low cost, excellent stability, and simple fabrication process. However, the electroluminescence efficiencies of NiOx-based PeLEDs are greatly limited by inefficient hole injection and exciton quenching at the NiOx-perovskite interfaces. Here, a novel interfacial engineering method with sodium dodecyl sulfate-oxygen plasma (SDS-OP) is demonstrated to simultaneously overcome the aforementioned issues. Experimental results reveal that a short OP treatment on the top of the SDS-coated NiOx significantly deepens the NiOx work function (from 4.23 to 4.85 eV) because of the formation of a large surface dipole, allowing for efficient hole injection. Moreover, the SDS-OP layer passivates the electronic surface trap states of perovskite films and suppresses the exciton quenching by NiOx. These improvements inhibit the nonradiative decays at the NiOx-perovskite interface. As a result, the external quantum efficiency of CsPbBr3 LEDs is increased from 0.052 to 2.5%; that of FAPbBr3 nanocrystals LEDs is increased from 5.6 to 7.6%.

Improving Efficiency and Stability in Quasi-2D Perovskite Light-Emitting Diodes by a Multifunctional LiF Interlayer.

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.