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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. [ABSTRACT FROM AUTHOR]

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 challenge.sup.1-3. 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. Using lanthanide-doped nanomaterials and flexible substrates, an approach that enables flat-panel-free, high-resolution, three-dimensional imaging is demonstrated and termed X-ray luminescence extension imaging., Author(s): Xiangyu Ou [sup.1] , Xian Qin [sup.2] , Bolong Huang [sup.3] , Jie Zan [sup.1] , Qinxia Wu [sup.1] , Zhongzhu Hong [sup.1] , Lili Xie [sup.1] , Hongyu [...]

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 NaLuF 4 :Mn 2+ /Gd 3+ nanocrystal sublattices through Gd 3+ -driven microenvironment engineering and Mn 2+ -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 2.38×10 5 and 1.34×10 7  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., (© 2024 Wiley-VCH GmbH.)