Scott E. Fisher

Transparent ceramic scintillators for gamma spectroscopy and radiography

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 <0.1 cm-1. We have fabricated Cerium-doped Gadolinium Garnets with light yields of ~50,000 Ph/MeV and energy resolution of <5% at 662 keV. We have also developed methods to form sheets of the high-Z ceramic scintillator, Europium-doped Lutetium Oxide Bixbyite, producing ~75,000 Ph/MeV for radiographic imaging applications.

Comparative gamma spectroscopy with SrI 2 (Eu), GYGAG(Ce) and Bi-loaded plastic scintillators

We are developing new scintillator materials that offer potential for high resolution gamma ray spectroscopy at low cost. Single crystal SrI<inf>2</inf>(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.

High energy resolution with transparent ceramic garnet scintillators

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.

Ce-doped single crystal and ceramic garnet for γ-ray detection

Ceramic and single crystal Lutetium Aluminum Garnet scintillators exhibit energy resolution with bialkali photomultiplier tube detection as good as 8.6% at 662 keV. Ceramic fabrication allows production of garnets that cannot easily be grown as single crystals, such as Gadolinium Aluminum Garnet and Terbium Aluminum Garnet. Measured scintillation light yields of Cerium-doped ceramic garnets indicate prospects for high energy resolution.

Characteristics of undoped and europium-doped SrI 2 scintillator detectors

High energy resolution gamma-ray detectors that can be formed into relatively large sizes while operating at room temperature offer many advantages for national security applications. We are working toward that goal through the development of SrI2(Eu) scintillator detectors, which routinely provide &#60;3.0% energy resolution at 662 keV with volumes >10 cm3. In this study, we have tested pure, undoped SrI2 to gain a better understanding of the scintillation properties and spectroscopic performance achievable without activation. An undoped crystal grown from 99.999% pure SrI2 pellets was tested for its spectroscopic performance, its light yield, and uniformity of scintillation light collection as a function of gamma-ray interaction position relative to the crystal growth direction. Undoped SrI2 was found to provide energy resolution of 5.3% at 662 keV, and the light collection nonuniformity varied by only 0.72% over the length of the crystal. Measurements of both a 3% Eu-doped and the undoped SrI2 crystal were carried out in the SLYNCI facility and indicate differences in their light yield non-proportionality. The surprisingly good scintillation properties of the pure SrI2 crystal suggests that with high-purity feedstock, further reduction of the Eu concentration can be made to grow larger crystals while not adversely impacting the spectroscopic performance.

Transparent ceramic scintillators for gamma spectroscopy and MeV imaging

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 <100 ns, and light yield of 50,000 Ph/MeV. Gdgarnet ceramic scintillators offer the best energy resolution of any oxide scintillator, as good as R(662 keV) = 3% (Si-PD readout) for small sizes and typically R(662 keV) < 5% for cubic inch sizes. For radiography, the bixbyite transparent ceramic scintillator, (Gd,Lu,Eu)2O3, or “GLO,” offers excellent x-ray stopping, with ρ = 9.1 g/cm3 and Zeff = 68. Several 10” diameter by 0.1” thickness GLO scintillators have been fabricated. GLO outperforms scintillator glass for high energy radiography, due to higher light yield (55,000 Ph/MeV) and better stopping, while providing spatial resolution of >8 lp/mm.

Strontium Iodide Instrument Development for Gamma Spectroscopy and Radioisotope Identification

Development of the Europium-doped Strontium Iodide scintillator, SrI2(Eu2+), has progressed significantly in recent years. SrI2(Eu2+) has excellent material properties for gamma ray spectroscopy: high light yield (<80,000 ph/MeV), excellent light yield proportionality, and high effective atomic number (Z = 49) for high photoelectric cross-section. High quality 1.5” and 2” diameter boules are now available due to rapid advances in SrI2(Eu) crystal growth. In these large SrI2(Eu) crystals, optical self-absorption by Eu2+ degrades the energy resolution as measured by analog electronics, but we mitigate this effect through on-the-fly correction of the scintillation pulses by digital readout electronics. Using this digital correction technique we have demonstrated energy resolution of 2.9% FWHM at 662 keV for a 4 in3 SrI2(Eu) crystal, over 2.6 inches long. Based on this digital readout technology, we have developed a detector prototype with greatly improved radioisotope identification capability compared to Sodium Iodide, NaI(Tl). The higher resolution of SrI2(Eu) yields a factor of 2 to 5 improvement in radioisotope identification (RIID) error rate compared to NaI(Tl).

History and current status of strontium iodide scintillators

Eu-doped strontium iodide single crystal growth has reached maturity and prototype SrI2(Eu)-based gamma ray spectrometers provide detection performance advantages over standard detectors. SrI2(Eu) offers a high, proportional light yield of >80,000 photons/MeV. Energy resolution of <3% at 662 keV with 1.5” x 1.5” SrI2(Eu) crystals is routinely achieved, by employing either a small taper at the top of the crystal or a digital readout technique. These methods overcome light-trapping, in which scintillation light is re-absorbed and re-emitted in Eu2+-doped crystals. Its excellent energy resolution, lack of intrinsic radioactivity or toxicity, and commercial availability make SrI2(Eu) the ideal scintillator for use in handheld radioisotope identification devices. A 6-lb SrI2(Eu) radioisotope identifier is described.

Recent advances in garnet scintillator gamma spectrometers (Conference Presentation)

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.