Erik L. Swanberg

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.

Nonproportionality of Scintillator Detectors. III. Temperature Dependence Studies

This paper is the third in a series of articles on the basic physics of nonproportionality in scintillators. Here, we focus on the temperature dependence of six scintillators, NaI(Tl), CsI(Tl), CsI(Na), CeBr₃, LaBr₃(Ce), and undoped SrI₂, and report their nonproportionality curves at -40^°C, 0^°C and + 40^°C. We fit the data to a modified form of our previously employed model, including the competition of carrier trapping with the Onsager-mediated attraction between electrons and holes.

Nonproportionality of Scintillator Detectors. V. Comparing the Gamma and Electron Response

This paper is the fifth in a series of articles on the basic physics of light yield nonproportionality in scintillators. Here, we compare and contrast the nonproportionality as registered by gamma rays and high-energy electrons. As has been noted in the past, these two types of data have different curve shapes (for plots of the light yield against electron or gamma energy). Herein, we show how the experimental gamma nonproportionality curve can be calculated from the electron response by accounting for the distribution of high energy electrons created by the gamma photon via the photoelectric interaction. Similarly, we measure and model the gamma-induced resolution as a function of energy and compare this data to predictions from our model. The utility of the model is explored using data acquired with the scintillators SrI2(Eu), GYGAG(Ce) and CsI(Na).

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.

Oxidation/reduction reactions at the metal contact-TlBr interface: an x-ray photoelectron spectroscopy study

TlBr radiation detector operation degrades with time at room temperature and is thought to be due to electromigration of Tl and Br vacancies within the crystal as well as the metal contacts migrating into the TlBr crystal itself due to electrochemical reactions at the metal/TlBr interface. X-ray photoemission spectroscopy (XPS) was used to investigate the metal contact surface/interfacial structure on TlBr devices. Device-grade TlBr was polished and subjected to a 32% HCl etch to remove surface damage prior to Mo or Pt contact deposition. High-resolution photoemission measurements on the Tl 4f, Br 3d, Cl 2p, Mo 3d and Pt 4f core lines were used to evaluate surface chemistry and non-equilibrium interfacial diffusion. Results indicate that anion substitution at the TlBr surface due to the HCl etch forms TlBr1-xClx with consequent formation of a shallow heterojunction. In addition, a reduction of Tl1+ to Tl0 is observed at the metal contacts after device operation in both air and N2 at ambient temperature. Understanding contact/device degradation versus operating environment is useful for improving radiation detector performance.

Bismuth-loaded plastic scintillator portal monitors

Plastic scintillators incorporating 8 weight percent elemental Bismuth offer enhanced sensitivity and distinct photopeak spectra in the <1000 keV range typically used in radiation portal monitors. The Bismuth-loaded plastic is based on polyvinyl toluene with standard singlet fluors. It produces ~6,000 photons/MeV with a maximum emission at 430 nm and a ~10 ns decay. Energy resolution of 49% at 59.5 keV and 16% at 662 keV are obtained for a 14 in3 Bismuth plastic scintillator plate. Count rates compared to standard plastic scintillator of the same size reveal a sensitivity improvement of >5x in the <200 keV range. Future spectroscopic radiation portal monitors based on the Bismuth plastic scintillator could provide moderate resolution spectroscopy for radioisotope identification. In addition, the Bismuth plastic offers outstanding environmental stability to weathering effects, in contrast with standard plastic scintillator formulations.

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.

Transparent ceramic garnet scintillator optimization via composition and co-doping for high-energy resolution gamma spectrometers(Conference Presentation)

Breakthrough energy resolution, R(662keV) <4%, has been achieved with an oxide scintillator, Cerium-doped Gadolinium Yttrium Gallium Aluminum Garnet, or GYGAG(Ce), by optimizing fabrication conditions. Here we describe the dependence of scintillation light yield and energy resolution on several variables: (1) Stoichiometry, in particular Gd/Y and Ga/Al ratios which modify the bandgap energy, (2) Processing methods, including vacuum vs. oxygen sintering, and (3) Trace co-dopants that influence the formation of Ce4+ and modify the intra-bandgap trap distribution. To learn about how chemical composition influences the scintillation properties of transparent ceramic garnet scintillators, we have measured: scintillation decay component 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. Optimized GYGAG(Ce) provides R(662 keV) =3.0%, for 0.05 cm3 size ceramics with Silicon photodiode readout, and R(662 keV) =4.6%, at 2 in3 size with PMT readout.