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Transparent ceramic Er:YAG laser rods were fabricated via the direct ink write (DIW) method with engineered doping profiles featuring an Er-doped core with endcaps and core-clad structures. Laser rods up to 11 cm in length were produced which required development of a scalable process. To achieve this, multiple improvements were implemented, including printing the rods horizontally on a substrate, rather than vertically, eliminating the need for an external support structure and using a sacrificial drying layer to mitigate warping and defects. Highly transparent rods were achieved with optical scatter levels as low as 0.5%/cm (at 543 nm). A small refractive index difference of 5.7 ppm was measured at the interface between the Er-doped core and the Lu-doped endcaps and cladding. These results demonstrate DIW as a straightforward method for making good optical quality laser rods with engineered doping profiles to improve laser performance.

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.

A novel type of Yb:YAG transparent ceramic thin disk laser amplifier is demonstrated, based on fabricating a composite gain element with a paraboloidal interface between gain and no-gain regions and employing side-pumping of the thin disk. The pump-induced gain and the impact of amplified spontaneous emission on the achievable inversion are reported.

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.

A new narrowband red phosphor, Ba0.8Sr0.2Mg3SiN4:Eu, suitable for use in LED lighting, has been identified as the optimal composition from the series of Ba(1-x)SrxMg3SiN4:Eu including x = 0, 0.2, 0.5, 0.8, and 1. Experimental X-ray diffraction measurements and structures calculated via density functional theory reveal that Ba(1-x)SrxMg3SiN4:Eu stabilizes in a tetragonal crystal structure, changing to the triclinic structure for Ba >0.8. Narrow band Eu2+ emission is observed in the tetragonal phase, but as a function of Ba substitution onto the Sr site, several properties change in concert: the emission maximum shifts to longer wavelengths, room temperature quantum efficiency improves, Eu2+ decay time increases and thermal stability of emission improves. Concomitant with the structure change to triclinic, the narrow Eu2+ emission band becomes broadened, the bandgap increases, and decay time slows to a typical Eu2+ decay of ∼1 μs. Although significantly moisture-sensitive, the strong absorption of Ba0.8Sr0.2Mg3SiN4:Eu at 450 nm, its emission peak at 635 nm and width of 51 nm FWHM provide efficient color rendering in the red, potentially achieving CRI and R9 values in excess of 95, along with good efficacy, in combination with other phosphors. Excitation intensity droop is comparable to other similar Eu-doped nitrides, but while thermally induced quenching is reduced with Ba substitution, it is still significant. The measured photoluminescence decay for Ba0.8Sr0.2Mg3SiN4:Eu of ∼200 ns is faster than of related Eu-doped nitrides, and together with a Q.E. of only ∼40% suggests the presence of competing non-radiative decay routes, thought to be due to thermal ionization of the Eu2+ excited state to the conduction band. Improved Q.E. for SrMg3SiN4:Eu partially substituted with Ba is likely due to the cation disorder this introduces, suppressing nonradiative processes correlated with lattice vibrations and increasing the population of shallow traps that release electrons on the emission lifetime timescale, consistent with the emission decay time lengthening and Q.E. improvement as a function of Ba content.

We have developed a handheld $\gamma $ -ray spectrometer based on 1024 pixels, $2.8\,\,\text {mm} \times 2.8\,\,\text {mm} \times 6$ mm in size, of gadolinium–yttrium–gallium–aluminum garnet (GYGAG) ((Gd,Y,Ce)3(Ga,Al)5O12) ceramic scintillator (total of 48-cm3 detector volume) coupled to silicon photodiode (SiPD) arrays. The SiPD arrays and readout ASIC, originally developed for medical imaging applications, have been adapted for portability in a lightweight box with heatsink and thermoelectric cooling. Custom readout firmware for $\gamma $ -ray spectroscopy has been implemented, and a system user interface was developed that runs on an Android tablet. We have optimized the processing of the GYGAG(Ce), the pixel optical coupling, and electronics readout parameters to obtain single pixel energy resolution as good as $R (662\,\,\text {keV}) = 3.1$ % full-width at half-maximum and full device resolution with singles events from all pixels summed of 4.5%. When Compton-summed events are included, full-energy peak efficiency increases by $\sim 2\times $ , and $R (662\,\,\text {keV}) = 4.7$ % is obtained for the full device. The pixelated architecture is leveraged to locate point sources of radiological materials using Compton imaging and active masking techniques. Directional detection of a 1 mCi Cs-137 source at 10 m can be made to ±10° in ~2 s.

Solid-state laser gain media based on the garnet structure with two spatially distinct but optically contiguous regions have been fabricated. Transparent gain media comprised of a central core of Y2.97Nd0.03Al5.00O12.00 (Nd:YAG) and an undoped cladding region of Y3Al5O12 (YAG) were fabricated by direct ink write and transparent ceramic processing. Direct ink write (DIW) was employed to form the green body, offering a general route to preparing functionally structured solid-state laser gain media. Fully-dense transparent optical ceramics in a “top hat” geometry with YAG/Nd:YAG have been fabricated by DIW methods with optical scatter at 1064 nm of

Spatially distinct and graded doping profiles may be formed in YAG transparent ceramic laser gain media via additive manufacturing. Near-uniform refractive index may be obtained with co-doping of the undoped region with a compensating ion.

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

A new, to the best of our knowledge, 3D additive manufacturing technique utilizing particle-loaded ink jet printing to fabricate transparent ceramic Yb:YAG planar waveguides for laser gain media was demonstrated. Rheological optimization of YAG particle-loaded inks resulted in successful droplet formation and printing resolution. Planar waveguides composed of a Yb:YAG guide encased in undoped YAG cladding were printed with guide thicknesses ranging between 25 and 350 µm and consolidated to high optical quality via solid-state sintering. Sufficiently low optical (1–3%/cm) and intermodal scatter allowed single-mode propagation with a core/clad index difference of Δ n ∼ 5.0 × 10 − 4 (corresponding to 3 at.% Yb). The waveguides were cladding-pumped longitudinally with a 940 nm diode array resulting in 23.6% slope efficiency in 2 ms pulsed operation.

Development of next generation red phosphors for commercial lighting requires understanding of how increased luminescence is achieved by various treatment strategies. In this work, we compare co-doping with Nb to NH 3 treatment of CaTiO 3 :Pr phosphors to reveal a general mechanism responsible for the increased luminescence. The phosphors were synthesized using standard solid-state synthesis techniques and the fluorescence was characterized for potential use in fluorescent lighting, with 254 nm excitation. The lifetime of the fluorescence was determined and used to identify a change in a trap state by the co-doping of Nb 5+ in the phosphor. The oxidation state of the Pr was probed by NEXAFS and revealed that both Nb 5+ co-doping and NH 3 treatment reduced the number of non-fluorescing Pr 4+ centers. Calculations were performed to determine the energetically favorable defects. Vacuum annealing was also used to further probe the nature of the trap state. It was determined that NH 3 treatments reduce the number of Pr 4+ non-fluorescing centers, while Nb 5+ co-doping additionally reduces the number of excess oxygen trap states that quench the fluorescence.

We report high efficiency luminescence with a manganese-doped aluminum nitride red-emitting phosphor under 254 nm excitation, as well as its excellent lumen maintenance in fluorescent lamp conditions, making it a candidate replacement for the widely deployed europium-doped yttria red phosphor. Solid-state reaction of aluminum nitride powders with manganese metal at 1900 °C, 10 atm N2 in a reducing environment results in nitrogen deficiency, as revealed diffuse reflectance spectra. When these powders are subsequently annealed in flowing nitrogen at 1650 °C, higher nitrogen content is recovered, resulting in white powders. Silicon was added to samples as an oxygen getter to improve emission efficiency. NEXAFS spectra and DFT calculations indicate that the Mn dopant is divalent. From DFT calculations, the UV absorption band is proposed to be due to an aluminum vacancy coupled with oxygen impurity dopants, and Mn2+ is assumed to be closely associated with this site. In contrast with some previous reports, we find that the highest quantum efficiency with 254 nm excitation (Q.E. = 0.86 ± 0.14) is obtained in aluminum nitride with a low manganese doping level of 0.06 mol.%. The principal Mn2+ decay of 1.25 ms is assigned to non-interacting Mn sites, while additional components in the microsecond range appear with higher Mn doping, consistent with Mn clustering and resultant exchange coupling. Slower components are present in samples with low Mn doping, as well as strong afterglow, assigned to trapping on shallow traps followed by detrapping and subsequent trapping on Mn.

A new transparent ceramic phosphor for use in LED lighting has been fabricated. The previously reported and optimized narrow-emitting red phosphor, K2SiF6:Mn4+ (KSF), has been consolidated into a transparent ceramic phosphor for the first time, accomplished via hot-pressing the feedstock phosphor powder in a die under vacuum. KSF ceramics were fabricated with varying doping concentrations of Mn4+ and their properties studied. The absorption and emission spectra of the ceramics were identical to the feedstock phosphor powders and are ideal for LED lighting with strong absorption at 450 nm and narrow emission around 630 nm. The absorbance of the ceramics was directly proportional to the doping concentration. The ceramics were excited at various blue light fluxes and their emission intensities measured to study the effect of Mn4+ concentration on intensity-driven “droop” in the emission output. The ceramics with a lower Mn4+ doping were more efficient under higher light fluxes due to a decrease in Auger upconversion losses. KSF ceramics can allow a much longer path length of the diode light through the phosphor, as compared to phosphor-in-silicone, enabling the use of low optical absorption and the associated reduced activator concentration. The ceramics are measured to have a thermal conductivity of ~1.0 W/m-K, higher than that of phosphor-in-silicone or phosphor-in-glass. Several of these properties make KSF ceramics potentially desirable for use in white light LEDs. Greater thermal conductivity helps with heat dissipation, the lower surface area of the ceramic compared to the powder minimizes the environmental vulnerability of KSF, and the ability to lower the Mn4+ concentration reduces Auger recombination losses and mitigates the temperature rise, particularly at higher light flux.

Yttrium Aluminum Garnet (YAG) solid state laser gain media rods with an active Neodymium-doped core and an optically-clear cladding region were additively manufactured via direct-ink-writing (DIW), followed by sintering and hot isostatic pressing to form fully dense optical ceramics. Lutetium and Gadolinium were chosen as optically-inert co-doping ions in the clad to match the increase in refractive index caused by the Neodymium in the core. Either 11.6% Lutetium or 3.8% Gadolinium can be used to match the index change from 2% neodymium; however, differences in diffusion distances across the core-clad interface lead to large fluctuations in index in that region. These index fluctuations can be minimized either by matching dopants with similar diffusion distances, or by implementing a gradual gradient in the doping profile, possible through DIW, rather than a sharp compositional interface attainable via more standard fabrication methods. This improvement in index homogeneity resulted in a 40% improvement in lasing performance compared with that of a core-clad rod fabricated with a sharp interface between the doped and undoped regions.

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.

New transparent ceramic scintillators offer advantages for applications in gamma spectroscopy and X-ray imaging. For gamma spectroscopy, excellent light yield, material uniformity, light yield proportionality, mechanical and environmental ruggedness can be achieved in polycrystalline ceramic oxide garnets. We have fabricated 5 in3 Ce-doped Gd garnet transparent ceramics. GYGAG(Ce) garnet transparent ceramics offer $^{\mathbf {\rho \, =\, 5.8g/cm^{3},\,}}$, $z_{eff}=48$, principal decay of 2 O 3 structure structure. The 12” x 12” GLO imaging plates outperform scintillator glass for MeV radiography, due to higher light yield (55,000 Ph/MeV) and better stopping, while providing spatial resolution of >8 lp/mm for MeV X-rays.

Transparent polycrystalline ceramic scintillators based on the garnet structure and incorporating gadolinium for high stopping power are being developed for use in gamma spectrometers. Optimization of energy resolution for gamma spectroscopy involves refining the material composition for high stopping and high light yield, developing ceramics fabrication methodology for material homogeneity, as well as selecting the size and geometry of the scintillator to match the photodetector characteristics and readout electronics. We have demonstrated energy resolution of 4% at 662 keV for 0.05 cm3 GYGAG(Ce) ceramics with photodiode readout, and 4.9% resolution at 662 keV for 18 cm 3 GYGAG(Ce) ceramics and PMT readout. Comparative gamma spectra acquired with GYGAG(Ce) and NaI(Tl) depict the higher resolution of GYGAG(Ce) for radioisotope identification applications. Light yield non-proportionality of garnets fabricated following different methods reveal that the fundamental shapes of the light yield dependence on energy are not intrinsic to the crystal structure, but may instead depend on trap state distributions. With exposure to 9 MeV Brehmsstrahlung radiation, we also find that GYGAG(Ce) ceramics exhibit excellent radiation hardness.

Breakthrough energy resolution, R(662keV)

Gadolinium lutetium oxide transparent ceramics doped with europium (Gd,Lu) 2 O 3 :Eu were fabricated via vacuum sintering and hot isostatic pressing (HIP). Nano-scale starting powder with the composition Gd x Lu 1.9− x Eu 0.1 O 3 ( x = 0, 0.3, 0.6, 0.9, 1.0, and 1.1) were uniaxially pressed and sintered under high vacuum at 1625 °C to obtain ∼97% dense structures with closed porosity. Sintered compacts were then subjected to 200 MPa argon gas at temperatures between 1750 and 1900 °C to reach full density. It was observed that a small portion of the Eu 3+ ions were exsolved from the Lu 2 O 3 cubic crystal lattice and concentrated at the grain boundaries, where they precipitated into a secondary monoclinic phase creating optical scattering defects. Addition of Gd 3+ ions into the Lu 2 O 3 cubic lattice formed the solid solution (Gd,Lu) 2 O 3 :Eu and stretched the lattice parameter allowing the larger Eu 3+ ions to stay in solid solution, reducing the secondary phase and improving the transparency of the ceramics. Excess gadolinium, however, resulted in a complete phase transformation to monoclinic at pressures and temperatures sufficient for densification. Light yield performance was measured and all samples show equal amounts of the characteristic Eu 3+ luminescence, indicating gadolinium addition had no adverse effect. This material has potential to improve the performance of high energy radiography devices.

X-ray computed tomography devices and X-ray diffraction techniques are powerful tools: the former provide volumetric data of samples during a non-destructive examination for biology and material science, and the latter measure grain orientation and strain, as well as crystalline phase identification and structure refinement. Today, the European Synchrotron Radiation Facility (ESRF) provides increasingly higher energy beams, up to 150 keV combined with higher brilliance (1013 X-ray photons/sec). This means that detectors suffer from low X-ray absorption at high spatial resolution (1-10 μm) and from radiation damage in tomography and diffraction applications. In addition, more and more experiments in medicine require the absorbed dose by the sample to be reduced. In this context, more efficient scintillators are developed and evaluated at the ESRF. In order to perform sub-micrometer and micrometer resolution imaging scintillators 1 μm to 500 μm thin are required. Single Crystal Film scintillators (SCF), 1 μm to 100 μm can be obtained via Liquid Phase Epitaxy for sub-micrometer resolution. Transparent ceramics, 100 μm to 500 μm thick are promising candidates for X-ray imaging requiring high X-ray absorption and good contrast with micrometer resolution. Commonly available scintillators, such as CdWO4 and YAG:Ce suffer from low efficiency, therefore new scintillators with higher light yield and stopping-power are required. A first test was carried out to evaluate an Europium doped Lutetium Oxide ceramic for micrometer resolution and new SCFs of Lu3Ga5-xInxO12:Eu for sub-micrometer resolution are investigated. Performance of Lu2O3 and LuInGG, i.e absorption, light yield, afterglow, spatial resolution will be presented and compared to standard screens (YAG, GGG). First results will be illustrated with X-ray images and will demonstrate the absorption efficiency improvement at high spatial resolution.

Detection of x-rays and gamma rays with high spatial resolution can be achieved with scintillators that are optically coupled to electron-multiplying charge-coupled devices (EMCCDs). These can be operated at typical frame rates of 50 Hz with low noise. In such a set-up, scintillation light within each frame is integrated after which the frame is analyzed for the presence of scintillation events. This method allows for the use of scintillator materials with relatively long decay times of a few milliseconds, not previously considered for use in photon-counting gamma cameras, opening up an unexplored range of dense scintillators. In this paper, we test CdWO₄ and transparent polycrystalline ceramics of Lu₂O₃:Eu and (Gd,Lu)₂O₃:Eu as alternatives to currently used CsI:Tl in order to improve the performance of EMCCD-based gamma cameras. The tested scintillators were selected for their significantly larger cross-sections at 140 keV ((99m)Tc) compared to CsI:Tl combined with moderate to good light yield. A performance comparison based on gamma camera spatial and energy resolution was done with all tested scintillators having equal (66%) interaction probability at 140 keV. CdWO₄, Lu₂O₃:Eu and (Gd,Lu)₂O₃:Eu all result in a significantly improved spatial resolution over CsI:Tl, albeit at the cost of reduced energy resolution. Lu₂O₃:Eu transparent ceramic gives the best spatial resolution: 65 µm full-width-at-half-maximum (FWHM) compared to 147 µm FWHM for CsI:Tl. In conclusion, these 'slow' dense scintillators open up new possibilities for improving the spatial resolution of EMCCD-based scintillation cameras.

Evolution of porosity and microstructure was observed during densification of lutetium oxide ceramics doped with europium (Lu2O3:Eu) fabricated via vacuum sintering and hot isostatic pressing (HIP’ing). Nano-scale starting powder was uniaxially pressed and sintered under high vacuum at temperatures between 1575 and 1850 °C to obtain densities ranging between 94% and 99%, respectively. Sintered compacts were then subjected to 200 MPa argon gas at 1850 °C to reach full density. Vacuum sintering above 1650 °C led to rapid grain growth prior to densification, rendering the pores immobile. Sintering between 1600 and 1650 °C resulted in closed porosity yet a fine grain size to allow the pores to remain mobile during the subsequent HIP’ing step, resulting in a fully-dense highly transparent ceramic without the need for subsequent air anneal. Light yield performance was measured and Lu2O3:Eu showed ∼4 times higher light yield than commercially used scintillating glass indicating that this material has the potential to improve the performance of high energy radiography devices.

Transparent ceramic fabrication can offer a route to functionally structured solid-state laser gain media. We report here on high transparency, fully-dense transparent optical ceramics with compositional gradients, fabricated by direct ink write (DIW) methods.

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.

We are developing new scintillator materials that offer potential for high resolution gamma ray spectroscopy at low cost. Single crystal SrI 2 (Eu) offers ∼3% resolution at 662 keV, in sizes of ∼1 in3. We have developed ceramics processing technology allowing us to achieve cubic inch scale transparent ceramic scintillators offering gamma spectroscopy performance superior to NaI(Tl). Our bismuth-loaded plastic scintillator demonstrates energy resolution of ∼8% at 662 keV, for samples of ∼0.5 cm3.

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

Transparent ceramic scintillators with the composition Gd0.3Lu1.6Eu0.1O3 (GLO:Eu) have been prepared by different sintering profiles: a traditional profile consisting of a slow ramp followed by a dwell, and a two-step profile consisting of a fast ramp and short dwell followed by a long dwell at a lower temperature. A subsequent Hot Isostatic Press (HIP) step was used to achieve full density and transparency. Two-step sintering allowed full transparency to be achieved after HIPing at 1525°C, while traditionally sintered samples required 1850°C in the HIP to achieve high transparency indicating that two-step sintering is successful in maintaining a small grain size and therefore allowing densification to be decoupled from grain growth during the low temperature HIP step. HIPing at elevated temperatures between 1525 and 1850°C resulted in rapid grain growth from sub-micron to ~300 µm grains. Radioluminescence spectra show negligible difference between samples with sub-micron grain size and those with 300 µm grains.