High-resolution X-ray luminescence extension imaging.

Current X-ray imaging technologies involving flat-panel detectors have difficulty in imaging three-dimensional objects because fabrication of large-area, flexible, silicon-based photodetectors on highly curved surfaces remains a challenge1-3. Here we demonstrate ultralong-lived X-ray trapping for flat-panel-free, high-resolution, three-dimensional imaging using a series of solution-processable, lanthanide-doped nanoscintillators. Corroborated by quantum mechanical simulations of defect formation and electronic structures, our experimental characterizations reveal that slow hopping of trapped electrons due to radiation-triggered anionic migration in host lattices can induce more than 30 days of persistent radioluminescence. We further demonstrate X-ray luminescence extension imaging with resolution greater than 20 line pairs per millimetre and optical memory longer than 15 days. These findings provide insight into mechanisms underlying X-ray energy conversion through enduring electron trapping and offer a paradigm to motivate future research in wearable X-ray detectors for patient-centred radiography and mammography, imaging-guided therapeutics, high-energy physics and deep learning in radiology.

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.

High-Confidentiality X-Ray Imaging Encryption Using Prolonged Imperceptible Radioluminescence Memory Scintillators.

X-ray imaging plays an increasingly crucial role in clinical radiography, industrial inspection, and military applications. However, current X-ray imaging technologies have difficulty in protecting against information leakage caused by brute force attacks via trial-and-error. Here high-confidentiality X-ray imaging encryption by fabricating ultralong radioluminescence memory films composed of lanthanide-activated nanoscintillators (NaLuF4 : Gd3+ or Ce3+ ) with imperceptible purely-ultraviolet (UV) emission is reported. Mechanistic investigations unveil that ultralong X-ray memory is attributed to the long-lived trapping of thermalized charge carriers within Frenkel defect states and subsequent slow release in the form of imperceptible radioluminescence. The encrypted X-ray imaging can be securely stored in the memory film for more than 7 days and optically decoded by perovskite nanocrystal. Importantly, this encryption strategy can protect X-ray imaging information against brute force trial-and-error attacks through the perception of lifetime change in the persistent radioluminescence. It is further demonstrated that the as-fabricated flexible memory film enables achieving of 3D X-ray imaging encryption of curved objects with a high spatial resolution of 20 lp/mm and excellent recyclability. This study provides valuable insights into the fundamental understanding of X-ray-to-UV conversion in nanocrystal lattices and opens up a new avenue toward the development of high-confidential 3D X-ray imaging encryption technologies.

High-resolution flexible X-ray luminescence imaging enabled by eco-friendly CuI scintillators.

Solution-processed scintillators hold great promise in fabrication of low-cost X-ray detectors. However, state of the art of these scintillators is still challenging in their environmental toxicity and instability. In this study, we develop a class of tetradecagonal CuI microcrystals as highly stable, eco-friendly, and low-cost scintillators that exhibit intense radioluminescence under X-ray irradiation. The red broadband emission is attributed to the recombination of self-trapped excitons in CuI microcrystals. We demonstrate the incorporation of such CuI microscintillator into a flexible polymer to fabricate an X-ray detector for high-resolution imaging with a spatial resolution up to 20 line pairs per millimeter (lp mm-1), which enables sharp image effects by attaching the flexible imaging detectors onto curved object surfaces.

A Perovskite-Based Paper Microfluidic Sensor for Haloalkane Assays.

Detection of haloalkanes is of great industrial and scientific importance because some haloalkanes are found serious biological and atmospheric issues. The development of a flexible, wearable sensing device for haloalkane assays is highly desired. Here, we develop a paper-based microfluidic sensor to achieve low-cost, high-throughput, and convenient detection of haloalkanes using perovskite nanocrystals as a nanoprobe through anion exchanging. We demonstrate that the CsPbX3 (X = Cl, Br, or I) nanocrystals are selectively and sensitively in response to haloalkanes (CH2Cl2, CH2Br2), and their concentrations can be determined as a function of photoluminescence spectral shifts of perovskite nanocrystals. In particular, an addition of nucleophilic trialkyl phosphines (TOP) or a UV-photon-induced electron transfer from CsPbX3 nanocrystals is responsible for achieving fast sensing of haloalkanes. We further fabricate a paper-based multichannel microfluidic sensor to implement fast colorimetric assays of CH2Cl2 and CH2Br2. We also demonstrate a direct experimental observation on chemical kinetics of anion exchanging in lead-halide perovskite nanocrystals using a slow solvent diffusion strategy. Our studies may offer an opportunity to develop flexible, wearable microfluidic sensors for haloalkane sensing, and advance the in-depth fundamental understanding of the physical origin of anion-exchanged nanocrystals.

Broadband Detection of X-ray, Ultraviolet, and Near-Infrared Photons using Solution-Processed Perovskite-Lanthanide Nanotransducers.

Solution-processed metal-halide perovskites hold great promise in developing next-generation low-cost, high-performance photodetectors. However, the weak absorption of perovskites beyond the near-infrared spectral region posts a stringent limitation on their use for broadband photodetectors. Here, the rational design and synthesis of an upconversion nanoparticles (UCNPs)-perovskite nanotransducer are presented, namely UCNPs@mSiO2 @MAPbX3 (X = Cl, Br, or I), for broadband photon detection spanning from X-rays, UV, to NIR. It is demonstrated that, by in situ crystallization and deliberately tuning the material composition in the lanthanide core and perovskites, the nanotransducers allow for a high stability and show a wide linear response to X-rays of various dose rates, as well as UV/NIR photons of various power densities. The findings provide an opportunity to explore the next-generation broadband photodetectors in the field of high-quality imaging and optoelectronic devices.

Polyethylene Oxide-Based Composites as Solid-State Polymer Electrolytes for Lithium Metal Batteries: A Mini Review.

Solid-state polymer electrolytes (SPEs) have great processing flexibility and electrode-electrolyte contact and have been employed as the promising electrolytes for lithium metal batteries. Among them, poly(ethylene oxide) (PEO)-based SPEs have attracted widespread attention because of easy synthesis, low mass density, good mechanical stability, low binding energy with lithium salts, and excellent mobility of charge carriers. In order to overcome the low room-temperature ionic conductivity and the poor thermodynamic stability in high-voltage devices (>4.2 V) of the PEO materials, composition modulations by incorporating PEO with inorganic and/or organic components have been designed, which could effectively enable the applications of PEO-based SPEs with widened electro-stable voltage ranges. In this mini review, we describe recent progresses of several kinds of PEO composite structures for SPEs, and we compare the synthesis strategies and properties of these SPEs in lithium batteries. Further developments and improvements of the PEO-based materials for building better rechargeable batteries are also discussed.