Ultrafast and Radiation-Hard Lead Halide Perovskite Nanocomposite Scintillators.

The use of scintillators for the detection of ionizing radiation is a critical aspect in many fields, including medicine, nuclear monitoring, and homeland security. Recently, lead halide perovskite nanocrystals (LHP-NCs) have emerged as promising scintillator materials. However, the difficulty of affordably upscaling synthesis to the multigram level and embedding NCs in optical-grade nanocomposites without compromising their optical properties still limits their widespread use. In addition, fundamental aspects of the scintillation mechanisms are not fully understood, leaving the scientific community without suitable fabrication protocols and rational guidelines for the full exploitation of their potential. In this work, we realize large polyacrylate nanocomposite scintillators based on CsPbBr3 NCs, which are synthesized via a novel room temperature, low waste turbo-emulsification approach, followed by their in situ transformation during the mass polymerization process. The interaction between NCs and polymer chains strengthens the scintillator structure, homogenizes the particle size distribution and passivates NC defects, resulting in nanocomposite prototypes with luminescence efficiency >90%, exceptional radiation hardness, 4800 ph/MeV scintillation yield even at low NC loading, and ultrafast response time, with over 30% of scintillation occurring in the first 80 ps, promising for fast-time applications in precision medicine and high-energy physics. Ultrafast radioluminescence and optical spectroscopy experiments using pulsed synchrotron light further disambiguate the origin of the scintillation kinetics as the result of charged-exciton and multiexciton recombination formed under ionizing excitation. This highlights the role of nonradiative Auger decay, whose potential impact on fast timing applications we anticipate via a kinetic model.

Bragg coherent diffraction imaging with the CITIUS charge-integrating detector.

The CITIUS detector is a next-generation high-speed X-ray imaging detector. It has integrating-type pixels and is designed to show a consistent linear response at a frame rate of 17.4 kHz, which results in a saturation count rate of over 30 Mcps pixel-1 when operating at an acquisition duty cycle close to 100%, and up to 20 times higher with special extended acquisition modes. Here, its application for Bragg coherent diffraction imaging is demonstrated by taking advantage of the fourth-generation Extremely Brilliant Source of the European Synchrotron (ESRF-EBS, Grenoble, France). The CITIUS detector outperformed a photon-counting detector, similar spatial resolution being achieved (20 ±â€…6 nm versus 22 ±â€…9 nm) with greatly reduced acquisition times (23 s versus 200 s). It is also shown how the CITIUS detector can be expected to perform during dynamic Bragg coherent diffraction imaging measurements. Finally, the current limitations of the CITIUS detector and further optimizations for coherent imaging techniques are discussed.

Indirect X-ray detectors with single-photon sensitivity.

The new generation of synchrotron light sources are pushing X-ray detectors to their limits. Very demanding conditions with unprecedented flux and higher operating energies now require high-performance X-ray detectors combining sensitivity, efficiency and scalability. Over the years, hybrid pixel detectors have supplemented indirect detectors based on scintillation, with undeniable advantages. Such detectors based on silicon are, however, rather expensive to produce and are no more satisfying in terms of X-ray stopping power when targeting energies above 20 keV. An indirect detector with single X-ray photon sensitivity therefore offers promising opportunities for applications operating over a wide range of energies and fluxes. In this work, the performances of such an approach are investigated with state-of-the-art elements: a commercial sCMOS camera with fiber-optics plate coupling and a Gd2O2S:Tb powder-based scintillator. A simple method is presented for evaluation of the single X-ray photon detection limit and single X-ray sensitivity is demonstrated with the studied detector above 20 keV. Geant4 simulations also provide insight to better define the limiting factors. Finally, guidelines are provided for future R&D in the design and assembly of an innovative detector combining advantages of direct and indirect detection schemes.

Radiation hardness of Ce-doped sol-gel silica fibers for high energy physics applications.

The results of irradiation tests on Ce-doped sol-gel silica using x- and γ-rays up to 10 kGy are reported in order to investigate the radiation hardness of this material for high-energy physics applications. Sol-gel silica fibers with Ce concentrations of 0.0125 and 0.05 mol. % are characterized by means of optical absorption and attenuation length measurements before and after irradiation. The two different techniques give comparable results, evidencing the formation of a main broad radiation-induced absorption band, peaking at about 2.2 eV, related to radiation-induced color centers. The results are compared with those obtained on bulk silica. This study reveals that an improvement of the radiation hardness of Ce-doped silica fibers can be achieved by reducing Ce content inside the fiber core, paving the way for further material development.

Measurement of intrinsic rise times for various L(Y)SO and LuAG scintillators with a general study of prompt photons to achieve 10 ps in TOF-PET.

The coincidence time resolution (CTR) of scintillator based detectors commonly used in positron emission tomography is well known to be dependent on the scintillation decay time (τd) and the number of photons detected (n'), i.e. CTR proportional variant √τd/n'. However, it is still an open question to what extent the scintillation rise time (τr) and other fast or prompt photons, e.g. Cherenkov photons, at the beginning of the scintillation process influence the CTR. This paper presents measurements of the scintillation emission rate for different LSO type crystals, i.e. LSO:Ce, LYSO:Ce, LSO:Ce codoped Ca and LGSO:Ce. For the various LSO-type samples measured we find an average value of 70 ps for the scintillation rise time, although some crystals like LSO:Ce codoped Ca seem to have a much faster rise time in the order of 20 ps. Additional measurements for LuAG:Ce and LuAG:Pr show a rise time of 535 ps and 251 ps, respectively. For these crystals, prompt photons (Cherenkov) can be observed at the beginning of the scintillation event. Furthermore a significantly lower rise time value is observed when codoping with calcium. To quantitatively investigate the influence of the rise time to the time resolution we measured the CTR with the same L(Y)SO samples and compared the values to Monte Carlo simulations. Using the measured relative light yields, rise- and decay times of the scintillators we are able to quantitatively understand the measured CTRs in our simulations. Although the rise time is important to fully explain the CTR variation for the different samples tested we determined its influence on the CTR to be in the order of a few percent only. This result is surprising because, if only photonstatistics of the scintillation process is considered, the CTR would be proportional to the square root of the rise time. The unexpected small rise time influence on the CTR can be explained by the convolution of the scintillation rate with the single photon time resolution (SPTR) of the photodetector and the photon travel spread (PTS) in the crystal. The timing benefits of prompt photons at the beginning of the scintillation process (Cherenkov etc) are further studied, which leads to the conclusion that the scintillation rise time, SPTR and PTS have to be lowered simultaneously to fully profit from these fast photons in order to improve the CTR significantly.

In vivo imaging of S-layer nanoarrays on Corynebacterium glutamicum.

Crystalline bacterial cell surface layers (S-layers) are monomolecular arrays of (glyco)proteins that have recently produced a wealth of new opportunities in nanotechnology. Whereas the in vitro imaging of isolated S-layers is well established, their direct imaging on live cells remains very challenging. Here we use atomic force microscopy (AFM) to visualize S-layer nanoarrays on living Corynebacterium glutamicum bacteria. We demonstrate the presence of two highly ordered surface layers. The most external layer represents the hexagonal S-layer, and the inner layer displays regular patterns of nanogrooves that could act as a biomolecular template promoting the 2-D assembly of S-layer monomers. These nanoscale analyses open new avenues for understanding the structure of protein monomolecular arrays, which is a crucial challenge in current nanoscience and life science research.