Perovskite light-emitting diodes with external quantum efficiency exceeding 20 per cent.

Metal halide perovskite materials are an emerging class of solution-processable semiconductors with considerable potential for use in optoelectronic devices1-3. For example, light-emitting diodes (LEDs) based on these materials could see application in flat-panel displays and solid-state lighting, owing to their potential to be made at low cost via facile solution processing, and could provide tunable colours and narrow emission line widths at high photoluminescence quantum yields4-8. However, the highest reported external quantum efficiencies of green- and red-light-emitting perovskite LEDs are around 14 per cent7,9 and 12 per cent8, respectively-still well behind the performance of organic LEDs10-12 and inorganic quantum dot LEDs13. Here we describe visible-light-emitting perovskite LEDs that surpass the quantum efficiency milestone of 20 per cent. This achievement stems from a new strategy for managing the compositional distribution in the device-an approach that simultaneously provides high luminescence and balanced charge injection. Specifically, we mixed a presynthesized CsPbBr3 perovskite with a MABr additive (where MA is CH3NH3), the differing solubilities of which yield sequential crystallization into a CsPbBr3/MABr quasi-core/shell structure. The MABr shell passivates the nonradiative defects that would otherwise be present in CsPbBr3 crystals, boosting the photoluminescence quantum efficiency, while the MABr capping layer enables balanced charge injection. The resulting 20.3 per cent external quantum efficiency represents a substantial step towards the practical application of perovskite LEDs in lighting and display.

Efficient and Stable Low-Bandgap Perovskite Solar Cells Enabled by a CsPbBr3-Cluster Assisted Bottom-up Crystallization Approach.

Recently, low-bandgap formamidinium lead iodide FAPbI3-based perovskites are of particular interest for high-performance perovskite solar cells (PSCs) due to their broad spectral response and high photocurrent output. However, to inhibit the spontaneous α-to-δ phase transition, 15-17% (molar ratio) of bromide and cesium or methylammonium incorporated into the FAPbI3 are indispensable to achieve efficient PSCs. In return, the high bromide content will increase bandgap and narrow the spectral response region. If simply reducing the bromide content, the corresponding PSCs exhibit inferior operational stability due to α-to-δ phase transition, interface degradation, and halide migration. Herein, we report a CsPbBr3-cluster assisted vertically bottom-up crystallization approach to fabricate low-bromide (1% ∼ 6%), α-phase pure, and MA-free FAPbI3-based PSCs. The clusters, in the size of several nanometers, could act as nuclei to facilitate vertical growth of high quality α-FAPbI3 perovskite crystals. Moreover, these clusters can show further intake by perovskite after thermal annealing, which improves the phase homogeneity of the as-prepared perovskite films. As a result, the corresponding mesoporous PSCs deliver a champion efficiency of 21.78% with photoresponse extended to 830 nm. Moreover, these devices show remarkably improved operational stability, retaining ∼82% of the initial efficiency after 1,000 h of maximum power point tracking under 1 sun condition.

Dendritic CsSnI3 for Efficient and Flexible Near-Infrared Perovskite Light-Emitting Diodes.

All-inorganic and lead-free CsSnI3 is emerging as one of the most promising candidates for near-infrared perovskite light-emitting diodes (NIR Pero-LEDs), which find practical applications including facial recognition, biomedical apparatus, night vision camera, and Light Fidelity. However, in the CsSnI3 -based Pero-LEDs, the holes injection is significantly higher than that of electrons, resulting in unbalanced charge injection, undesired exciton dissipation, and poor device performance. Herein, it is proposed to manage charge injection and recombination behavior by tuning the interface area of perovskite and charge-transporter. A dendritic CsSnI3 structure is prepared on the hole-transporter, only making a bottom contact with the hole-transporter and exposing all other available crystal surfaces to the electron-transporter. In other words, the interface area of perovskite/electron-transporter is significantly higher than that of perovskite/hole-transporter. Moreover, the embedding interface of perovskite/electron-transporter can spatially confine holes and electrons, increasing the radiation recombination. By taking advantage of the dendritic structure, efficient lead-free NIR Pero-LEDs are achieved with a record external quantum efficiency (EQE) of 5.4%. More importantly, the dendritic structure shows great superiorities in flexible devices, for there is almost no morphology change after 2000-cycles of bends, and the fabricated Pero-LEDs can keep 93.4% of initial EQEs after 50-cycles of bends.

Composition engineering to obtain efficient hybrid perovskite light-emitting diodes.

Metal halide perovskites have received considerable attention in the field of electroluminescence, and the external quantum efficiency of perovskite light-emitting diodes has exceeded 20%. CH3NH3PbBr3 has been intensely investigated as an emitting layer in perovskite light-emitting diodes. However, perovskite films comprising CH3NH3PbBr3 often exhibit low surface coverage and poor crystallinity, leading to high current leakage, severe nonradiative recombination, and limited device performance. Herein, we demonstrate a rationale for composition engineering to obtain high-quality perovskite films. We first reduce pinholes by adding excess CH3NH3Br to the actual CH3NH3PbBr3 films, and we then add CsBr to improve the crystalline quality and to passivate nonradiative defects. As a result, the (CH3NH3)1-xCsxPbBr3 based perovskite light-emitting diodes exhibit significantly improved external quantum and power efficiencies of 6.97% and 25.18 lm/W, respectively, representing an improvement in performance dozens of times greater than that of pristine CH3NH3PbBr3-based perovskite light-emitting diodes. Our study demonstrates that composition engineering is an effective strategy for enhancing the device performance of perovskite light-emitting diodes.

Ultrathin PEDOT:PSS Enables Colorful and Efficient Perovskite Light-Emitting Diodes.

Recently, metal halide perovskite light-emitting diodes (Pero-LEDs) have achieved significant improvement in device performance, especially for external quantum efficiency (EQE). And EQE is mostly determined by internal quantum efficiency of the emitting material, charge injection balancing factor (ηc), and light extraction efficiency (LEE) of the device. Herein, an ultrathin poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (UT-PEDOT:PSS) hole transporter layer is prepared by a water stripping method, and the UT-PEDOT:PSS can enhance ηc and LEE simultaneously in Pero-LEDs, mostly due to the improved carrier mobility, more matched energy level alignment, and reduced photon loss. More importantly, the performance enhancement from UT-PEDOT:PSS is quite universal and applicable in different kinds of Pero-LEDs. As a result, the EQEs of Pero-LEDs based on 3D, quasi-3D, and quasi-2D perovskites obtain enhancements of 42%, 87%, and 111%, and the corresponding maximum EQE reaches 17.6%, 15.0%, and 6.8%, respectively.