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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.

Thallium bromide (TlBr) is a compound semiconductor with a band gap of 2.68 eV making it ideal for room temperature radiation detection. The high atomic numbers, 81 and 35, and the high density of 7.56 g/cm3 give it excellent gamma-ray stopping power. TlBr is a cubic material that melts congruently at a relatively low temperature (~ 480 C). These properties make it relatively easy to grow good quality crystals with high yield. As a result of improvements in the purification of TlBr mobility-lifetime product of electrons, µτe, is now on the order of 10-2 cm2/V, which is similar to that of CZT. High µτe enables the fabrication of thicker detectors with good charge collection and energy resolution. The properties of TlBr make it ideal for use in room temperature gamma radiation operation [Smith 2013]. Single carrier devices such as small pixel arrays [O'Neal 2018a] and Frisch collar devices [Hitomi, et al.2013] which were developed for CZT can also been applied to TlBr. For example, better than 1% FWHM at 662 keV has been obtained for single pixel events with small (e.g. 3 x 3 pixels, 1-mm pitch, 5-mm thick) arrays.

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.

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

We have previously made improvements to the longevity of TlBr semiconductor gamma ray detectors by applying electrodes having the mixed semiconductor composition Tl(Cl,Br) via surface treatments in HCl, leading to a significant enhancement to the lifetime of the detectors. In order to examine the electron transport properties more closely, we have monitored the first-derivative of the cathode waveform (being proportional to velocity and number of carriers) as a function of time and the point of the gamma-interaction. The observed decay in this signal, especially at lower voltage, would naturally be interpreted as the usual trapping phenomenon. However, this phenomenon alone is not able to account for the observed waveforms, most dramatically for the case of increasing signal as the electrons approach the anode, for waveforms originating at the cathode. After detailed consideration of alternative explanations, the cathode waveform data has been interpreted in terms of a non-uniform field owing to variation in the resistivity as a function of position. We have interpreted the shape of the decay as a “built-in” resistivity profile and have further verified this interpretation by reversing the sense of the field (which as expected reverses the “sense” of the waveform). We modeled this effect in order to quantitatively deduce the resistivity profile and are currently working to relate the waveform observations to the relative orientation of the crystal growth direction and the applied electrodes.

Plastic scintillators incorporating 8 weight percent elemental Bismuth offer enhanced sensitivity and distinct photopeak spectra in the 3 Bismuth plastic scintillator plate. Count rates compared to standard plastic scintillator of the same size reveal a sensitivity improvement of >5x in the

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.

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

Due to its wide band gap (2.68 eV) and high stopping power, thallium bromide (TlBr) is being investigated as a room-temperature semiconductor gamma-ray spectrometer. When cooled to −20°C, performance of better than 1% FWHM at 662 keV has been observed on 5×5×5 mm3 pixelated TlBr detectors. The room-temperature lifetime (under continuous bias) of thick TlBr detectors operated at high fields (∼2000 V/cm) has been limited to weeks or months due to polarization caused by ionic conduction. Previous work has shown that the degradation process is limited to the surface and that surface preparation techniques can extend the lifetime of thin planar TlBr devices at room temperature. In this work, the lifetime and stability of two large 5×5×5 mm3 pixelated TlBr arrays are presented. Detector performance is compared for different surface preparation techniques and improved stability is observed. Additionally, we use depth-sensing techniques to track the depth-dependent photopeak centroids over time and conclude that once surface degradation effects are mitigated, TlBr performance can improve over time at room temperature. The improvement is likely similar to conditioning at −20°C in which the electric field stabilizes and becomes more uniform.

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.

Degradation of room temperature operation of TlBr radiation detectors with time 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. Scanning Auger electron spectroscopy (AES) in combination with sputter depth profiling 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 and create a TlBr1-xClx surface layer prior to metal contact deposition. Auger compositional depth profiling results reveal non-equilibrium interfacial diffusion after device operation in both air and N2 at ambient temperature. These results improve our understanding of contact/device degradation versus operating environment for further enhancing radiation detector performance.

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.