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Lens-coupled X-ray computed tomography (X-ray CT) using a transparent scintillator imaged on a CCD camera obtains higher spatial resolution than the more commonly employed phosphor-enhanced amorphous silicon (A-Si) panels. A-Si panels are limited to resolution typically greater than ~200 microns, have a limited working life due to degradation with dose, and provide intrinsically low efficiency with thin (few hundred microns thick) phosphor coatings. Demanding applications such as imaging the interior of complex additively manufactured components require high throughput and high resolution, best achieved with a lens-coupled system. However, for large fields-of-view, very large area but thin transparent scintillators are required – a format difficult to fabricate with high light yield single crystals – therefore, glass scintillators with both modest X-ray interaction and light yield have been used for years. We have developed a new polycrystalline transparent ceramic scintillator, Gd0.3Lu1.6Eu0.1O3, or “GLO,” that offers excellent stopping power and light yield for improved contrast in sizes up to 14” x 14” plates, with thicknesses in the 2-10 mm range, and we are implementing it in systems to increase imaging throughput for 9 MeV Bremsstrahlung X-ray CT. CT imaging performance will be described.

We report on a small gamma spectrometer with directional detection, based on two modules. Each module contains an array of 128 scintillator pixels coupled to reverse-biased photodiodes, an ASIC and a microcontroller. Modules communicate via USB and are operated via an Android GUI on a WiFi-connected device. Transparent ceramic GYGAG ((Gd,Y,Ce)3(Ga,Al)5O12) garnet scintillator pixels offer energy resolution as good as 3.1% at 662 keV for individual pixels. We previously reported on an eight-module planar spectrometer, based on the same technology1. The current compact system uses two modules in a back-to-back configuration to improve its speed and accuracy in locating a gamma-emitting source in a 4-pi field of view. This dual module system (~2.5 x 2.5 x 3.5 inches) is suitable as a pager-sized RIID or spectroscopic personal radiation detector (SPRD). Multiple dual module units can be combined for improved efficiency. Spectroscopic and directional performance will be described.

Transparent ceramic fabrication via solid state sintering is opening a path to a new category of laser gain media with tailor-made doping and index profiles. Techniques such as assembly of green structure pieces, direct ink writing, and Ink jet printing allow the fabrication of a wide variety of tailored optics including; slabs, rods, gradient doping, thin disks, ceramic-clad single-crystal fibers, and planar waveguides. The potential for 3D printed gain media to have a profound impact on new laser design and integrated optics is yet untapped. This work was performed under the auspices of the U.S. DOE by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. LLNL-ABS-816729

High energy X-rays and neutrons can provide 3-D volumetric views of large objects made of multiple materials. Lenscoupled computed tomography using a scintillator imaged on a CCD camera obtains high spatial resolution, while a surface-mounted segmented scintillator on an amorphous silicon (A-Si) array can provide high throughput. For MeV Xray CT, a new polycrystalline transparent ceramic scintillator referred to as “GLO” offers excellent stopping power and light yield for improved contrast in sizes up to a 12” field-of-view. For MeV neutron CT, we have fabricated both contiguous and segmented plates of “Hi-LY” plastic scintillator, offering light yields 3x higher than standard plastic.

Inexpensive spectroscopic personal radiation detectors (SPRDs) are needed to monitor environmental radioactivity and search for sources. For gamma spectroscopy, excellent light yield, material uniformity, light yield proportionality, mechanical and environmental ruggedness can be achieved in polycrystalline ceramic oxide garnets. We are building a compact detector based on 14 cm3 of transparent ceramic garnet, formed into 256 pixels (3mm x 3mm x 6mm each) and mounted on two stacked silicon photodiode arrays. GYGAG(Ce) garnet transparent ceramics offer density = 5.8g/cm3, Zeff = 48, principal decay of

Gadolinium Garnet transparent ceramics doped with Ce, ((Gd,Y,Ce)3(Ga,Al)5O12), for gamma-ray spectroscopy provide high density, high light yield, high energy resolution , high Z, mechanical robustness, and they are unreactive to air and water. Gadolinium garnet single crystals are costly to grow, due to their high melting points, and suffer from non-uniform light yield, due to Ce segregation. In contrast, transparent polycrystalline ceramic Garnets are never melted, and therefore are less costly to produce and provide the uniform light yield required to achieve high energy resolution with a scintillator. GYGAG(Ce) transparent ceramics offer energy resolution as good as R(662 keV) = 3.5%, in a pixelated detector utilizing Silicon photodiode array readout. We have developed a modular handheld detector based on pixelated GYGAG(Ce) on a photodiode array, that offers directional detection for point source detection as well as gamma spectroscopy. Individual modules can be assembled into detectors ranging from pocket-size to large panels, for a range of applications. Large GYGAG(Ce) transparent ceramics in the 2-5 in3 size range have been fabricated at LLNL. Instrumentation of these ceramics with Silicon photomultipliers (SiPMs) and super bi-alkali PMTs has been explored and energy resolution as good as R(662 keV) = 5% has been obtained. Further improvements with SiPM readout will leverage their high quantum efficiency in the 500-650 nm range where GYGAG(Ce) emits, and implement electronics that minimize the effect of SiPM dark current and capacitance on the pulse height spectra. This work was performed under the auspices of the U.S. DOE by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344, and has been supported by the US Department of Homeland Security, Domestic Nuclear Detection Office, under competitively awarded IAA HSHQDC-12-X-00149 under Contract No. DE-AC03-76SF00098. LLNL-ABS-724480.

Breakthrough energy resolution, R(662keV)

We report on the development of two new mechanically rugged, high light yield transparent ceramic scintillators: (1) Ce-doped Gd-garnet for gamma spectroscopy, and (2) Eu-doped Gd-Lu-bixbyite for radiography. GYGAG(Ce) garnet transparent ceramics offer ρ = 5.8g/cm3, Zeff = 48, principal decay of 8 lp/mm.

Breakthrough energy resolution, R(662keV) < 4%, has been achieved with an oxide scintillator, Cerium-doped Gadolinium Yttrium Gallium Aluminum Garnet, or GYGAG(Ce). Transparent ceramic GYGAG(Ce), has a peak emission wavelength of 550 nm that is better matched to Silicon photodetectors than to standard PMTs. We are therefore developing a spectrometer based on pixelated GYGAG(Ce) on a Silicon photodiode array that can provide R(662 keV) = 3.6%. In comparison, with large 1-2 in3 size GYGAG(Ce) ceramics we obtain R(662 keV) = 4.6% with PMT readout. We find that ceramic GYGAG(Ce) of a given stoichiometric chemical composition can exhibit very different scintillation properties, depending on sintering conditions and post-anneal treatments. Among the characteristics of transparent ceramic garnet scintillators that can be controlled by fabrication conditions are: scintillation decay components and their amplitudes, intensity and duration of afterglow, thermoluminescence glow curve peak positions and amplitudes, integrated light yield, light yield non-proportionality - as measured in the Scintillator Light Yield Non-Proportionality Characterization Instrument (SLYNCI), and energy resolution for gamma spectroscopy. Garnet samples exhibiting a significant fraction of Cerium dopant in the tetravalent valence also exhibit: faster overall scintillation decay, very low afterglow, high light yield, but poor light yield proportionality and degraded energy resolution.

Results are presented of investigations into the composition, uniformity and gamma-ray imaging performance of new ceramic scintillators with synthetic garnet structure. The ceramic scintillators were produced by a process that uses flame pyrolysis to make nanoparticles which are sintered into a ceramic and then compacted by hot isostatic compression into a transparent material. There is concern that the resulting ceramic scintillator might not have the uniformity of composition necessary for use in gamma-ray spectroscopy and gamma-ray imaging. The compositional uniformity of four samples of three ceramic scintillator types (GYGAG:Ce, GLuGAG:Ce and LuAG:Pr) was tested using an electron microprobe. It was found that all samples were uniform in elemental composition to the limit of sensitivity of the microprobe (few tenths of a percent atomic) over distance scales from ~ 1 cm to ~ 1 um. The light yield and energy resolution of all ceramic scintillator samples were mapped with a highly collimated 57Co source (122 keV) and performance was uniform at mapping scale of 0.25 mm. Good imaging performance with single gamma-ray photon detection was demonstrated for all samples using a BazookaSPECT system, and the imaging spatial resolution, measured as the FWHM of a LSF was 150 um.

Recently discovered scintillators for gamma ray spectroscopy, single crystal SrI{sub 2}(Eu), GYGAG(Ce) transparent ceramic and Bismuth-loaded plastics, offer resolution and fabrication advantages compared to commercial scintillators, such as NaI(Tl) and standard PVT plastic. Energy resolution at 662 keV of 2.7% is obtained with SrI{sub 2}(Eu), while 4.5% is obtained with GYGAG(Ce). A new transparent ceramic scintillator for radiographic imaging systems, GLO(Eu) offers high light yield of 70,000 Photons/MeV, high stopping, and low radiation damage. Implementation of single crystal SrI{sub 2}(Eu), Gd-based transparent ceramics, and Bi-loaded plastic scintillators can advance the state-of-the art in ionizing radiation detection systems.

Transparent ceramics combine the scintillation performance of single crystals with the ruggedness and processability of glass. We have developed a versatile, scaleable fabrication method, wherein nanoparticle feedstock is consolidated at temperatures well below melting to form inch-scale phase-pure transparent ceramics with optical scatter of α