High-resolution X-ray Imaging Research Articles

Stable Luminescent Organic Manganese Halide Used for High-Resolution X-ray Imaging

Stable Luminescent Organic Manganese Halide Used for High-Resolution X-ray Imaging

Mitigation of Parasitic and Drift Capacitance-Induced Nonlinear Current Responses for Stable and Sensitive Perovskite X-ray Detectors.

The development of perovskite direct X-ray detectors shows potential for advancing medical imaging and industrial inspection precision. To ensure the optimal energy conversion efficiency of X-rays for reducing radiation doses, it is necessary for perovskites with thicknesses reaching hundreds of micrometers or even several millimeters to be utilized. However, the nonlinear current response becomes uncertain with such high thicknesses. For instance, the prevailing theory regarding the rapid trapping and release of charges by shallow-level defects falls short in explaining the nonlinear current response observed in high-quality single-crystal samples. Moreover, a significant nonlinear current response can degrade the detection performance. Here, we elucidate peculiar parasitic and drift capacitance-induced nonlinear current responses in perovskites, which arise from bulk structural deficiencies and interface junction width variation in addition to shallow-level defects. Both theoretical analysis and experimental findings demonstrate the effective suppression of nonlinear current responses by establishing bulk heterojunctions and refining interface junctions. Consequently, we have successfully developed highly linear current-responsive detectors based on polycrystalline MAPbI3 thick films. Notably, these detectors achieve a record sensitivity of 2.3 × 104 μC·Gyair-1·cm-2 under 100 kVp X-ray irradiation with a low bias of 0.1 V/μm, enabling enduring and high-resolution X-ray imaging for high-density objects. Successful fabrication and testing of a 64 × 64-pixel flat-panel prototype detector affirm the widespread applicability of these strategies in rectifying nonlinear current responses in perovskite-based X-ray detectors.

Thermal stability and flexible X-Ray scintillation screen through in-situ assembling Cs3Cu2Cl5 nanocrystals in polymer matrix

Copper-based halides have emerged as promising scintillator materials for X-ray imaging, attributed to their favorable photophysical characteristics, such as negligible self-absorption, high light output, and fast decay. Within this category of materials, Cs3Cu2Cl5 composite polymer scintillator films stand out, delivering excellent performance as flexible X-ray detector screens. However, severe scattering and light degradation induced by the inevitable agglomeration during recombination restricted the application in high-resolution and flexible X-ray imaging. In this study, a Cs3Cu2Cl5@PMMA film prepared by in-situ growth strategy is successfully developed, which represents uniform area, adjustable flexibility and excellent scintillation performance. The prepared large-area film exhibits green emission at 527 nm, with a high light yield, low detection limit and excellent spatial resolution. Meanwhile, the Cs3Cu2Cl5@PMMA film exhibits a remarkable degree of flexibility, enabling imaging applications on non-planar surfaces. Furthermore, it also demonstrates excellent resistance to high temperature environment, maintaining its high-quality imaging performance at 403 K.

Large-Area Transparent Antimony-Based Perovskite Glass for High-Resolution X-ray Imaging.

Nonlead low-dimensional halide perovskites attract considerable attention as X-ray scintillators. However, most scintillation screens exhibit pronounced light scattering, which detrimentally reduces the quality of X-ray imaging. Herein, we employed a simple and straightforward solvent-free melt-quenching method to fabricate a large-area zero-dimension (0D) antimony-based perovskite transparent medium, namely (C20H20P)2SbCl5 (C20H20P+ = ethyltriphenylphosphine). The transparency is due to the large steric hindrance of C20H20P+, which hinders the formation of crystals during the quenching process, thus forming a glass with low refractive index and uniform structure. This medium exhibits a high transmittance exceeding 80% in the range of 450-800 nm and shows a large Stokes shift of 245 nm, thereby minimizing light scattering, mitigating self-absorption, and enhancing the clarity of X-ray imaging. Moreover, it exhibits a high radioluminescence light yield of ∼12,535 photons MeV-1 and displays a high X-ray spatial resolution of 30 lp mm-1 owing to its high transparency. This study presents an alternative candidate for achieving high-quality X-ray detection and extends the applicability of transparent perovskite scintillators.

Synthetic X-ray Image Generation for Non-Destructive Testing using Generative Adversarial Networks

Developing and optimizing a Machine Learning (ML) based Non-Destructive Testing (NDT) tool for automotive manufacturing can be challenging due to the need for a significant amount of annotated training data. Obtaining such an extent of real X-ray images of different defects can be challenging and expensive. Hence, generating synthetic images with adequate defects is a viable option to fill this gap. This contribution presents a novel approach that harnesses Generative Adversarial Networks (GANs) to simulate industrial X-ray images of specific parts of a car wheel (rim and spokes) with defects and their annotations. The presented method draws inspiration from techniques used in medical healthcare radiography as well as the NDT field for simulating synthetic X-ray images. We propose a novel deep neural network architecture for generating high-resolution X-ray images of size 1024 x 512 pixels with porous defects in specified locations. These images are automatically generated from edge masks of the desired structure. We conducted separate evaluations for both, the generated images and the included defects. To assess the generated image quality, we used image properties and structural similarity metrics. The generated images achieved an MSSIM index of over 0.90. We analyzed the local gray-scale profile of synthetic images to evaluate the quality of generated defects. A state-of-the-art defect detector (ISAR, developed by Fraunhofer EZRT) was used to estimate defect detection based on various IoU thresholds. In conclusion, the presented research demonstrates the feasibility of leveraging GANs to generate synthetic 2D X- ray image data, including defects for training ML-based NDT tools. This approach opens new possibilities for developing and optimizing robust NDT solutions by overcoming the challenges of obtaining real data with defects.

Mn(II)-Based Metal Halide with Near-Unity Quantum Yield for White LEDs and High-Resolution X-ray Imaging.

Metal halides have drawn great interest as luminescent materials and scintillators due to their outstanding optical properties. Exploring new types of phosphors with easy production processes, excellent photophysical properties, high light yields, and environmentally friendly compositions is crucial and quite challenging. Herein, a novel Mn(II)-based metal halide (4-BTP)2MnBr4 was produced using a facile solvent evaporation method, which exhibited a strong green emission peaking at 524 nm from the d-d transition of tetrahedral-coordinated Mn2+ ion and a near-unity quantum yield. The prepared white light-emitting diode device has a wide color gamut of 100.7% NTSC with CIE chromaticity coordinates of (0.32, 0.32). In addition, (4-BTP)2MnBr4 demonstrates excellent characteristics in X-ray scintillation, including a high light yield of 98 000 photons/MeV, a sensitive detection limit of 37.4 nGy/s, excellent resistance to radiation damage, and successful demonstration of X-ray imaging with high resolution at 21.3 lp/mm, revealing the potential for application in diagnostic X-ray medical imaging and industry radiation detection.

High-Resolution X-ray Image from Copper-Based Perovskite Hybrid Polymer.

Cs3Cu2I5 nanocrystals (NCs) are considered to be promising materials due to their high photoluminescence efficiency, lack of lead toxicity, and X-ray responsiveness. However, during the crystallization process, NCs are prone to agglomeration and exhibit uneven size distribution, resulting in several light scattering that severely affect their imaging resolution. Herein, we successfully developed a high-resolution scintillator film by growing copper-based perovskite NCs within a hybrid polymer matrix. By leveraging the ingenious integration of polyvinylidene fluoride (PVDF) and polymethyl methacrylate (PMMA), the size and distribution uniformity of Cs3Cu2I5 NCs can be effectively controlled. Consequently, a high spatial resolution of 14.3 lp mm-1 and a low detection limit of 105 nGy s-1 are achieved, and the scintillator film has excellent flexibility and stability. These results highlight the promising application of Cs3Cu2I5 scintillator films in low-cost, flexible, and high-performance medical imaging.

High-Throughput Growth of Armored Perovskite Single Crystal Fibers for Pixelated Arrays.

The poor machinability of halide perovskite crystals severely hampered their practical applications. Here a high-throughput growth method is reported for armored perovskite single-crystal fibers (SCFs). The mold-embedded melt growth (MEG) method provides each SCF with a capillary quartz shell, thus guaranteeing their integrality when cutting and polishing. Hundreds of perovskite SCFs, exemplified by CsPbBr3, CsPbCl3, and CsPbBr2.5I0.5, with customized dimensions (inner diameters of 150-1000µm and length of several centimeters), are grown in one batch, with all the SCFs bearing homogeneity in shape, orientation, and optical/electronic properties. Versatile assembly protocols are proposed to directly integrate the SCFs into arrays. The assembled array detectors demonstrated low-level dark currents (< 1nA) with negligible drift, low detection limit (< 44.84nGys-1), and high sensitivity (61147µCGy-1cm-2). Moreover, the SCFs as isolated pixels are free of signal crosstalk while showing uniform X-ray photocurrents, which is in favor of high spatial resolution X-ray imaging. As both MEG and the assembly of SCFs involve none sophisticated processes limiting the scalable fabrication, the strategy is considered to meet the preconditions of high-throughput productions.

Uncovering the First AGN Jets with AXIS

Jets powered by AGN in the early Universe (z≳6) have the potential to not only define the evolutionary trajectories of the first-forming massive galaxies but to enable the accelerated growth of their associated SMBHs. Under typical assumptions, jets could even rectify observed quasars with light seed formation scenarios; however, not only are constraints on the parameters of the first jets lacking, observations of these objects are scarce. Owing to the significant energy density of the CMB at these epochs capable of quenching radio emission, observations will require powerful, high angular resolution X-ray imaging to map and characterize these jets. As such, AXIS will be necessary to understand early SMBH growth and feedback. This White Paper is part of a series commissioned for the AXIS Probe Concept Mission; additional AXIS White Papers can be found at the AXIS website.

Probing Energy-Funneling Kinetics in Nanocrystal Sublattices for Superior X-Ray Imaging.

Long-lasting radioluminescence scintillators have recently attracted substantial attention from both research and industrial communities, primarily due to their distinctive capabilities of converting and storing X-ray energy. However, determination of energy-conversion kinetics in these nanocrystals remains unexplored. Here we present a strategy to probe and unveil energy-funneling kinetics in NaLuF4:Mn2+/Gd3+ nanocrystal sublattices through Gd3+-driven microenvironment engineering and Mn2+-mediated radioluminescence profiling. Our photophysical studies reveal effective control of energy-funneling kinetics and demonstrate the tunability of electron trap depth ranging from 0.66 to 0.96 eV, with the corresponding trap density varying between 2.38×105 and 1.34×107 cm-3. This enables controlled release of captured electrons over durations spanning from seconds to 30 days. It allows tailorable emission wavelength within the range of 520-580 nm and fine-tuning of thermally-stimulated temperature between 313-403 K. We further utilize these scintillators to fabricate high-density, large-area scintillation screens that exhibit a 6-fold improvement in X-ray sensitivity, 22 lp/mm high-resolution X-ray imaging, and a 30-day-long optical memory. This enables high-contrast imaging of injured mice through fast thermally-stimulated radioluminescence readout. These findings offer new insights into the correlation of radioluminescence dynamics with energy-funneling kinetics, thereby contributing to the advancement of high-energy nanophotonic applications.

In-situ growth of Cs5Cu3Cl6I2 nanocrystals within AAO arrays for X-ray imaging

Lead-free halide perovskites have shown promising application for indirect X-ray detection as fascinating scintillator. The fabrication of pixelated scintillator films leveraging directional confinement allows high-resolution imaging, yet process complexity and the potential crystal structure damage pose challenges that compromises the corresponding scintillator performance. In this work, a facile in-situ strategy for growing scintillation perovskite of Cs5Cu3Cl6I2 within anodic aluminum oxide (AAO) membrane is developed as scintillator Cs5Cu3Cl6I2@AAO film. The as-fabricated pixelated scintillator array with an enhanced light directional confinement for high-resolution X-ray imaging is demonstrated. The corresponding film achieves a spatial resolution of approximately 20 lp mm−1 and a detection limit of 0.152 Gy·s−1. Moreover, the Cs5Cu3Cl6I2@AAO film performs excellent stability under long-term X-ray irradiation, making it a reliable option for cost-effective pixelated indirect X-ray imaging.

Monolithic integration of perovskite heterojunction on TFT backplanes through vapor deposition for sensitive and stable x-ray imaging.

Metal halide perovskites exhibit substantial potential for advancing next-generation x-ray detection. However, fabricating high-performance pixelated imaging arrays remains challenging due to the substantial dark current density and stability issues associated with common organic-inorganic hybrid perovskites. Here, we develop a vapor deposition method to create the first all-inorganic perovskite heterojunction film. The heterojunction introduction effectively reduces the dark current density of detectors to about 0.8 nA·cm-2, satisfying thin-film transistor (TFT) integration standards, while also increases sensitivity to above 2.6 × 104 μC·Gyair-1·cm-2, thus giving rise to a record low detection limit of <1 nGyair·s-1 among all polycrystalline perovskite-based x-ray detectors. The devices also demonstrate remarkable stability across multifarious demanding working conditions. Last, through monolithic integration of the heterojunction film with a 64 × 64 pixelated TFT array, we have achieved high-resolution real-time x-ray imaging, which paves the way for the application of all-inorganic perovskite in low-dose flat-panel x-ray detection.

Anomalous X-ray pulse responses in MAPbBr3 single crystal-based detectors

Organic-inorganic perovskite single crystals (SCs) are considered promising semiconductors for high-sensitivity X-ray detectors because of their strong X-ray interaction, low-temperature processability, and excellent properties such as long diffusion length, low defect density, and long carrier lifetime. However, the specific pulse response of MAPbBr3 SC-based X-ray detectors frequently exhibits a tail and over/undershoots at several conditions, which degrades the X-ray image quality; however, no detailed analysis of these characteristics has been reported thus far. For high-resolution X-ray imaging, it is necessary to obtain an ideal pulse response that is free of tails and over/undershoots. In this study, we investigated the specific X-ray responses of solution-grown MAPbBr3 SC-based X-ray detectors under various externally applied voltages. Based on the study on charge carrier dynamics, we analyzed the origin of the tail and over/undershoots in X-ray pulse response shapes. We theoretically verified that the unideal pulse response in perovskite SC-based X-ray detectors is attributed to the defect states inherent in perovskite SCs.

Growth of ultimate high-density scintillating films for high-resolution X-ray imaging at synchrotrons

Scintillators are X-ray to visible light converters applied in X-ray imaging detectors used at synchrotrons. Drastically improved performances of the 4th generation synchrotron sources enable us to perform X-ray imaging experiments at higher energies. For high spatial resolution X-ray imaging (micrometer to submicrometer), thin scintillating films are required. Consequently, especially for high X-ray energies (30keV to 100keV), the detection efficiency is limited due to the low X-ray absorption efficiency of the thin films. We have used Liquid Phase Epitaxy (LPE) to grow thin films of one of the ultimate high-density materials, Lu2Hf2O7:Eu3+, which demonstrate scintillating properties and thus combine high spatial resolution and maximized absorption efficiency. X-ray imaging experiments demonstrate that the Modulation Transfer Function (MTF) reaches 10% at 900 lp/mm, and radiographs visually confirm the promising imaging properties. We present structural, luminescent, and scintillation characterization of Lu2Hf2O7:Eu thin films grown on ZrO2:Y substrates, showing that the films crystallize in the disordered fluorite structure and the europium ions incorporate into the structure and enhance the luminescence intensity. This contribution is a first step toward developing promising ultra-dense, hafnate-based scintillating screens for high spatial resolution X-ray imaging.

High-resolution X-Ray imaging of small animal samples based on Commercial-Off-The-Shelf CMOS image sensors.

An automated system for acquiring microscopic-resolution radiographic images of biological samples was developed. Mass-produced, low-cost, and easily automated components were used, such as Commercial-Off-The-Self CMOS image sensors (CIS), stepper motors, and control boards based on Arduino and RaspberryPi. System configuration, imaging protocols, and Image processing (filtering and stitching) were defined to obtain high-resolution images and for successful computational image reconstruction. Radiographic images were obtained for animal samples including the widely used animal models zebrafish (Danio rerio) and the fruit-fly (Drosophila melanogaster), as well as other small animal samples. The use of phosphotungstic acid (PTA) as a contrast agent was also studied. Radiographic images with resolutions of up to (7±0.6)μm were obtained, making this system comparable to commercial ones. This work constitutes a starting point for the development of more complex systems such as X-ray attenuation micro-tomography systems based on low-cost off-the-shelf technology. It will also bring the possibility to expand the studies that can be carried out with small animal models at many institutions (mostly those working on tight budgets), particularly those on the effects of ionizing radiation and absorption of heavy metal contaminants in animal tissues.

A detachable interface for stable low-voltage stretchable transistor arrays and high-resolution X-ray imaging

Challenges associated with stretchable optoelectronic devices, such as pixel size, power consumption and stability, severely brock their realization in high-resolution digital imaging. Herein, we develop a universal detachable interface technique that allows uniform, damage-free and reproducible integration of micropatterned stretchable electrodes for pixel-dense intrinsically stretchable organic transistor arrays. Benefiting from the ideal heterocontact and short channel length (2 μm) in our transistors, switching current ratio exceeding 106, device density of 41,000 transistors/cm2, operational voltage down to 5 V and excellent stability are simultaneously achieved. The resultant stretchable transistor-based image sensors exhibit ultrasensitive X-ray detection and high-resolution imaging capability. A megapixel image is demonstrated, which is unprecedented for stretchable direct-conversion X-ray detectors. These results forge a bright future for the stretchable photonic integration toward next-generation visualization equipment.

Correlative light and X-ray tomography jointly unveil the critical role of connexin43 channels on inflammation-induced cellular ultrastructural alterations

Non-junctional connexin43 (Cx43) plasma membrane hemichannels have been implicated in several inflammatory diseases, particularly playing a role in ATP release that triggers activation of the inflammasome. Therapies targeting the blocking of the hemichannels to prevent the pathological release or uptake of ions and signalling molecules through its pores are of therapeutic interest. To date, there is no close-to-native, high-definition documentation of the impact of Cx43 hemichannel-mediated inflammation on cellular ultrastructure, neither is there a robust account of the ultrastructural changes that occur following treatment with selective Cx43 hemichannel blockers such as Xentry-Gap19 (XG19).A combination of same-sample correlative high-resolution three-dimensional fluorescence microscopy and soft X-ray tomography at cryogenic temperatures, enabled in the identification of novel 3D molecular interactions within the cellular milieu when comparing behaviour in healthy states and during the early onset or late stages under inflammatory conditions. Notably, our findings suggest that XG19 blockage of connexin hemichannels under pro-inflammatory conditions may be crucial in preventing the direct degradation of connexosomes by lysosomes, without affecting connexin protein translation and trafficking. We also delineated fine and gross cellular phenotypes, characteristic of inflammatory insult or road-to-recovery from inflammation, where XG19 could indirectly prevent and reverse inflammatory cytokine-induced mitochondrial swelling and cellular hypertrophy through its action on Cx43 hemichannels. Our findings suggest that XG19 might have prophylactic and therapeutic effects on the inflammatory response, in line with functional studies.

Bifocal photon sieve imaging in the hard x-ray region.

Hard x-rays are widely used for plasma diagnosis, nondestructive inspection, and high-resolution x-ray imaging. A typical x-ray source is a tabletop micro-focus x-ray source. Here, a bifocal photon sieve (PS) with the smallest diameter of 59.6 nm was designed and fabricated by electron-beam lithography to focus hard x-rays on variable-resolution array images. An imaging experiment at 8.39 keV demonstrates that the designed and fabricated PS has two different focal lengths. The numerous pinholes that can be optimized provide richer degrees of freedom to realize considerably more functionalities. A multi-focal PS provides the possibility of splitting x-rays and further extends interferometry from visible light to hard x-rays.

Layered Chalcogenide Scintillators Enabled by Reversible Hydrous-Induced Phase Transformation for High-Resolution X-ray Imaging.

Scintillation materials have been widely used in various fields, such as medical diagnosis and industrial detection. Chalcogenides have the potential to become a new generation of high-performance scintillation materials due to their high effective atomic number and good resistance to radiation damage. However, research on their application in radiation detection is currently very scarce. Herein, single crystals of rare earth ion-doped ternary chalcogenides NaGaS2/Eu were grown by a high-temperature solid-phase method. It exhibits unique characteristics of structure transformation by absorbing water molecules from the air. To maintain the anhydrous phase of the material, we have used a strategy of organic-inorganic composites of epoxy resin and NaGaS2/Eu to prepare devices for radiation detection and discuss the irradiation luminescence properties of the two phases. The anhydrous phase of NaGaS2/Eu demonstrates excellent sensitivity to X-rays, with a low detection limit of 250 nGy s-1, which is approximately 1/22 of the medical imaging dose. Additionally, composite flexible films were prepared, which exhibited excellent performance in X-ray imaging. These films enable clear observation of a wide range of objects with a high spatial resolution of up to 13.2 line pairs per millimeter (lp mm-1), indicating that chalcogenide holds promising prospects in the realm of X-ray imaging applications.

Preparing the In-doped lead-free Cs3Cu2I5 perovskite scintillator by a co-firing technique for its application in high-resolution X-ray imaging

The perovskite scintillators have been extensively studied recently for their merits of tunable emission spectra and simple preparation processes. However, the practical applications of perovskite scintillator-based X-ray image sensor are still impeded by inadequate radioluminescence, poor environmental stability, and low imaging resolution. Herein, we demonstrate a scalable co-firing method to fabricate high-quality lead-free Cs3Cu2I5 perovskite scintillator and an Indium (In)-doping strategy is introduced to enhance its radioluminescence performance at the same time. The In-doped Cs3Cu2I5 obtains a high PLQY of 77.9% and a relative light output of 53372 ph/MeV, which are 0.34 and 1.08 times higher than those of the undoped counterpart, respectively. The X-ray detection limit of the In:Cs3Cu2I5 can reach 150.55 nGyair/s, 36.53 times lower than the requirement for X-ray medical diagnosis. The synthesized scintillator also shows superior stability under continuous high dose X-ray irradiation of 6800 μGyair/s for 120 minutes, maintaining 95% of its initial radioluminescence intensity. Furthermore, a large-area (300 cm2) flexible perovskite scintillator film is prepared, which owns a much competitive resolution of 10 lp/mm and less distortion in X-ray imaging. This work provides a practical path for the wide application of perovskite scintillator in the field of X-ray detection and imaging in near future.