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Fiscal Year 2020 Report for the Radiation Detection for Nuclear Security Summer School

The Pacific Northwest National Laboratory (PNNL) planned to hold its 6th Radiation Detection for Nuclear Security Summer School 15-26 June 2020. The COVID-19 pandemic prevented an in-person school from happening, and PNNL staff did not have adequate time to prepare a virtual format school. So fiscal year 2020 was taken as an off year with the intention of hosting an in-person or online summer school in 2021. As with typical off years, some course materials and activities were refined to better achieve the key objectives of 1) exposing students to the range of nuclear security applications for which radiation detection is necessary, 2) articulating the relevance of student research into the broader context, and 3) growing student interest in careers in nuclear security.

61 RADIATION PROTECTION AND DOSIMETRY↗

Partnership for Radiation Studies (PaRS): A Consortium for Advancing Radiation Science among Underrepresented STEM Students

The Partnership for Radiation Studies (PaRS) consortium was recently awarded by U.S. Department of Energy’s National Nuclear Security Administration (NNSA). The five-year grant aims to increase the number of underrepresented students in STEM disciplines, with simultaneous advancement of nuclear radiation science. The goal is to hire more underrepresented minorities at national laboratories. The consortium’s progress will be tracked/reported annually. This paper and subsequent presentation cover details of the consortium, highlighting the key activities of participating national laboratories in assisting the minority-serving institutions.

Minority Serving Institutions Partnership Program,↗

The Radiation Detection for Nuclear Security Summer School: Fiscal Year 2024 Report

The Pacific Northwest National Laboratory (PNNL) hosts the Radiation Detection for Nuclear Security (RDNS) Summer School. This unique course provides students with an overview of nuclear security missions, the technical foundation of applied radiation detection technology, and interactive demonstrations and exercises to connect theory to practice in an evolving research and development area. Fiscal year 2024, an off-year year for the school, included reviewing course content, and sharing about the school in a student engagement session at the Institute of Nuclear Materials Management Annual Meeting. Planning is underway for the 10 th RDNS summer school is planned for the summer of 2025.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Summary Report for the 2019 Radiation Detection for Nuclear Security Summer School

The Pacific Northwest National Laboratory (PNNL) hosted students from across the United States at the 6th Radiation Detection for Nuclear Security Summer School 17-28 June 2019. The summer school provided students with a unique understanding of nuclear security challenges faced in the field and exposed them to the technical foundations, analyses, and insight that will be required by future leaders in technology development and implementation. The course heavily emphasized laboratory and field demonstrations including measurements of special nuclear material. Student evaluations and feedback from student advisors indicates that the summer school achieved its objectives of 1) exposing students to the range of nuclear security applications for which radiation detection is necessary, 2) articulating the relevance of student research into the broader context, and 3) growing student interest in careers in nuclear security.

61 RADIATION PROTECTION AND DOSIMETRY↗

Nuclear and Chemical Sciences Division: Investment Strategy 2023

The mission of the Nuclear and Chemical Sciences (NACS) Division within the Physical and Life Sciences (PLS) Directorate is to advance scientific understanding, capabilities, and technologies in nuclear and particle physics, radiochemistry, forensic science, and isotope systems to support LLNL’s national security mission. NACS Division personnel conduct a diverse range of research activities in particle physics, nuclear physics, radiation detection, nuclear measurements, chemical and nuclear forensic science, nuclear and radiochemistry, isotope geochemistry, and environmental science. These areas are leveraged to address evolving national security challenges. Scientific research provides the foundation for addressing these challenges, and it is also the principal means of attracting, training, and retaining staff scientists who can deliver solutions across the Laboratory’s mission space. The overarching strategy is to position the NACS Division at the nexus between fundamental nuclear and chemical science research and nuclear security applications. This approach will support efforts to recruit, train, and retain top-flight scientists and engineers who will play a key role in executing the Laboratory’s core nuclear security missions, while also enhancing LLNL’s reputation as a center for innovative scientific research. This document describes the strategic vision that will be used to guide key investments aimed at enabling NACS scientists to lead new efforts and meet future challenges.

07 ISOTOPE AND RADIATION SOURCES↗

Cadmium Magnesium Telluride for Next Generation X-Ray Free Electron Laser, Synchrotron and Many Other Applications

We developed a picosecond photodetector based on our Bridgman grown and specially engineered Cadmium Magnesium Telluride (Cd 1-x Mg x Te) single crystal that is sensitive to both optical and x-ray pulses for coarse timing in Free Electron Laser applications. Cd 1-x Mg x Te is a wide bandgap semiconductor material with potential applications, not only in optoelectronics, but also in particle physics as an intense pulse radiation detector for bremsstrahlung, X-ray/gamma ray radiation, thermal neutrons, and medical imaging. However, for femtosecond optical and x-ray cross correlation, the material has to have very short lifetime, a condition that is opposite to that required for nuclear spectroscopy applications. At the same time, the material also needs to have very low bulk leakage current, in the 0.10 pA range. Hence the ability to tailor or engineer the material is very crucial. In this paper, picosecond response and the crystal growth of this specially engineered cadmium magnesium telluride material will be presented. Other material characterization and transient measurements will also be discussed along with room temperature semiconductor detector performance for other nuclear radiation detection applications.

36 MATERIALS SCIENCE↗

Problems of Nuclear Technology and Radiation Safety

This work discusses ethical issues arising in the course of the development of nuclear technologies and related issues of radiation safety. Attention is paid to ethical dilemmas and proposed solutions. The author suggests a critical analysis of the relevant discussions, conducted, first of all, in the English-language literature, and muses on the specifics associated with their transfer to the Russian context. This study considers ethical problems arising in context of the depletion of uranium resources and nuclear waste management and including the inevitable risks for the present and future generations, such as inter- and intragenerational justice (Gardiner's problem) and the problem of the identity of future generations (Parfit’s problem); problems of collectivity and individuality in the assessment of permissible radiation doses for workers at nuclear enterprises and the population associated with the need to combine deontological and utilitarian approaches in the practice of radiation protection. The author demonstrates cultural differences in attitudes towards the safety of the current and future generations of the population of countries and regions and the associated ambiguities in the choice of technology for nuclear reactors, long-term disposal or processing of nuclear waste; double standards in ensuring the radiation safety of personnel of nuclear facilities and the population; ethical problems of risk compensation to workers of radiation-hazardous production facilities; issues of gender differences in sensitivity to radiation exposure, gender equality and discrimination in relation to access to the labor market in the nuclear industry. The article elucidates the importance of socio-humanitarian discussion of the ethical problems of nuclear technologies and radiation safety Such debates currently are almost absent in the Russian-language philosophical literature, despite its exceptional importance due to both the level of development of nuclear energy in Russia and the potential risks that these technologies pose to current and future generations of both employees of nuclear facilities and the population of the country, neighboring countries, and the world. The purpose of this article, thus, is to initiate such a discussion.

ethics of science and technology↗

Irradiation Characterization of Pressure Transducers

The advancement of reactor technologies for space and remote applications requires further investigation into the long-term operation of instrumentation without the chance for standard scheduled maintenance. Specifically, the degradation of instrumentation due to exposure to nuclear radiation needs to be understood. Determining the methods of degradation can improve material selection for instrument construction and provide foundational data for the development of corrective algorithms. Initial work has been focused on the development of nuclear thermal rocket technology and the instrumentation needs that will led to its eventual deployment.

Floyd, Dan↗

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 ↗

2023 Radiation Detection for Nuclear Security Summer School (Summary Report)

The Pacific Northwest National Laboratory (PNNL) hosted the 9th Radiation Detection for Nuclear Security Summer School 20-30 June 2023 in Richland, WA. The school provided students with an understanding of nuclear security challenges faced in the field and exposed them to the technical foundations and insight needed to contribute to this applied research and development area.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Principal Component Analysis of Nuclear Cable Insulation Subjected to Elevated Temperature and Gamma Radiation

In nuclear power plants (NPPs), the aging of electrical cable insulation occurs due to elevated temperature, ionizing radiation, and other environmental factors. To ensure the safe and efficient operation of NPPs, determination of key indicators of cable aging is critical to predict the remaining useful lifetime of electrical cable insulation. In this work, the effects of simultaneous and sequential thermal and gamma radiation on the aging of cross-linked polyethylene (XLPE) electrical cable insulation are investigated. The chemical changes of the insulation were monitored non-destructively through the use of Fourier transform infrared (FTIR) spectroscopy. The FTIR spectra were measured stepwise after predetermined exposure intervals, with a total irradiation dose up to 320 kGy at a dose rate of 300 Gy/hr in two exposure scenarios; simultaneously aged samples were heated at 150 °C during irradiation, while sequentially aged samples were heated at 150 °C for designated durations followed by corresponding times of irradiation at ambient temperature. A data-driven approach using principal component analysis (PCA) was developed to highlight changes in the carbonyl region of the infrared spectra of the aged samples due to oxidation and to differentiate oxidation rates under the simultaneous and sequential exposure conditions. Findings indicate that the sequential aging scenario may be more conservative than the simultaneous aging scenario for XLPE electrical cable insulation.

Li, Donghui↗

Characterization of CdZnTeSe Nuclear Detector Chemically Etched in Bromine Methanol

Semiconductor nuclear radiation detectors made from tertiary and quaternary compounds of cadmium telluride (CdTe) can operate at room temperature without cryogenic cooling. One of such materials that have become of great interest is cadmium zinc telluride selenide (CdZnTeSe). Compared to other CdTe-based materials, such as cadmium zinc telluride (CdZnTe), CdZnTeSe can be grown with much less Te inclusions and sub-grain boundary networks. Chemical etching is often used to smoothen wafer surfaces during detector fabrication. This paper presents the characterization of CdZnTeSe that is chemically etched using bromine methanol solution. Infrared imaging shows that the wafer has no sub-grain boundary networks that often limit detector performance. The current-voltage (I-V) characterization experiment gave a resistivity of 4.6 × 10 10 Ω-cm for the sample. The I-V curve was linear in the ±10 to ±50 volts range. An energy resolution of 7.2% was recorded at 100 V for the 59.6-keV gamma line of 241 Am.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

GPR Robotic Assisted Non-Destructive Evaluation of Concrete Structures - 20196

Reinforced concrete structures are always under exposure of internal or external deteriorations due to many factors such as environmental, nuclear radiation or even construction deficiencies. The use of nondestructive test is one of the reliable methods to inspect structural members. In this case, GPR has a good capability to detect inside deteriorations of concrete structures. However, in many cases it is hard to inspect structural members by hand due to safety issues or inaccessibility. Thus, an alternative way to reduce such risks is to employ robot to carry nondestructive equipment. In this research, twelve reinforced concrete RC beams (8 x 16 x 96, width, height and length) are cast in the lab. Three RC beams have no defect and nine others various defects such as corrosion, de-bonded bars, void, delamination and honeycombing. The one-point load is applied at the center of the RC beam. The loading level is carried out at three levels: 50%, 75% and 100% of maximum load and total load-displacement diagram are performed. The load is held at each level and the robotic GPR is used to scan the side of RC beams. Then, RADAN software is employed to find out any defects at different loading conditions and visualize the crack propagation. The RADAN results show that the pattern of crack propagation for corrosion and debonding are same. Also, the load-displacement results present that inside defect cause reduction of load-capacity of RC beam. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Alternating chempolishing and electropolishing for interior and exterior surface finishing of additively manufactured (AM) metal components

Additively manufactured (AM) components’ surface finishing is crucial in adopting them for intended applications in challenging environments involving fatigue, corrosion, high temperature, and nuclear radiation. In our prior research, chempolishing (C) was utilized as an electroless etching process that uniformly smoothens complex AM components’ accessible interior and exterior surfaces (Tyagi et al. Additive Manufacturing, 25:32–38, 22). A wide range of electropolishing (E) has been demonstrated for AM surface finishing. However, electropolishing can impact a surface that can be juxtaposed to counter electrode and can yield a very smooth surface to sub-micrometer level roughness. However, a knowledge gap exists about the impact of applying both approaches on the same surface one after another and what new advantages may arise because of combining two methods. This paper uses dual-stage liquid-based surface finishing strategies produced by alternating the chempolishing (C) and electropolishing (E) steps. Two dual-stage surface finishing approaches, i.e., chempolishing followed by electropolishing (CE) and electropolishing followed by chempolishing (EC), were performed on the 316 stainless AM steel component. Impacts of EC and CE approaches were compared with single-stage C and E surface finishing approaches. An optical microscope and mechanical profilometer were utilized to investigate the wide range of surface roughness parameters. CE and EC produced Ra ~ 1.4 µm and ~ 1.6 µm, respectively. Surface roughness on CE- and EC-treated AM samples was lower than those individually treated by C and E approaches. Scanning electron microscopy provided further insights into the microstructural difference between CE- and EC-treated AM samples. This paper reports a liquid contact angle study on CE- and EC-treated AM samples to provide insights into the relative difference in surface energy that is crucial for making coatings on AM parts. A spectroscopic reflectance study was also employed to register the difference in physical properties of AM components treated with CE and EC approaches. Further, this study reveals industrially practicable interior and exterior surface finishing approaches for complex AM metal components that require minimum tooling and real-time process monitoring.

36 MATERIALS SCIENCE↗

Plastic scintillators stable for operating in wide ranges of humidity and temperature variations

To provide efficient and reproducible response to nuclear radiation, scintillating plastics should be prepared as materials of high optical transparency and homogeneity that should remain intact during the lifetime of their operation. A problem with traditionally used polyvinyltoluene (PVT) or polystyrene (PS) plastic scintillators arises from their exposure to repeated large temperature swings that cause surface and volume defects, resulting in decreased sensitivity of the detection properties. We find that the problem can be avoided by composition modifications that enable preparation of plastics with properties that are resistant to the continuous variations in environmental conditions. This paper describes improvements in physical properties that can be achieved by the addition of crosslinkers (such as divinylbenzene, DVB) and oxygen-containing compounds or copolymers (e.g. polymethylamethacrylate, PMMA) to the traditional PVT or PS polymer matrices. Results of characterization show that the new materials can be prepared with the scintillation performance equal to that of commercial plastic scintillators, such as EJ-200.

36 MATERIALS SCIENCE↗

Light output quenching in response to deuterium-ions and alpha particles and pulse shape discrimination in deuterated trans-stilbene

We characterized the light output response of a new 140 cm 3 stilbene-d 12 crystal up to 14.1 MeV neutron energies using a coincidence neutron scattering system. We also characterized its light output response to alpha particles in the 5 to 6 MeV energy range. The excellent PSD capability of the stilbene-d 12 detector allowed us to select light pulses produced by particles of increasing ionization density, namely electrons, protons, deuterium-ions, and alpha particles. The measured fast decay component of the light pulses is increasingly quenched as the ionization density of the particle in the crystal increases. Consistently with this finding, the Birks’ quenching parameter of alpha particles is approximately 8.5 times larger compared to the quenching of deuterium ions, produced by neutron scattering interactions. The reported experimental characterization will allow high-fidelity modeling of the detector enabling its application for fast-neutron detection and spectroscopy in nuclear physics, radiation protection, nuclear security, and non-proliferation.

36 MATERIALS SCIENCE↗

Effects of Selenium Doping in Zinc Telluride from First Principles

We report point defects and compensation in zinc telluride have been subjects of study for several decades due to the compound’s scientific/technological applications. Despite this, there remains some disagreement in the literature as to the fine details of its defect chemistry. Recently, it has also come under renewed interest due to the emerging Cd( 1–x )Zn x Te( 1–y )Se y material family, used in nuclear radiation detector applications. In this article, we use state-of-the-art computational tools to re-examine the native defect chemistry of ZnTe and explore how it changes upon addition of selenium using density functional theory with screened hybrid exchange–correlation functionals, thermochemical models of the equilibration environment, and statistical mechanics models of the point defect ensemble.

II-VI semiconductors↗

Demonstration of Energy-Resolved γ-Ray Detection at Room Temperature by the CsPbCl 3 Perovskite Semiconductor

The detection of gamma-rays at room temperature with high-energy resolution using semiconductors is one of the most challenging applications. The presence of even the smallest amount of defects is sufficient to kill the signal generated from gamma-rays which makes the availability of semiconductors detectors a rarity. Lead halide perovskite semiconductors exhibit unusually high defect tolerance leading to outstanding and unique optoelectronic properties and are poised to strongly impact applications in photoelectric conversion/detection. Here we demonstrate for the first time that large size single crystals of the all-inorganic perovskite CsPbCl 3 semiconductor can function as a high-performance detector for gamma-ray nuclear radiation at room temperature. CsPbCl 3 is a wide-gap semiconductor with a bandgap of 3.03 eV and possesses a high effective atomic number of 69.8. We identified the two distinct phase transitions in CsPbCl 3 , from cubic (Pm-3m) to tetragonal (P4/mbm) at 325 K and finally to orthorhombic (Pbnm) at 316 K. Despite crystal twinning induced by phase transitions, CsPbCl 3 crystals in detector grade can be obtained with high electrical resistivity of similar to 1.7 X 10 9 Ω∙cm. The crystals were grown from the melt with volume over several cubic centimeters and have a low thermal conductivity of 0.6 W m -1 K -1 . The mobilities for electron and hole carriers were determined to similar to 30 cm 2 /(V s). Using photoemission yield spectroscopy in air (PYSA), we determined the valence band maximum at 5.66 +/- 0.05 eV. Under gamma-ray exposure, our Schottky-type planar CsPbCl 3 detector achieved an excellent energy resolution (similar to 16% at 122 keV) accompanied by a high figure-of-merit hole mobility-lifetime product (3.2 x 10 -4 cm 2 /V) and a long hole lifetime (16 mu s). The results demonstrate considerable defect tolerance of CsPbCl 3 and suggest its strong potential for gamma-radiation and X-ray detection at room temperature and above.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗