Oriented-Structured CsCu2I3 Film by Close-Space Sublimation and Nanoscale Seed Screening for High-Resolution X-ray Imaging.

An all-inorganic lead-free halides Cs-Cu-I system, represented by Cs3Cu2I5 and CsCu2I3, has attracted attention for their good photophysical characteristics recently. Successive works had reported their application potential in light-emitting devices. However, there is no report for CsCu2I3 in X-ray scintillation detectors so far. We notice that CsCu2I3 may be advantageous in such an application due to the one-dimensional crystal structure, the congruent-melting feature, and the high spectral matching to some photosensors. In this work, we explore the scintillation properties and imaging application of CsCu2I3 in X-ray scintillator detector. The oriented structure is designed to enhance the imaging performance of a CsCu2I3 detector. Close-space sublimation process and nanoscale seed screening strategy are employed to realize this design by producing a large-area (25 cm2) CsCu2I3 thick film layer with the oriented nanorod structure. This CsCu2I3 detector eventually achieves a high spatial resolution of 7.5 lp mm-1 in X-ray imaging.

Efficient and Reabsorption-Free Radioluminescence in Cs3Cu2I5 Nanocrystals with Self-Trapped Excitons.

Radioluminescent materials (scintillators) are widely applied in medical imaging, nondestructive testing, security inspection, nuclear and radiation industries, and scientific research. Recently, all-inorganic lead halide perovskite nanocrystal (NC) scintillators have attracted great attention due to their facile solution processability and ultrasensitive X-ray detection, which allows for large area and flexible X-ray imaging. However, the light yield of these perovskite NCs is relatively low because of the strong self-absorption that reduces the light out-coupling efficiency. Here, NCs with self-trapped excitons emission are demonstrated to be sensitive, reabsorption-free scintillators. Highly luminescent and stable Cs3Cu2I5 NCs with a photoluminescence quantum yields of 73.7%, which is a new record for blue emission lead-free perovskite or perovskite-like NCs, is produced with the assistance of InI3. The PL peak of the Cs3Cu2I5 NCs locates at 445 nm that matches with the response peak of a silicon photomultiplier. Thus, Cs3Cu2I5 NCs are demonstrated as efficient scintillators with zero self-absorption and extremely high light yield (≈79 279 photons per MeV). Both Cs3Cu2I5 NC colloidal solution and film exhibit strong radioluminescence under X-ray irradiation. The potential application of Cs3Cu2I5 NCs as reabsorption-free, low cost, large area, and flexible scintillators is demonstrated by a prototype X-ray imaging with a high spatial resolution.

All-Inorganic Copper Halide as a Stable and Self-Absorption-Free X-ray Scintillator.

Lead halide perovskites have recently shown great potential as X-ray scintillators; however, the toxicity of the lead element seriously restricts their applications. Herein we report a new lead-free and self-absorption-free scintillator based on Rb2CuCl3 metal halide. The Rb2CuCl3 exhibits a near-unity photoluminescence quantum yield (99.4%) as well as a long photoluminescence lifetime (11.3 µs). Furthermore, Rb2CuCl3 demonstrates an appreciable light yield of 16 600 photons per megaelectronvolt and a large scintillation response with a linear range from 48.6 nGyair s-1 to 15.7 µGyair s-1. Notably, the detection limit is as low as 88.5 nGyair s-1, enabling a reduced radiation dose to the human body when a medical and security check is conducted. In addition, Rb2CuCl3 exhibits good stability against the atmosphere, continuous ultraviolet light, as well as X-ray irradiation. The combination of the decent scintillation performance, low toxicity and good stability suggests the Rb2CuCl3 could be a possible promising X-ray scintillator.

Hot-Pressed CsPbBr3 Quasi-Monocrystalline Film for Sensitive Direct X-ray Detection.

An X-ray detector with high sensitivity would be able to increase the generated signal and reduce the dose rate; thus, this type of detector is beneficial for applications such as medical imaging and product inspection. The inorganic lead halide perovskite CsPbBr3 possesses relatively larger density and a higher atomic number in contrast to its hybrid counterpart. Therefore, it is expected to provide high detection sensitivity for X-rays; however, it has rarely been studied as a direct X-ray detector. Here, a hot-pressing method is employed to fabricate thick quasi-monocrystalline CsPbBr3 films, and a record sensitivity of 55 684 µC Gyair -1 cm-2 is achieved, surpassing all other X-ray detectors (direct and indirect). The hot-pressing method is simple and produces thick quasi-monocrystalline CsPbBr3 films with uniform orientations. The high crystalline quality of the CsPbBr3 films and the formation of self-formed shallow bromide vacancy defects during the high-temperature process result in a large µτ product and, therefore, a high photoconductivity gain factor and high detection sensitivity. The detectors also exhibit relatively fast response speed, negligible baseline drift, and good stability, making a CsPbBr3 X-ray detector extremely competitive for high-contrast X-ray detections.

Lead-Free Halide Rb2 CuBr3 as Sensitive X-Ray Scintillator.

Scintillators are widely utilized for radiation detections in many fields, such as nondestructive inspection, medical imaging, and space exploration. Lead halide perovskite scintillators have recently received extensive research attention owing to their tunable emission wavelength, low detection limit, and ease of fabrication. However, the low light yields toward X-ray irradiation and the lead toxicity of these perovskites severely restricts their practical application. A novel lead-free halide is presented, namely Rb2 CuBr3 , as a scintillator with exceptionally high light yield. Rb2 CuBr3 exhibits a 1D crystal structure and enjoys strong carrier confinement and near-unity photoluminescence quantum yield (98.6%) in violet emission. The high photoluminescence quantum yield combined with negligible self-absorption from self-trapped exciton emission and strong X-ray absorption capability enables a record high light yield of ≈91056 photons per MeV among perovskite and relative scintillators. Overall, Rb2 CuBr3 provides nontoxicity, high radioluminescence intensity, and good stability, thus laying good foundations for potential application in low-dose radiography.

Heteroepitaxial passivation of Cs2AgBiBr6 wafers with suppressed ionic migration for X-ray imaging.

X-ray detectors are broadly utilized in medical imaging and product inspection. Halide perovskites recently demonstrate excellent performance for direct X-ray detection. However, ionic migration causes large noise and baseline drift, limiting the detection and imaging performance. Here we largely eliminate the ionic migration in cesium silver bismuth bromide (Cs2AgBiBr6) polycrystalline wafers by introducing bismuth oxybromide (BiOBr) as heteroepitaxial passivation layers. Good lattice match between BiOBr and Cs2AgBiBr6 enables complete defect passivation and suppressed ionic migration. The detector hence achieves outstanding balanced performance with a signal drifting one order of magnitude lower than all previous studies, low noise (1/f noise free), a high sensitivity of 250 µC Gy air-1 cm-2, and a spatial resolution of 4.9 lp mm-1. The wafer area could be easily scaled up by the isostatic-pressing method, together with the heteroepitaxial passivation, strengthens the competitiveness of Cs2AgBiBr6-based X-ray detectors as next-generation X-ray imaging flat panels.

High Pressure Structural and Optical Properties of Two-Dimensional Hybrid Halide Perovskite (CH3NH3)3Bi2Br9.

Two-dimensional (2D) hybrid halide perovskite is emerging as the next generation of photoelectronic materials. Herein, a typical 2D halide perovskite of MA3Bi2Br9 (MA = CH3NH3) is chosen for high pressure research to explore the distinct structural and property characteristics of the inorganic and organic compositions therein. Upon compression above 4.3 GPa, the distortion and tilting of inorganic BiBr6 octahedra dominate the phase transition of MA3Bi2Br9 from trigonal to monoclinic. Meanwhile, exceptionally anisotropic compressibilities are observed between intra- and interlayer structures, which originate from the unique geometry of puckered layer. In addition, the presence of organic MA+ cations contributes to the flexible structural nature of MA3Bi2Br9. Meanwhile, the geometrical changes of inorganic components determine the relationships between structure and band gap under pressure. This work not only demonstrates the intriguing structure nature of MA3Bi2Br9 but also reveals the individual contributions on the structure-property diagram from inorganic (BiBr6 octahedra) and organic (MA cations) components.