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.
Thanks to its strong X-ray absorption and large carrier diffusion length, perovskites have demonstrated excellent performance for X-ray detection. Combination of perovskite with thin-film transistor (TFT) arrays to construct flat-panel X-ray imager (FPXI) is required for X-ray imaging, yet this is rarely reported. Solution processing of perovskite thick film onto TFT can enable the electronic connection, however the amounts of pinholes inevitably form during the solvent evaporation and result in a porous film with deteriorated performance and stability. Here a novel strategy is raised to achieve high-quality perovskite thick films for TFT integration via soft-pressing and in situ polymerization of multi-functional binder (TMTA). The combined process largely eliminates the pinholes, improves the surface smoothness, passivates grains boundaries, reduces ionic migration, and improves stability. Accordingly, a compact and smooth MAPbI 3 thick film integrating with TFT arrays is prepared for flat-panel X-ray imaging. The largest film (28 × 28 cm 2 ) is obtained with the state-of-theart performance (ratio of sensitivity to noise current: 1.41 × 10 11 µC Gy −1 A −1 ) among polycrystalline films. It is hoped that the work provides guidance for fabricating compact perovskite thick films and push perovskite FPXI one step further for low-dose X-ray imaging.
Controlling the carrier polarity and concentration underlies most electronic and optoelectronic devices. However, for the intensively studied lead halide perovskites, the doping tunability is inefficient. In this work, taking CsPbBr3 as an example, it is revealed that the coexistence of metallic Pb or CsBr3/Br2, rather than the precursor ratio, can provide Pb‐rich/Br‐poor or Br‐rich/Pb‐poor chemical conditions, enabling the tunability of electrical properties from weak n‐type, intrinsic, to moderate p‐type. Experimentally, under Br2‐exposure treatment, a shift of the Fermi level as large as 1.00 eV is achieved, which is one of the highest value among all kinds of doping methods. The X‐ray detector based on the intrinsic CsPbBr3 exhibits excellent performance, with a negligible dark‐current drift of 7.1 × 10−4 nA cm−1 s−1 V−1, a low detection limit of 103.6 nGyair s−1, and a high sensitivity of 9085 μC Gyair−1 cm−2. This work provides a critical understanding and guidance for tuning the electrical properties of lead halide perovskites, which establishes good foundations for achieving intrinsic perovskite semiconductors and also constructing potential homojunction devices.
Multi-energy X-ray detection is sought after for a wide range of applications including medical imaging, security checking and industrial flaw inspection. Perovskite X-ray detectors are superior in terms of high sensitivity and low detection limit, which lays a foundation for multi-energy discrimination. However, the extended capability of the perovskite detector for multi-energy X-ray detection is challenging and has never been reported. Herein we report the design of vertical matrix perovskite X-ray detectors for multi-energy detection, based on the attenuation behavior of X-ray within the detector and machine learning algorithm. This platform is independent of the complex X-ray source components that constrain the energy discrimination capability. We show that the incident X-ray spectra could be accurately reconstructed from the conversion matrix and measured photocurrent response. Moreover, the detector could produce a set of images containing the density-graded information under single exposure, and locate the concealed position for all low-, medium- and high-density substances. Our findings suggest a new generation of X-ray detectors with features of multi-energy discrimination, density differentiation, and contrast-enhanced imaging.
Metal halide perovskites have recently been reported as excellent scintillators for X-ray detection. However, perovskite based scintillators are susceptible to moisture and oxygen atmosphere, such as the water solubility of CsPbBr3, and oxidation vulnerability of Sn2+, Cu+. The traditional metal halide scintillators (NaI: Tl, LaBr3, etc.) are also severely restricted by their high hygroscopicity. Here we report a new kind of lead free perovskite with excellent water and radiation stability, Rb2Sn1-x
Te
x
Cl6. The equivalent doping of Te could break the in-phase bonding interaction between neighboring octahedra in Rb2SnCl6, and thus decrease the electron and hole dimensionality. The optimized Te content of 5% resulted in high photoluminescence quantum yield of 92.4%, and low X-ray detection limit of 0.7 µGyair s−1. The photoluminescence and radioluminescence could be maintained without any loss when immersing in water or after 480,000 Gy radiations, outperforming previous perovskite and traditional metal halides scintillators.
Metal halide perovskites (MHPs) have demonstrated excellent performances in detection of X-rays and gamma-rays. Most studies focus on improving the sensitivity of single-pixel MHP detectors. However, little work pays attention to the dark current, which is crucial for the back-end circuit integration. Herein, the requirement of dark current is quantitatively evaluated as low as 10−9 A/cm2 for X-ray imagers integrated on pixel circuits. Moreover, through the semiconductor device analysis and simulation, we reveal that the main current compositions of thick perovskite X-ray detectors are the thermionic-emission current (JT) and the generation-recombination current (Jg-r). The typical observed failures of p–n junctions in thick detectors are caused by the high generation-recombination current due to the band mismatch and interface defects. This work provides a deep insight into the design of high sensitivity and low dark current perovskite X-ray detectors.
Graphical Abstract
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