Peter A. Thelin

Development of Transparent Ceramic Ce-Doped Gadolinium Garnet Gamma Spectrometers

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.

Instrument Development and Gamma Spectroscopy With Strontium Iodide

Development of the Europium-doped Strontium Iodide scintillator, SrI2(Eu), involves advances in crystal growth, optics and readout methodology for prototype detectors. We have demonstrated energy resolution of 3% at 662 keV for a 26 cm3 SrI2(Eu) crystal, which is equivalent to the performance obtained with Cerium-doped Lanthanum Bromide of equivalent size. Compared to standard analog readout, use of a digital readout method allows improved energy resolution to be obtained with large volume SrI2(Eu) crystals. Comparative gamma spectra acquired with LaBr3(Ce) and NaI(Tl) quantitatively depict the value of the high resolution of SrI2(Eu) in discriminating closely spaced gamma lines for radioisotope identification applications.

Bismuth-loaded plastic scintillators for gamma spectroscopy and neutron active interrogation

Bismuth-loaded plastic scintillators capable of gamma spectroscopy are being scaled up to multiple cubic inch sizes. High light yields of >38,888 Ph/MeV are obtained with Iridium-complex fluors due to efficient harvesting of both singlet and triplet excitons, providing energy resolution of ~10% at 662 keV for 3 in3 scintillators. Although singlet fluors provide a poorer light yield of ~12,888 Ph/MeV and resolution at 662 keV of 14% in the Bismuth-loaded plastics, the fast decay time of <;100 ns and the low neutron capture cross-sections of the constituent elements lend themselves to applications in neutron active interrogation. Measurements of the scintillation light yield non-proportionality reveal that exciton-exciton annihilation is suppressed in Iridium-complex activated plastic, in contrast with the singlet fluor activated plastic.

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.