Highly bright light-emitting diodes based on solution-processed all-inorganic perovskite thin film are demonstrated. The cesium lead bromide (CsPbBr ) created using a new poly(ethylene oxide)-additive spin-coating method exhibits photoluminescence quantum yield up to 60% and excellent uniformity of electrical current distribution. Using the smooth CsPbBr films as emitting layers, green perovskite-based light-emitting diodes (PeLEDs) exhibit electroluminescent brightness and efficiency above 53 000 cd m and 4%: a new benchmark of device performance for all-inorganic PeLEDs.
The functionality and performance of a semiconductor is determined by its bandgap. Alloying, as for instance in InxGa1-xN, has been a mainstream strategy for tuning the bandgap. Keeping the semiconductor alloys in the miscibility gap (being homogeneous), however, is non-trivial. This challenge is now being extended to halide perovskites – an emerging class of photovoltaic materials. While the bandgap can be conveniently tuned by mixing different halogen ions, as in CsPb(BrxI1-x)3, the so-called mixed-halide perovskites suffer from severe phase separation under illumination. Here, we discover that such phase separation can be highly suppressed by embedding nanocrystals of mixed-halide perovskites in an endotaxial matrix. The tuned bandgap remains remarkably stable under extremely intensive illumination. The agreement between the experiments and a nucleation model suggests that the size of the nanocrystals and the host-guest interfaces are critical for the photo-stability. The stabilized bandgap will be essential for the development of perovskite-based optoelectronics, such as tandem solar cells and full-color LEDs.
Perovskite light-emitting diodes (LEDs) have recently attracted great research interest for their narrow emissions and solution processability. Remarkable progress has been achieved in green perovskite LEDs in recent years, but not blue or red ones. Here, highly efficient and spectrally stable red perovskite LEDs with quasi-2D perovskite/poly(ethylene oxide) (PEO) composite thin films as the light-emitting layer are reported. By controlling the molar ratios of organic salt (benzylammonium iodide) to inorganic salts (cesium iodide and lead iodide), luminescent quasi-2D perovskite thin films are obtained with tunable emission colors from red to deep red. The perovskite/polymer composite approach enables quasi-2D perovskite/PEO composite thin films to possess much higher photoluminescence quantum efficiencies and smoothness than their neat quasi-2D perovskite counterparts. Electrically driven LEDs with emissions peaked at 638, 664, 680, and 690 nm have been fabricated to exhibit high brightness and external quantum efficiencies (EQEs). For instance, the perovskite LED with an emission peaked at 680 nm exhibits a brightness of 1392 cd m and an EQE of 6.23%. Moreover, exceptional electroluminescence spectral stability under continuous device operation has been achieved for these red perovskite LEDs.
The halide perovskite CsPbBr has shown its promise for green light-emitting diodes. The optimal conditions of photoluminescence and the underlying photophysics, however, remain controversial. To address the inconsistency seen in the previous reports and to offer high-quality luminescent materials that can be readily integrated into functional devices with layered architecture, we created thin films of CsPbBr/CsPbBr composites based on a dual-source vapor-deposition method. With the capability of tuning the material composition in a broad range, CsPbBr is identified as the only light emitter in the composites. Interestingly, the presence of the photoluminescence-inactive CsPbBr can significantly enhance the light emitting efficiency of the composites. The unique negative thermal quenching observed near the liquid nitrogen temperature indicates that a type of shallow state generated at the CsPbBr/CsPbBr interfaces is responsible for the enhancement of photoluminescence.
With rapid advances of perovskite light-emitting diodes (PeLEDs), the large-scale fabrication of patterned PeLEDs towards display panels is of increasing importance. However, most state-of-the-art PeLEDs are fabricated by solution-processed techniques, which are difficult to simultaneously achieve high-resolution pixels and large-scale production. To this end, we construct efficient CsPbBr3 PeLEDs employing a vacuum deposition technique, which has been demonstrated as the most successful route for commercial organic LED displays. By carefully controlling the strength of the spatial confinement in CsPbBr3 film, its radiative recombination is greatly enhanced while the nonradiative recombination is suppressed. As a result, the external quantum efficiency (EQE) of thermally evaporated PeLED reaches 8.0%, a record for vacuum processed PeLEDs. Benefitting from the excellent uniformity and scalability of the thermal evaporation, we demonstrate PeLED with a functional area up to 40.2 cm2 and a peak EQE of 7.1%, representing one of the most efficient large-area PeLEDs. We further achieve high-resolution patterned perovskite film with 100 μm pixels using fine metal masks, laying the foundation for potential display applications. We believe the strategy of confinement strength regulation in thermally evaporated perovskites provides an effective way to process high-efficiency and large-area PeLEDs towards commercial display panels.
CsPbBr 3 is a promising type of light-emitting halide perovskite with inorganic composition and desirable thermal stability. The luminescence efficiency of pristine CsPbBr 3 thin films, however, appeared to be limited. In this work, we have demonstrated light emitting diodes based on CsPbBr 3 |Cs 4 PbBr 6 composites. Both quantum efficiency and emission brightness have been improved significantly compared with similar devices constructed using pure CsPbBr 3 . The high brightness can be attributed to the enhanced radiative recombination from CsPbBr 3 crystallites confined in the Cs 4 PbBr 6 host matrix. The unfavorable charge transport property of Cs 4 PbBr 6 can be circumvented by optimizing the ratio between the host and the guest components and the total thickness of the composite thin films. The inorganic composition of the emitting layer also leads to improved device stability under the condition of continuous operation.
Three-dimensional (3D) microfibrillar network represents an important structural design for various natural tissues and synthetic aerogels. Despite extensive efforts, achieving high mechanical properties for synthetic 3D microfibrillar networks remains challenging. Here, we report ultrastrong polymeric aerogels involving self-assembled 3D networks of aramid nanofiber composites. The interactions between the nanoscale constituents lead to assembled networks with high nodal connectivity and strong crosslinking between fibrils. As revealed by theoretical simulations of 3D networks, these features at fibrillar joints may lead to an enhancement of macroscopic mechanical properties by orders of magnitude even with a constant level of solid content. Indeed, the polymeric aerogels achieved both high specific tensile modulus of ~625.3 MPa cm3 g−1 and fracture energy of ~4700 J m−2, which are advantageous for diverse structural applications. Furthermore, their simple processing techniques allow fabrication into various functional devices, such as wearable electronics, thermal stealth, and filtration membranes. The mechanistic insights and manufacturability provided by these robust microfibrillar aerogels may create further opportunities for materials design and technological innovation.
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