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DOE OSTI2011

Recent Developments in Fast Neutron Detection and Multiplicity Counting with Liquid Scintillator

For many years, LLNL researchers have been developing time-correlated neutron detection techniques and algorithms for applications such as Arms Control, Threat Detection and Nuclear Material Assay. Many of the techniques have been developed specifically for the relatively low efficiency (a few percent) attainable by detector systems limited to man-portability. Historically, thermal neutron detectors (mainly {sup 3}He) were used, taking advantage of the high thermal neutron interaction cross sections. More recently, we have been investigating the use of fast neutron detection with liquid scintillators, inorganic crystals, and in the near future, pulse-shape discriminating plastics that respond over 1000 times faster (ns versus tens of {mu}s) than thermal neutron detectors. Fast neutron detection offers considerable advantages since the inherent ns production timescales of spontaneous fission and neutron-induced fission are preserved and measured instead of being lost by thermalization required for thermal neutron detectors. We are now applying fast neutron technology to the safeguards regime in the form of fast portable digital electronics as well as faster and less hazardous scintillator formulations. Faster detector response times and sensitivity to neutron momentum show promise for measuring, differentiating, and assaying samples that have modest to very high count rates, as well as mixed fission sources like Cm and Pu. We report on measured results with our existing liquid scintillator array and progress on the design of a nuclear material assay system that incorporates fast neutron detection, including the surprising result that fast liquid scintillator detectors become competitive and even surpass the precision of {sup 3}He-based counters measuring correlated pairs in modest (kg) samples of plutonium.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2013

Compensational scintillation detector with a flat energy response for flash X-ray measurements

To measure the intensity of flash X-ray sources directly, a novel scintillation detector with a fast time response and flat energy response is developed by combining film scintillators of doped ZnO crystal and fast organic scintillator together. Through compensation design, the dual-scintillator detector (DSD) achieved a flat energy response to X-rays from tens of keV to several MeV, and sub-nanosecond time response by coupling to ultrafast photo-electronic devices. A prototype detector was fabricated according to the theoretical design; it employed ZnO:In and EJ228 with thicknesses of 0.3 mm and 0.1 mm, respectively. The energy response of this detector was tested on monoenergetic X-ray and {gamma}-ray sources. The detector performs very well with a sensitivity fluctuation below 5% for 8 discrete energy points within the 40-250 keV energy region and for other energies of 662 keV and 1.25 MeV as well, showing good accordance with the theoretical design. Additionally, the detector works properly for the application to the flash X-ray radiation field absolute intensity measurement. This DSD may be very useful for the diagnosis of time-resolved dynamic physical processes of flash X-ray sources without knowing the exact energy spectrum.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2013

Plasmonic light yield enhancement of a liquid scintillator

We demonstrate modifications to the light yield properties of an organic liquid scintillator due to the localization of the tertiary fluorophore component to the surface of Ag-core silica-shell nanoparticles. We attribute this enhancement to the near-field interaction of Ag nanoparticle plasmons with these fluor molecules. The scintillation light yield enhancement is shown to be equal to the fluorescence enhancement within measurement uncertainties. With a suitable choice of plasmon energy and scintillation fluor, this effect may be used to engineer scintillators with enhanced light yields for radiation detection applications.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2013

Energy resolution and related charge carrier mobility in LaBr{sub 3}:Ce scintillators

The scintillation response of LaBr{sub 3}:Ce scintillation crystals was studied as function of temperature and Ce concentration with synchrotron X-rays between 9 keV and 100 keV. The results were analyzed using the theory of carrier transport in wide band gap semiconductors to gain new insights into charge carrier generation, diffusion, and capture mechanisms. Their influence on the efficiency of energy transfer and conversion from X-ray or γ-ray photon to optical photons and therefore on the energy resolution of lanthanum halide scintillators was studied. From this, we will propose that scattering of carriers by both the lattice phonons and by ionized impurities are key processes determining the temperature dependence of carrier mobility and ultimately the scintillation efficiency and energy resolution. When assuming about 100 ppm ionized impurity concentration in 0.2% Ce{sup 3+} doped LaBr{sub 3,} mobilities are such that we can reproduce the observed temperature dependence of the energy resolution, and in particular, the minimum in resolution near room temperature is reproduced.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Signal pulse emulation for scintillation detectors using Geant4 Monte Carlo with light tracking simulation

The anode pulse of a photomultiplier tube (PMT) coupled with a scintillator is used for pulse shape discrimination (PSD) analysis. We have developed a novel emulation technique for the PMT anode pulse based on optical photon transport and a PMT response function. The photon transport was calculated using Geant4 Monte Carlo code and the response function with a BC408 organic scintillator. The obtained percentage RMS value of the difference between the measured and simulated pulse with suitable scintillation properties using GSO:Ce (0.4, 1.0, 1.5 mol%), LaBr{sub 3}:Ce and BGO scintillators were 2.41%, 2.58%, 2.16%, 2.01%, and 3.32%, respectively. The proposed technique demonstrates high reproducibility of the measured pulse and can be applied to simulation studies of various radiation measurements.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2018

Brightness and uniformity measurements of plastic scintillator tiles at the CERN H2 test beam

Here, we study the light output, light collection efficiency and signal timing of a variety of organic scintillators that are being considered for the upgrade of the hadronic calorimeter of the CMS detector. The experimental data are collected at the H2 test-beam area at CERN, using a 150 GeV muon beam. In particular, we investigate the usage of over-doped and green-emitting plastic scintillators, two solutions that have not been extensively considered. We present a study of the energy distribution in plastic-scintillator tiles, the hit efficiency as a function of the hit position, and a study of the signal timing for blue and green scintillators.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2011

Positronium signature in organic liquid scintillators for neutrino experiments

Electron antineutrinos are commonly detected in liquid scintillator experiments via inverse {beta} decay by looking at the coincidence between the reaction products: neutrons and positrons. Prior to positron annihilation, an electron-positron pair may form an orthopositronium (o-Ps) state, with a mean lifetime of a few nanoseconds. Even if the o-Ps decay is speeded up by spin-flip or pick-off effects, it may introduce distortions in the photon emission time distribution, crucial for position reconstruction and pulse shape discrimination algorithms in antineutrino experiments. Reversing the problem, the o-Ps-induced time distortion represents a new signature for tagging antineutrinos in liquid scintillator. In this article, we report the results of measurements of the o-Ps formation probability and lifetime for the most used solvents for organic liquid scintillators in neutrino physics (pseudocumene, linear alkyl benzene, phenylxylylethane, and dodecane). We characterize also a mixture of pseudocumene +1.5 g/l of 2,5-diphenyloxazole, a fluor acting as wavelength shifter. In the second part of the article, we demonstrate that the o-Ps-induced distortion of the scintillation photon emission time distributions represent an optimal signature for tagging positrons on an event by event basis, potentially enhancing the antineutrino detection.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2015

Compensated gadolinium-loaded plastic scintillators for thermal neutron detection (and counting)

Plastic scintillator loading with gadolinium-rich organometallic complexes shows a high potential for the deployment of efficient and cost-effective neutron detectors. Due to the low-energy photon and electron signature of thermal neutron capture by gadolinium-155 and gadolinium-157, alternative treatment to Pulse Shape Discrimination has to be proposed in order to display a trustable count rate. This paper discloses the principle of a compensation method applied to a two-scintillator system: a detection scintillator interacts with photon radiation and is loaded with gadolinium organometallic compound to become a thermal neutron absorber, while a non-gadolinium loaded compensation scintillator solely interacts with the photon part of the incident radiation. Posterior to the nonlinear smoothing of the counting signals, a hypothesis test determines whether the resulting count rate after photon response compensation falls into statistical fluctuations or provides a robust image of a neutron activity. A laboratory prototype is tested under both photon and neutron irradiations, allowing us to investigate the performance of the overall compensation system in terms of neutron detection, especially with regards to a commercial helium-3 counter. The study reveals satisfactory results in terms of sensitivity and orientates future investigation toward promising axes. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2018

Correlation of Non-proportionality and Scintillation Properties with Cerium Concentration in YAlO 3 :Ce

Cerium doped YAlO3 (YAP:Ce) is an interesting oxide scintillator in that it exhibits a wider range of light yield non-proportionality on a sample-to-sample basis than most other well-known oxide scintillators. In general, most oxide materials, such as BGO and LSO:Ce, are thought to have an intrinsic proportional response that is nearly constant between samples and independent of growth conditions. Since light yield nonproportionality is responsible for degrading the achievable energy resolution of all known scintillators, it is important to understand what contributes to the behavior. In this study, in an attempt to understand if the phenomenon can be affected by growth parameters or by other means, seven samples of YAP:Ce were collected from various sources, and eight samples were grown inhouse using the Czochralski method. Based on optical and scintillation measurement as well as direct measurement of the cerium concentration, it was determined that the light yield proportionality in YAlO3:Ce is strongly related to the cerium concentration. In this work, samples that were found to have a higher relative cerium concentration displayed a more proportional light yield response. In addition, it was determined that samples with a higher cerium concentration also exhibit a faster decay time and an enhanced energy resolution when compared to samples with less cerium. Finally, it was also determined that growth in a reducing atmosphere can effectively suppress a parasitic optical absorption band.

36 MATERIALS SCIENCE↗

DOE OSTI2013

Studies on Ca2+-Doped CeBr3 Scintillating Materials

Despite the outstanding scintillation performance characteristics of cerium tribromide (CeBr3) and cerium-activated lanthanum tribromide (LaBr3:Ce), their commercial availability and application is limited due to the difficulties of growing large, crack-free single crystals from these fragile materials. The objective of this investigation was to employ aliovalent doping to increase crystal strength while maintaining the optical properties of the crystal. One divalent dopant (Ca2+) was investigated as a dopant to strengthen CeBr3 without negatively impacting scintillation performance. Ingots containing nominal concentrations of 1.9% of the Ca2+ dopant were grown. Preliminary scintillation measurements are presented for this aliovalently doped scintillator. Ca2+-doped CeBr3 exhibited little or no change in the peak fluorescence emission for 371 nm optical excitation for CeBr3. The structural, electronic, and optical properties of CeBr3 crystals were investigated using the density functional theory within generalized gradient approximation. The calculated lattice parameters are in good agreement with the experimental data. The energy band structures and density of states were obtained. The optical properties of CeBr3, including the dielectric function, were calculated.

aliovalent substitution↗

DOE OSTI2010

Monte Carlo study of the energy and angular dependence of the response of plastic scintillation detectors in photon beams

Purpose: By using Monte Carlo simulations, the authors investigated the energy and angular dependence of the response of plastic scintillation detectors (PSDs) in photon beams. Methods: Three PSDs were modeled in this study: A plastic scintillator (BC-400) and a scintillating fiber (BCF-12), both attached by a plastic-core optical fiber stem, and a plastic scintillator (BC-400) attached by an air-core optical fiber stem with a silica tube coated with silver. The authors then calculated, with low statistical uncertainty, the energy and angular dependences of the PSDs' responses in a water phantom. For energy dependence, the response of the detectors is calculated as the detector dose per unit water dose. The perturbation caused by the optical fiber stem connected to the PSD to guide the optical light to a photodetector was studied in simulations using different optical fiber materials. Results: For the energy dependence of the PSDs in photon beams, the PSDs with plastic-core fiber have excellent energy independence within about 0.5% at photon energies ranging from 300 keV (monoenergetic) to 18 MV (linac beam). The PSD with an air-core optical fiber with a silica tube also has good energy independence within 1% in the same photon energy range. For the angular dependence, the relative response of all the three modeled PSDs is within 2% for all the angles in a 6 MV photon beam. This is also true in a 300 keV monoenergetic photon beam for PSDs with plastic-core fiber. For the PSD with an air-core fiber with a silica tube in the 300 keV beam, the relative response varies within 1% for most of the angles, except in the case when the fiber stem is pointing right to the radiation source in which case the PSD may over-response by more than 10%. Conclusions: At {+-}1% level, no beam energy correction is necessary for the response of all three PSDs modeled in this study in the photon energy ranges from 200 keV (monoenergetic) to 18 MV (linac beam). The PSD would be even closer to water equivalent if there is a silica tube around the sensitive volume. The angular dependence of the response of the three PSDs in a 6 MV photon beam is not of concern at 2% level.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2015

The design of the TASD (totally active scintillator detector) prototype

Totally active and magnetic segmented scintillation neutrino detectors are developed for the nextgeneration accelerator neutrino experiments. Such detectors will incorporate scintillation modules with scintillation counters that form X and Y planes. A single counter is a 7 × 10 × 90 mm{sup 3} scintillation bar with gluedin wavelength-shifting fibers and micropixel avalanche photodiodes. The results of measurements of the parameters of these detectors are presented.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2012

Characteristics of Un doped and Europium-dopedSrI2 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 SrI{sub 2}(Eu) scintillator detectors, which routinely provide <;3.0% energy resolution at 662 keV with volumes >;10 cm{sup 3}. In this study, we have tested pure, undoped SrI{sub 2} to gain a better understanding of the scintillation properties and spectroscopic performance achievable without activation. An undoped crystal grown from 99.999% pure SrI{sub 2} 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 SrI{sub 2} 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 SrI{sub 2} 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 SrI{sub 2} 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.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2013

Studies on Ca2+-Doped CeBr3 Scintillating Materials

aliovalent substitution↗

DOE OSTI2022

Scintillation Hydro-Gel for Isotopic Neutron (SHINE): Eco-Friendly Quantum Dot Neutron Detectors

The development of new neutron detectors to replace helium-3 (3He) detectors is imperative due to a worldwide shortage of 3He following the draw down in nuclear weapons production since the end of the Cold War. The United States Department of Homeland Security would like to deploy monitors for the detection of neutron emissions from shipping containers housing illicit nuclear material; however, this effort has been put on hold until new replacements for 3He detectors can be developed. Scintillation Hydro-Gel for isotopic Neutron Emitters (SHINE) is a unique, first of its kind, 6Li-loaded quantum dot gel scintillator developed at INL. By incorporating 6Li with quantum dots in a gel matrix, SHINE displays the best properties of liquid and solid scintillators without their disadvantages such as continuous filtering to keep liquids free of contaminates, slow throughput of containers, higher base component costs, ‘dead’ voids in solid scintillators, and a high loading of 6Li without compromising on light transparency. Additionally, SHINE is completely eco-friendly, a breakthrough in high-efficiency detection systems. SHINE is a unique combination of 6LiCl, a highly water-soluble compound, and InP/ZnS core/shell quantum dots, which are poured into a gel-form using cross-linking polymers. In this presentation, SHINE has been successfully tested for neutron detection and shows promise as both a replacement for current 3He neutron detectors as well as potential use in handheld, compact neutron detection units and antineutrino detection.

36 MATERIALS SCIENCE↗

DOE OSTI2012

Organic scintillation detector response simulation using non-analog MCNPX-PoliMi

Organic liquid scintillation detectors are valuable for the detection of special nuclear material since they are capable of detecting both neutrons and gamma rays. Scintillators can also provide energy information which is helpful in identification and characterization of the source. In order to design scintillation based measurement systems appropriate simulation tools are needed. MCNPX-PoliMi is capable of simulating scintillation detector response; however, simulations have traditionally been run in analog mode which leads to long computation times. In this paper, non-analog MCNPX-PoliMi mode which uses variance reduction techniques is applied and tested. The non-analog MCNPX-PoliMi simulation test cases use source biasing, geometry splitting and a combination of both variance reduction techniques to efficiently simulate pulse height distribution and then time-of-flight for a heavily shielded case with a {sup 252}Cf source. An improvement factor (I), is calculated for distributions in each of the three cases above to analyze the effectiveness of the non-analog MCNPX-PoliMi simulations in reducing computation time. It is found that of the three cases, the last case which uses a combination of source biasing and geometry splitting shows the most improvement in simulation run time for the same desired variance. For pulse height distributions speedup ranging from a factor 5 to 25 is observed, while for time-of-flights the speedup factors range from 3 to 10. (authors)

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2015

Study of influence of plastic scintillators thicknesses to detect Beta particles and Gamma radiation by means of spectral analysis of {sup 90}Sr, {sup 90}Y and {sup 137}Cs sources

The Nuclear and Energy Research Institute - IPEN, offers post-graduate programs, namely: Nuclear Technology - Applications (TNA), Nuclear Technology - Materials (TNM), Nuclear Technology - Reactors (TNR). The Institute programs mission is to form expert technicians, physicists and engineers with a strong knowledge in their discipline to work in the nuclear area. The course: 'Theoretical Fundamentals and Practices of the Instrumentation used in Nuclear Data Acquisition' covers the use of laboratory nuclear instrumentation and the accomplishment of experiments to obtain nuclear parameters. One of these experimental exercises is object of this work: 'Study of influence of plastic scintillators to detect Beta particles and Gamma radiation by means of spectral analysis of {sup 90}Sr, {sup 90}Y and {sup 137}Cs sources'. The use of scintillators plastic for the detection has the advantage of low cost, high mechanical strength, is not hygroscopic and can be manufactured in large volumes. This work aims to present the analysis of relative efficiency of detection of plastic scintillators of various thicknesses for beta particles and gamma radiation by the spectrum of {sup 137}Cs and {sup 90}Sr. Due to lack of resolution of the detectors plastic scintillators we worked with relative efficiency. The evaluation was done by reading deposited energy, using the software MAESTRO, for each detector thickness. For beta particles was observed an ideal thickness around 3 mm and the better photon efficiency was observed with increasing the thickness of the detector. The present experiment does not intend to establish a new technique for this subject: it solely aims student's practical exercises in nuclear properties of elements and detectors being part of the nuclear experimental course. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Czochralski Growth and Characterization of a Compositionally Complex Rare Earth Aluminum Garnet Scintillator: (Gd 1/4 Y 1/4 Tb 1/4 Lu 1/4 ) 3 Al 5 O 12 :Ce

Compositionally complex oxides have garnered increasing interest for their enhanced phase stability and tunable functional properties, yet their development as bulk single crystal scintillators remains limited. Herein, we report the Czochralski growth and characterization of (Gd 1/4 Y 1/4 Tb 1/4 Lu 1/4 ) 3 Al 5 O 12 :Ce (GYTLAG), a compositionally complex garnet incorporating four dodecahedrally coordinated principal rare earth elements. The garnet phase was confirmed by powder and single crystal X-ray diffraction, and macroscopic defects are described. X-ray absorption near-edge structure measurements confirm the 3+ oxidation state of all rare earths and support their occupation of the same crystallographic site; white line intensity variations correlate with the anticipated segregation behavior. Elemental segregation is quantified by SEM/EDS and ICP-OES, and a linear trend was established between the segregation coefficient and the difference between each rare earth’s ionic radius (r) and the average ionic radius (AIR) of the dodecahedral site. This trend offers a predictive framework for compositional control in future REAG crystals grown by the Czochralski method. Photoluminescence and radioluminescence measurements reveal both Ce 3+ and Tb 3+ emission. Scintillation pulses exhibit four-component decay with dominant ~230 µs and ~1.2 ms components, and the light yield is estimated to be up to 43,000 ph/MeV under 137Cs γ-ray excitation. GYTLAG also demonstrates a strong radioluminescence efficiency and 50% lower afterglow at 20 ms compared to a LuAG:Ce reference, underscoring its promise for scintillator applications.

Compositionally complex oxide, high entropy oxide,↗