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Distance Dependent Quenching and Gamma-Ray Spectroscopy in Tin-Loaded Polystyrene Scintillators

IEEE Transactions on Nuclear Science

Feng, Patrick L.; Mengesha, Wondwosen M.; Anstey, Mitchell A.; Cordaro, Joseph G.

In this work, we report the synthesis and inclusion of rationally designed organotin compounds in polystyrene matrices as a route towards plastic scintillators capable of gamma-ray spectroscopy. Tin loading ratios of up to 15% w/w have been incorporated, resulting in photopeak energy resolution values as low as 10.9% for 662 keV gamma-rays. Scintillator constituents were selected based upon a previously reported distance-dependent quenching mechanism. Data obtained using UV-Vis and photoluminescence measurements are consistent with this phenomenon and are correlated with the steric and electronic properties of the respective organotin complexes. We also report fast scintillation decay behavior that is comparable to the quenched scintillators 0.5% trans-stilbene doped bibenzyl and the commercial plastic scintillator BC-422Q-1%. These observations are discussed in the context of practical considerations such as optical transparency, ease-of-preparation/scale-up, and total scintillator cost.

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Plastic Scintillators Light Yield Energy Calibration

Mengesha, Wondwosen M.; Feng, Patrick L.; Cordaro, Joseph G.; Anstey, Mitchell A.; Myllenbeck, Nicholas M.; Throckmorton, Daniel J.

Currently we are investigating the inclusion of organotin compounds in polystyrene material to improve plastic scintillators full gamma-ray energy sensitivity with the ultimate goal of achieving spectroscopy. Accurate evaluation of light yield from the newly developed scintillators is crucial to assess merits of compounds and chemical process used in the scintillators development. Full gamma-ray energy peak in measured gammaray spectrum, resulting from total absorption of gamma-ray energy, would be ideal in evaluating the light yield from the new scintillators. However, full energy sensitivity achieved thus far is not statistically viable for fast and accurate light yield energy calibration from the new scintillators. The Compton edge in measured gamma-ray spectrum has been found as an alternate gamma-ray spectrum feature that can be exploited for characterizing the light yield energy from the newly developed plastic scintillators. In this study we present technique implemented for accurate light yield energy calibration using the Compton edge. Results obtained were very encouraging and promise the possibility of using the Compton edge for energy calibration in detectors with poor energy resolution such as plastic and liquid scintillators.

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Scintillating Cocktail Mixtures and the Role of Water on the Optophysical Properties

Cordaro, Joseph G.; Feng, Patrick L.; Mengesha, Wondwosen M.; Murtagh, Dustin M.; Anstey, Mitchell A.

Two types of water - containing liquid scintillation mixtures were prepared in the present work. In the first, m ixtures of 2 - phenylethanol, water, diphenyl phosphate, sodium phenyl phosphate dibasic dihydrate, and the dye 2,5 - diphenyloxazole (PPO) have been investigated as liquid scintillators. In the second system, nonionic and mixed surfactant systems were investigated in conjunction with water and small amounts of toluene. In both cases, increasing amounts of water led to reductions in the scintillation light yield. Understanding what factors contr ibute to this phenomenon is the focus of this report. Changes in the solution microphase structure, diminishing aromatic content of the cocktail mixtures, and inefficient energy transfer to the dye a ppear to be responsible for the decreased light yield as more water is added . In the 2 - phenylethanol system, the observed experimental results are consistent with the formation of a bicontinuous microemulsion at higher water concentrations, which incorporates PPO and shields it from the quenching effects of the increasing polar matrix. Evidence for this proposed phase change comes from light scattering data, photo - and x - ray luminescence measurements, and optical transparency measurements . In the surfactant - based system, the quenching effect of water was found to be less than both commercially - available dioxane - naphthalene mixtures used for scintillation counting as well as the 2 - phenylethanol mixtures described above. The effect of different surfactant mixtures and concentrations were studied, revealing a benefic ial effect upon the scintillation light yield for mixed surfactant mixtures. These results are interpreted in the context of reactive radical species formation following water ionization , which leads to light - yield quenching in aqueous systems . The presence of surfactant(s) in these mixtures enables the formation of organic - rich regions that are spatially separated from the reactive radicals. This hypothesis is consistent with subsequent experiments that showed reduced light - yield quenching in the presence of radical - trapping additives. A notable result from these surfactant studies was the preparation of an aqueous scintillator that was transparent and showed neutron/gamma pulse - shape discrimination. Section II below provides background information on the significance of this finding. The combined work described herein has implications on other efforts to make water - based solution scintillators -- without aromatic content an efficient mechanism for ionizing radiation to sensitize emission from a dye is limited.

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Synthesis of water-soluble mono- and ditopic imidazoliums for carbene ligands

Sandia journal manuscript; Not yet accepted for publication

Anstey, Mitchell A.; Cordaro, Joseph G.; Feng, Patrick L.; Murtagh, Dustin M.; Mengesha, Wondwosen M.; Stavila, Vitalie S.

Synthesis of ditopic imidazoliums was achieved using a modular step-wise procedure. The procedure itself is amenable to a wide array of functional groups that can be incorporated into the imidazolium architecture. The resulting compounds range from ditopic zwitterions to highly-soluble dicationic aromatics

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Advanced plastic scintillators for fast neutron discrimination

Feng, Patrick L.; Anstey, Mitchell A.; Doty, Fred P.; Mengesha, Wondwosen M.

The present work addresses the need for solid-state, fast neutron discriminating scintillators that possess higher light yields and faster decay kinetics than existing organic scintillators. These respective attributes are of critical importance for improving the gamma-rejection capabilities and increasing the neutron discrimination performance under high-rate conditions. Two key applications that will benefit from these improvements include large-volume passive detection scenarios as well as active interrogation search for special nuclear materials. Molecular design principles were employed throughout this work, resulting in synthetically tailored materials that possess the targeted scintillation properties.

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Thermal neutron detection using alkali halide scintillators with Li-6 and pulse shape discrimination

Brubaker, Erik B.; Dibble, Dean C.; Mengesha, Wondwosen M.; Yang, Pin Y.

An ideal 3He detector replacement for the near- to medium-term future will use materials that are easy to produce and well understood, while maintaining thermal neutron detection efficiency and gamma rejection close to the 3He standard. Toward this end, we investigated the use of standard alkali halide scintillators interfaced with 6Li and read out with photomultiplier tubes (PMTs). Thermal neutrons are captured on 6Li with high efficiency, emitting high-energy and triton (3H) reaction products. These particles deposit energy in the scintillator, providing a thermal neutron signal; discrimination against gamma interactions is possible via pulse shape discrimination (PSD), since heavy particles produce faster pulses in alkali halide crystals. We constructed and tested two classes of detectors based on this concept. In one case 6Li is used as a dopant in polycrystalline NaI; in the other case a thin Li foil is used as a conversion layer. In the configurations studied here, these systems are sensitive to both gamma and neutron radiation, with discrimination between the two and good energy resolution for gamma spectroscopy. We present results from our investigations, including measurements of the neutron efficiency and gamma rejection for the two detector types. We also show a comparison with Cs2LiYCl6:Ce (CLYC), which is emerging as the standard scintillator for simultaneous gamma and thermal neutron detection, and also allows PSD. We conclude that 6Li foil with CsI scintillating crystals has near-term promise as a thermal neutron detector in applications previously dominated by 3He detectors. The other approach, 6Li-doped alkali halides, has some potential, but require more work to understand material properties and improve fabrication processes.

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Anomaly metrics to differentiate threat sources from benign sources in primary vehicle screening

Mengesha, Wondwosen M.

Discrimination of benign sources from threat sources at Port of Entries (POE) is of a great importance in efficient screening of cargo and vehicles using Radiation Portal Monitors (RPM). Currently RPM's ability to distinguish these radiological sources is seriously hampered by the energy resolution of the deployed RPMs. As naturally occurring radioactive materials (NORM) are ubiquitous in commerce, false alarms are problematic as they require additional resources in secondary inspection in addition to impacts on commerce. To increase the sensitivity of such detection systems without increasing false alarm rates, alarm metrics need to incorporate the ability to distinguish benign and threat sources. Principal component analysis (PCA) and clustering technique were implemented in the present study. Such techniques were investigated for their potential to lower false alarm rates and/or increase sensitivity to weaker threat sources without loss of specificity. Results of the investigation demonstrated improved sensitivity and specificity in discriminating benign sources from threat sources.

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Fast neutron resonance tomography using double scatter spectroscopy for materials identification

IEEE Nuclear Science Symposium Conference Record

Marleau, Peter M.; Brennan, James S.; Brubaker, Erik B.; Mengesha, Wondwosen M.; Mrowka, Stanley M.

Fast neutron based inspection systems are of interest in many Homeland Security applications because they offer the potential for elemental identification particularly for low Z elements which are the prime constituents of explosives. We are investigating a resonance tomography technique which may address some of the current problems found in fast neutron based inspection systems. A commercial off-the-shelf DT generator is used with an array of detectors to probe materials simultaneously over a large energy range and multiple viewing angles allowing for simultaneous 3-D imaging and materials identification. A prototype system has been constructed and we present here recent results for the identification of materials with differing H, C, N, O compositions. © 2011 IEEE.

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Directional neutron detectors for use with 14 MeV neutrons :fiber scintillation methods for directional neutron detection

Mascarenhas, Nicholas M.; Peel, Justin P.; Mengesha, Wondwosen M.; Sunnarborg, Duane A.

Current Joint Test Assembly (JTA) neutron monitors rely on knock-on proton type detectors that are susceptible to X-rays and low energy gamma rays. We investigated two novel plastic scintillating fiber directional neutron detector prototypes. One prototype used a fiber selected such that the fiber width was less than 2.1mm which is the range of a proton in plastic. The difference in the distribution of recoil proton energy deposited in the fiber was used to determine the incident neutron direction. The second prototype measured both the recoil proton energy and direction. The neutron direction was determined from the kinematics of single neutron-proton scatters. This report describes the development and performance of these detectors.

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21 Results
21 Results