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70 result(s) for "Dujardin, Christophe"
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Efficient radioactive gas detection by scintillating porous metal–organic frameworks
Natural and anthropogenic gas radionuclides such as radon, xenon, hydrogen and krypton isotopes must be monitored to be managed as pathogenic agents, radioactive diagnostic agents or nuclear activity indicators. State-of-the-art detectors based on liquid scintillators suffer from laborious preparation and limited solubility for gases, which affect the accuracy of the measurements. The actual challenge is to find solid scintillating materials simultaneously capable of concentrating radioactive gases and efficiently producing visible light revealed with high sensitivity. The high porosity, combined with the use of scintillating building blocks in metal–organic frameworks (MOFs), offers the possibility to satisfy these requisites. We demonstrate the capability of a hafnium-based MOF incorporating dicarboxy-9,10-diphenylanthracene as a scintillating conjugated ligand to detect gas radionuclides. Metal–organic frameworks show fast scintillation, a fluorescence yield of ∼40%, and accessible porosity suitable for hosting noble gas atoms and ions. Adsorption and detection of 85Kr, 222Rn and 3H radionuclides are explored through a newly developed device that is based on a time coincidence technique. Metal–organic framework crystalline powder demonstrated an improved sensitivity, showing a linear response down to a radioactivity value below 1 kBq m−3 for 85Kr, which outperforms commercial devices. These results support the possible use of scintillating porous MOFs to fabricate sensitive detectors of natural and anthropogenic radionuclides.Detection of gas radionuclides is limited in sensitivity with present methods, but may be useful in energy, security, medical and other sectors. In this work, gas-concentrating porous scintillating metal–organic frameworks are demonstrated for gas radionuclide detection.
Inorganic, Organic, and Perovskite Halides with Nanotechnology for High–Light Yield X- and γ-ray Scintillators
Trends in scintillators that are used in many applications, such as medical imaging, security, oil-logging, high energy physics and non-destructive inspections are reviewed. First, we address traditional inorganic and organic scintillators with respect of limitation in the scintillation light yields and lifetimes. The combination of high–light yield and fast response can be found in Ce 3 + , Pr 3 + and Nd 3 + lanthanide-doped scintillators while the maximum light yield conversion of 100,000 photons/MeV can be found in Eu 3 + doped SrI 2 . However, the fabrication of those lanthanide-doped scintillators is inefficient and expensive as it requires high-temperature furnaces. A self-grown single crystal using solution processes is already introduced in perovskite photovoltaic technology and it can be the key for low-cost scintillators. A novel class of materials in scintillation includes lead halide perovskites. These materials were explored decades ago due to the large X-ray absorption cross section. However, lately lead halide perovskites have become a focus of interest due to recently reported very high photoluminescence quantum yield and light yield conversion at low temperatures. In principle, 150,000–300,000 photons/MeV light yields can be proportional to the small energy bandgap of these materials, which is below 2 eV. Finally, we discuss the extraction efficiency improvements through the fabrication of the nanostructure in scintillators, which can be implemented in perovskite materials. The recent technology involving quantum dots and nanocrystals may also improve light conversion in perovskite scintillators.
A compact detector system for simultaneous measurements of the light yield non-linearity and timing properties of scintillators
This work presents an outline of a detection system that employs the Compton spectrometer method to assess the non-linearity of scintillator light yield. A novel approach is introduced, leading to more accurate measurements through the separate determination of the intrinsic light output parameters and the non-linearity of the scintillators. Key features of this system include the use of a portable scintillation detector with three photomultiplier tubes for precise measurement of the average number of detected photoelectrons and the incorporation of recent advancements in correction techniques for accidental coincidences. The integration of digital acquisition, offline data analysis, and geometric adaptation reduces the time required to perform a measurement. The developed detector can simultaneously measure different timing properties, as well as the relative intensities following ionization excitation in a scintillator. The system’s performance is demonstrated through measurements of the light yield dependence on the deposited energy for commercially available liquid, plastic, and inorganic scintillators. Such instrumentation serves as a valuable tool in the development of novel scintillating materials, including liquid or solid organic scintillators, inorganic scintillators, and composite scintillators for electron detection, in addition to traditional X-ray or γ -ray detection.
Lithium-doped two-dimensional perovskite scintillator for wide-range radiation detection
Two-dimensional lead halide perovskites have demonstrated their potential as high-performance scintillators for X- and gamma-ray detection, while also being low-cost. Here we adopt lithium chemical doping in two-dimensional phenethylammonium lead bromide (PEA)2PbBr4 perovskite crystals to improve the properties and add functionalities with other radiation detections. Li doping is confirmed by X-ray photoemission spectroscopy and the scintillation mechanisms are explored via temperature dependent X-ray and thermoluminescence measurements. Our 1:1 Li-doped (PEA)2PbBr4 demonstrates a fast decay time of 11 ns (80%), a clear photopeak with an energy resolution of 12.4%, and a scintillation yield of 11,000 photons per MeV under 662 keV gamma-ray radiation. Additionally, our Li-doped crystal shows a clear alpha particle/gamma-ray discrimination and promising thermal neutron detection through 6Li enrichment. X-ray imaging pictures with (PEA)2PbBr4 are also presented. All results demonstrate the potential of Li-doped (PEA)2PbBr4 as a versatile scintillator covering a wide radiation energy range for various applications.Two-dimensional lead halide perovskites have shown great potential as X- and γ-ray scintillators due to their high light yield, fast decay rate, and low fabrication cost. Here, their versatility is expanded by achieving, via Li-doping, α-particle/γ-ray discrimination and thermal neutron detection.
Low-Temperature Emission Dynamics of Methylammonium Lead Bromide Hybrid Perovskite Thin Films at the Sub-Micrometer Scale
We study the low-temperature (T = 4.7 K) emission dynamics of a thin film of methylammonium lead bromide (MAPbBr3), prepared via the anti-solvent method. Using intensity-dependent (over 5 decades) hyperspectral microscopy under quasi-resonant (532 nm) continuous wave excitation, we revealed spatial inhomogeneities in the thin film emission. This was drastically different at the band-edge (∼550 nm, sharp peaks) than in the emission tail (∼568 nm, continuum of emission). We are able to observe regions of the film at the micrometer scale where emission is dominated by excitons, in between regions of trap emission. Varying the density of absorbed photons by the MAPbBr3 thin films, two-color fluorescence lifetime imaging microscopy unraveled the emission dynamics: a fast, resolution-limited (∼200 ps) monoexponential tangled with a stretched exponential decay. We associate the first to the relaxation of excitons and the latter to trap emission dynamics. The obtained stretching exponents can be interpreted as the result of a two-dimensional electron diffusion process: Förster resonant transfer mechanism. Furthermore, the non-vanishing fast monoexponential component even in the tail of the MAPbBr3 emission indicates the subsistence of localized excitons. Finally, we estimate the density of traps in MAPbBr3 thin films prepared using the anti-solvent method at n∼1017 cm−3.
Radiation Dose‐Enhancement Is a Potent Radiotherapeutic Effect of Rare‐Earth Composite Nanoscintillators in Preclinical Models of Glioblastoma
To improve the prognosis of glioblastoma, innovative radiotherapy regimens are required to augment the effect of tolerable radiation doses while sparing surrounding tissues. In this context, nanoscintillators are emerging radiotherapeutics that down‐convert X‐rays into photons with energies ranging from UV to near‐infrared. During radiotherapy, these scintillating properties amplify radiation‐induced damage by UV‐C emission or photodynamic effects. Additionally, nanoscintillators that contain high‐Z elements are likely to induce another, currently unexplored effect: radiation dose‐enhancement. This phenomenon stems from a higher photoelectric absorption of orthovoltage X‐rays by high‐Z elements compared to tissues, resulting in increased production of tissue‐damaging photo‐ and Auger electrons. In this study, Geant4 simulations reveal that rare‐earth composite LaF3:Ce nanoscintillators effectively generate photo‐ and Auger‐electrons upon orthovoltage X‐rays. 3D spatially resolved X‐ray fluorescence microtomography shows that LaF3:Ce highly concentrates in microtumors and enhances radiotherapy in an X‐ray energy‐dependent manner. In an aggressive syngeneic model of orthotopic glioblastoma, intracerebral injection of LaF3:Ce is well tolerated and achieves complete tumor remission in 15% of the subjects receiving monochromatic synchrotron radiotherapy. This study provides unequivocal evidence for radiation dose‐enhancement by nanoscintillators, eliciting a prominent radiotherapeutic effect. Altogether, nanoscintillators have invaluable properties for enhancing the focal damage of radiotherapy in glioblastoma and other radioresistant cancers. Radiation dose‐enhancement induced by rare‐earth composite nanoscintillators is predicted by in silico simulations and unequivocally demonstrates in vitro in microtumor models of glioblastoma, using tunable monochromatic synchrotron radiation. Radiation dose‐enhancement ultimately elicitsa prominent radiotherapeutic effect in a syngeneic orthotopic model of aggressive glioblastoma. These results prove the strong ability of rare‐earth composite nanoscintillators to enhance the focal damage of radiotherapy.
Revisiting the Impact of Tungsten on the Catalytic Properties of Ammonia-SCR V2O5-WO3/TiO2 Catalysts: Geometric vs. Electronic Effects
The SCR performance of V2O5-WO3/TiO2 SCR-catalysts characterized by different surface W density (2.1W/nm2 and 9.5W/nm2) and different surface V density varying in the range 1–8V/nm2 has been investigated in order to clarify existing controversies on the preferential involvement of electronic and geometric effects in the catalytic properties. It was found that tungsten has a weak effect on the VOx cluster size distribution through contraction of dilution effect. In contrast, the optimal interaction between W and V, when both reach their highest composition, appears to be a relevant parameter that can enhance their acidic properties and improve the catalytic efficiency in dry conditions. On the other hand, an absence of significant interaction leads to discontinuity due to deactivation. In the presence of steam, acidic properties are averaged, lowering the impact of the V to W ratio. Finally, the critical importance of acidic properties which outperform redox properties in the definition of active site is pointed out in the light of this study.
Quantifying Titanium Exposure in Lung Tissues: A Novel Laser‐Induced Breakdown Spectroscopy Elemental Imaging‐Based Analytical Framework for Biomedical Applications
Occupational and environmental exposures, particularly those related to urban and suburban atmospheres, are increasingly linked to a range of pulmonary diseases. While diagnostic methods for these diseases are well established, analytical tools for assessing elemental contamination in lung tissue remain underutilized. This study introduces a novel framework based on laser‐induced breakdown spectroscopy (LIBS) for the in situ quantification of elemental titanium (Ti) in lung tissues from both animal models and human specimens. Rigorous validation is conducted using animal models exposed to TiO 2 P25 nanoparticles and a comparative analysis with inductively coupled plasma mass spectrometry. The novel quantitative metric demonstrates robust correlation with elemental concentrations, expanding LIBS utility to volumetric organ analysis. This validated methodology is subsequently applied to human lung specimens preserved in paraffin. The research holds significant promise as a diagnostic tool for assessing exposure levels to environmental or occupational hazards, thereby offering valuable contributions to the fields of toxicology and respiratory medicine.
Composite fast scintillators based on high-Z fluorescent metal–organic framework nanocrystals
Scintillators, materials that produce light pulses upon interaction with ionizing radiation, are widely employed in radiation detectors. In advanced medical-imaging technologies, fast scintillators enabling a time resolution of tens of picoseconds are required to achieve high-resolution imaging at the millimetre length scale. Here we demonstrate that composite materials based on fluorescent metal–organic framework (MOF) nanocrystals can work as fast scintillators. We present a prototype scintillator fabricated by embedding MOF nanocrystals in a polymer. The MOF comprises zirconium oxo-hydroxy clusters, high-Z linking nodes interacting with the ionizing radiation, arranged in an orderly fashion at a nanometric distance from 9,10-diphenylanthracene ligand emitters. Their incorporation in the framework enables fast sensitization of the ligand fluorescence, thus avoiding issues typically arising from the intimate mixing of complementary elements. This proof-of-concept prototype device shows an ultrafast scintillation rise time of ~50 ps, thus supporting the development of new scintillators based on engineered fluorescent MOF nanocrystals.Composites of fluorescent metal–organic framework nanocrystals in a polymer are exploited to create fast scintillators with a rise time of about 50 ps.