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Lithium indium diselenide — An advanced material for neutron detection

Here, this paper describes the synthesis, crystal growth, detector fabrication, radiation hardening studies, MCNP modeling, and characterization of lithium indium diselenide or LiInSe 2 . This newly-developed room temperature thermal neutron detector has semiconducting and scintillating properties and it is suitable for neutron detection application. LiInSe 2 was synthesized starting from elemental Li, In, Se in two steps due to high reactivity of Li. A single crystal of LiInSe 2 was grown using the Vertical Bridgman method. The room temperature band gap was found to be 2.8 eV using optical absorption measurements. Bulk resistivity was measured at ∼5 × 10 11 Ωcm. Photoconductivity measurements of LiInSe 2 wafers identified a peak in the photocurrent around 445 nm. Nuclear radiation detectors were fabricated from single crystal wafer and the responses to alpha particles at various biases were measured. The mobility-lifetime product was estimated. Gamma irradiation studies were performed with calculated absorbed doses ranging from 0.2126 to 21,262 Gy. The characterization of the two wafers for their scintillator performance was conducted after each irradiation. The gamma irradiation produced a reduction of the light yield that translated to a lower channel number for the centroid of alpha detection spectra. It also showed a considerable reduction of the decay time after the first irradiation. These are the first studies on gamma radiation hardening with this material.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Mixed Material Scintillator Systems for Neutron Detection

Scintillators are a fundamental technology that enables radiation detection. Their use has historically enabled the detection of incoming gamma radiation, with recent advances in plastic scintillator development enabling detection and discrimination of neutron and gamma radiation through pulse shape discrimination. However, scintillators have so far consisted of a single material, typically one primary dye and one secondary dye embedded in a plastic matrix. Based on the simulation studies described previously, mixed material scintillator systems with multiple secondary dyes arranged in alternating, periodic micro-sized regions opens the door for scintillators with a wide variety of different capability, such as directional sensing, positional reconstruction, particle identification, and pulse shape discrimination. However, fabrication of a mixed material scintillator system by conventional manufacturing methods is difficult to manufacture and scale, creating a barrier to their wide spread implementation. On the other hand, additive manufacturing additive manufacturing presents itself as the optimal method for fabricating mixed material scintillator systems based on its flexibility, ability to fabricate fine features, and potential for multimaterial fabrication.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

TU-F-BRE-07: In Vivo Neutron Detection in Patients Undergoing Stereotactic Ablative Radiotherapy (SABR) for Primary Kidney Cancer Using 6Li and 7Li Enriched TLD Pairs

Purpose: Stereotactic ablative radiotherapy (SABR) for primary kidney cancer often involves the use of high-energy photons combined with a large number of monitor units. While important for risk assessment, the additional neutron dose to untargeted healthy tissue is not accounted for in treatment planning. This work aims to detect out-of-field neutrons in vivo for patients undergoing SABR with high-energy (>10 MV) photons and provides preliminary estimates of neutron effective dose. Methods: 3 variations of high-sensitivity LiF:Mg,Cu,P thermoluminescent dosimeter (TLD) material, each with varying {sup 6}Li / {sup 7}Li concentrations, were used in custom-made Perspex holders for in vivo measurements. The variation in cross section for thermal neutrons between Li isotopes was exploited to distinguish neutron from photon signal. Measurements were made out-of-field for 7 patients, each undergoing 3D-conformal SABR treatment for primary kidney cancer on a Varian 21iX linear accelerator. Results: In vivo measurements show increased signal for the {sup 6}Li enriched material for patients treated with 18 MV photons. Measurements on one SABR patient treated using only 6 MV showed no difference between the 3 TLD materials. The out-of-field photon signal decreased exponentially with distance from the treatment field. The neutron signal, taken as the difference between {sup 6}Li enriched and {sup 7}Li enriched TLD response, remains almost constant up to 50 cm from the beam central axis. Estimates of neutron effective dose from preliminary TLD calibration suggest between 10 and 30 mSv per 1000 MU delivered at 18 MV for the 7 patients. Conclusion: TLD was proven to be a useful tool for the purpose of in vivo neutron detection at out-of-field locations. Further work is required to understand the relationship between TL signal and neutron dose. Dose estimates based on preliminary TLD calibration in a neutron beam suggest the additional neutron dose was <30 mSv per 1000 MU at 18 MV.

60 APPLIED LIFE SCIENCES↗

Improvements to neutron detection of Pu in solvent for an aqueous buffer tank, magnox reprocessing plant, Sellafield - 14216

The PP Active Feed Tank (PPAFT) is a buffer tank that is not safe by geometry and which is located between the Medium Active (MA) and Plutonium Purification (PP) cycles of the chemical separation process in the Magnox Reprocessing Plant. The PPAFT receives Pu nitrate in acid which has been conditioned ready for the extraction of Pu with TBP/OK (tri-butyl phosphate in kerosene) solvent in the PP Cycle. The criticality safety case for the PPAFT recognises that during both normal operations and potential maloperations solvent which is dissolved (TBP which is present in solution but can be released upon a change in acidity) and entrained (TBP/OK physically carried over but not in solution) will accumulate in the PPAFT. The only practicable route out for Pu in solvent in the PPAFT is the normal process route out from the base of the PPAFT to the PP cycle through intermediate vacuum lift and feed vessels. However, the dished end base of the PPAFT and the intermediate vacuum lift and feed vessels are of particularly challenging geometry. There are five neutron monitors placed around the PPAFT for the detection of Pu in solvent. The original design intent of the neutron detection system was that any single monitor should be able to reveal an accumulation of Pu in solvent before it would potentially be unsafe if fed downstream. However, over time there have been changes to the fuel feed and chemical process of the plant which have had the potential to affect the performance of the neutron monitoring system. The ability of the neutron monitoring system to function to its original intent was questioned. Work has recently been carried out to investigate the capabilities of the PPAFT neutron monitoring system for current plant conditions and to identify potential improvements while making best use of the existing neutron monitors. It was found that moving a neutron monitor from the side to the top of the PPAFT and adding alarms based on the ratio of signals from multiple neutron detectors would be effective in improving detection of Pu in solvent. This paper describes the challenges involved in detecting thin layers of Pu in solvent using neutron monitors, discusses the improvements made to the PPAFT neutron monitors and details the combination of real plant data and modelling with the shielding code MCBEND used to provide confidence in the enhanced neutron monitoring system. (author)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Thin epitaxial silicon PIN detectors for thermal neutron detection with improved gamma (γ) discrimination

In order to improve the gamma discrimination capability for thermal neutron measurements using silicon PIN detectors, a novel approach of use of thin epitaxial silicon PIN detectors was investigated. Thin epitaxial silicon detectors with thickness of 15 µm were developed and their performance was tested with thermal neutrons using {sup 10}B converter. The performance of this detector was compared with the performance of a 300 µm silicon detector. The results of experiments presented in this paper indicate that thin epitaxial silicon detectors can significantly improve γ discrimination for thermal neutron measurements.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

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 ↗

Characterization of a boron-loaded deuterated liquid scintillator for fast and thermal neutron detection

The preparation and characterization of novel boron-loaded deuterated liquid scintillators (BLDLS) are presented for the first time to investigate the performance of a detector sensitive to both fast and thermal neutrons intended for future neutron spectroscopy measurements. Three deuterated toluene-based scintillation cocktails were produced, one without boron, one loaded with ortho-carborane (natural boron isotopic abundance), and one with 96 wt% 10B enriched ortho-carborane. General optical and material properties were analyzed to include the composition, density, index of refraction, photoluminescence emission spectra, and absorbance spectra in addition to the relative light yield, resolution, relative efficiency, and pulse-shape-discrimination performance for all three scintillators and a hydrogen-based EJ-309 scintillator to evaluate the effects of boron loading in comparison with a common commercially-available scintillator and feasibility for future neutron spectroscopy measurements. Finally, the detection of shielded neutron sources was explored to capitalize on the 10B thermal neutron capture reaction. The results showed loading the scintillators with boron deteriorated the PSD performance slightly compared to the unloaded deuterated scintillator and resulted in a relative light yield loss of 26% and 41% for the 10B enriched and natural boron BLDLS, respectively. Lastly, the BLDLS have a higher relative detection efficiency than the unloaded deuterated scintillator for shielded neutron sources, based on total count rate, a desirable characteristic for missions related to finding and characterizing illicitly-trafficked special nuclear material.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

B{sub 4}C thin films for neutron detection

Due to the very limited availability of {sup 3}He, new kinds of neutron detectors, not based on {sup 3}He, are urgently needed. Here, we present a method to produce thin films of {sup 10}B{sub 4}C, with maximized detection efficiency, intended to be part of a new generation of large area neutron detectors. B{sub 4}C thin films have been deposited onto Al-blade and Si wafer substrates by dc magnetron sputtering from {sup nat}B{sub 4}C and {sup 10}B{sub 4}C targets in an Ar discharge, using an industrial deposition system. The films were characterized with scanning electron microscopy, elastic recoil detection analysis, x-ray reflectivity, and neutron radiography. We show that the film-substrate adhesion and film purity are improved by increased substrate temperature and deposition rate. A deposition rate of 3.8 A/s and substrate temperature of 400 deg. C result in films with a density close to bulk values and good adhesion to film thickness above 3 {mu}m. Boron-10 contents of almost 80 at. % are obtained in 6.3 m{sup 2} of 1 {mu}m thick {sup 10}B{sub 4}C thin films coated on Al-blades. Initial neutron absorption measurements agree with Monte Carlo simulations and show that the layer thickness, number of layers, neutron wavelength, and amount of impurities are determining factors. The study also shows the importance of having uniform layer thicknesses over large areas, which for a full-scale detector could be in total {approx}1000 m{sup 2} of two-side coated Al-blades with {approx}1 {mu}m thick {sup 10}B{sub 4}C films.

36 MATERIALS SCIENCE↗

Solution growth of a deuterated trans -stilbene crystal for fast neutron detection

The paper reports results on growth and characterization of the first deuterated analog of the trans -stilbene crystal. The high optical quality stilbene-d12 single crystal was grown by application of the solution technique using specially synthesized raw material and an aromatic solvent (anisole). Optical, physical, and scintillation properties of the new material are compared to those of the regular trans -stilbene crystal. In conclusion, the new deuterated material is promising for use in fast neutron spectroscopy without the need for time-of-flight measurements.

36 MATERIALS SCIENCE↗

SNM neutron detection using a time-gated synthetic aperture hybrid approach

This work focuses on using forward and adjoint transport in a hybrid application of 3-D deterministic (PENTRAN) and Monte Carlo (MCNP5) codes to model a series of neutron detector blocks. These blocks, or 'channels, ' contain a unique set of moderators with 4 atm He-3 detectors tuned to detect and profile a gross energy spectrum of a passing neutron (SNM) source. Ganging the units together as a large area system enables one to apply time gating the source-detector response to maximize signal to noise responses from a passing source with minimal background; multiple units may be positioned as a collective synthetic aperture detector array to be used as a way of performing real time neutron spectroscopy for detecting special nuclear materials in moving vehicles. The initial design, detector response coupling, confirmation of initial design functionality using adjoint transport calculations, and realistic simulation using PENTRAN and MCNP5 are presented. Future work will include optimization and application to realistic scenarios and additional sources. (authors)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗