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Verification of Special Nuclear Material (SNM) using Active Well Coincidence Counter (AWCC) and a High Purity Germanium (HPGe) Detector

SNM verification can be accomplished via two methods i.e. destructive analysis (DA) or nondestructive analysis (NDA). The DA modes are much more accurate compared to NDA modes; nevertheless, the sample's physical integrity is destroyed in the process. Techniques such as ICP-MS, ID-ICP-MS, TI-MS are few examples of DA, where a bulk material is ground and mixed with a solution (some form of acid) to acquire a homogenous sample. In contrast, NDA modes utilize signals emitted by the sample such as gamma, neutrons, light, or heat to analyze samples under investigation. HPGe detectors are some of the most frequently used gamma detectors to assay SNM. However, in a high activity scenario it provides a large uncertainty and sometimes becomes unfeasible to measure low energy gamma rays. Meanwhile, neutron detectors are not affected by the gamma background, therefore they can be used in addition to the gamma detectors to verify total fissile mass ({sup 235}U + {sup 239}Pu) of SNM. The AWCC is one of the thermal neutron NDA systems developed at the Los Alamos National Laboratory (LANL). It consists of 42 {sup 3}He detectors to measure gross neutrons (singles), coincidence neutrons (doubles), higher order multiplicity counting (triples, quadruples, etc.). It can effectively operate in both active and passive neutron interrogation modes. It can utilize AmLi, AmBe, or {sup 252}Cf active interrogation neutron sources. It is used to verify declared fissile mass ({sup 235}U or {sup 239}Pu) present in SNM. Objectives: Calibrate HPGe and AWCC for lightly irradiated (with enough {sup 137}Cs gamma background) ∼93% enriched HEU fuels; Verify fissile mass ({sup 235}U +{sup 239}Pu) content using AWCC and HPGe; Model and benchmark AWCC in MCNP6. Neutron coincidence and multiplicity counting: Two or more neutrons are coincident if they are detected by the system within the specified gate window; In AWCC: Gate window is 128 μsec; Induced fission in fissile material such as {sup 235}U and {sup 239}Pu - emission of time correlated neutrons - Singles, Doubles, Triples, or Quadruples; No induced fission in non-fissile materials- no correlated neutrons - only singles. SNM can be verified with high accuracy and precision using gamma and neutron NDA instruments such as HPGe and AWCC. Interaction with thermal neutrons. Non-fissile atoms - do not emit correlated neutrons. Fissile atoms - emit correlated neutrons during induced fission events. The time correlated neutrons can be detected by using coincidence or multiplicity counters such as AWCC. Likewise, {sup 235}U produces 186 keV gamma peak that can be measured by a HPGe gamma detector. Counts under 186 keV gamma peak provide information about {sup 235}U content. Combining AWCC and HPGe results can provide better understanding of special nuclear material under investigation.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

CLARION2-TRINITY: A Compton-suppressed HPGe and GAGG:Ce-Si-Si array for absolute cross-section measurements with heavy ions

The design and performance of a new Compton-suppressed HPGe and charged-particle array, CLARION2-TRINITY, are described. The TRINITY charged-particle array is comprised of 64 Cerium-doped Gadolinium Aluminum Gallium Garnet (GAGG:Ce) crystals configured into five rings spanning 7–54 degrees, and two annular silicon detectors that can shadow or extend the angular coverage to backward angles with minimal $\gamma$-ray attenuation. GAGG:Ce is a non-hygroscopic, bright, and relatively fast scintillator with a light distribution well matched to SiPMs. Count rates up to 40 kHz per crystal are sustainable. Fundamental characteristics of GAGG:Ce are measured and presented, including light- and heavy-ion particle identification (PID) capability, pulse-height defects, radiation hardness, and emission spectra. The CLARION2 array consists of up to 16 Compton-suppressed HPGe Clover detectors (efficiency at 1 MeV) configured into four rings (eight HPGe crystal rings) using a non-Archimedean geometry that suppresses back-to-back coincident 511-keV gamma rays. The entire array is instrumented with 100- and 500-MHz (14 bit) waveform digitizers which enable triggerless operation, pulse-shape discrimination, fast timing, and pileup correction. Lastly, two examples of experimental data taken during the commissioning of the CLARION2-TRINITY system are given: a PID spectrum from 16 O + 18 O fusion-evaporation, and PID and Doppler-corrected -ray spectra from 48 Ti + 12 C Coulomb excitation.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Field Scoping Study of Gamma-Ray Measurement of UF 6 Cristillini Samples with CZT and HPGe Detectors

A field scoping study was conducted to evaluate the ability of Cd-Zn-Te (CZT) detectors and High Purity Germanium (HPGe) detectors to quantify the U-235 enrichment in UF 6 samples collected on alumina in P-10 tubes, similar to the Cristillini method of sample collection for analysis by mass spectrometry. With in-field gamma-ray spectroscopy methods, international safeguards and verification missions could benefit from quick in-field confirmation of declared enrichment values prior to or without the need for additional shipping, sample preparation and analysis. Samples of depleted (DU), low-enriched (LEU) and high-assay low-enriched (HALEU) uranium were collected on Cristillini-type alumina in P-10 tubes and measured with two H3D, Inc. M400 CZT detectors as well as a Canberra Falcon HPGe detector. The M400 detectors were able to confirm enrichment in the DU and LEU samples but not the HALEU sample in measurements 8-40 hrs after collection. The Falcon system was able to confirm enrichment in all three samples. Improvements in detector geometry, increase in number of detectors as well as increase sample mass loading may allow measurement of U-235 enrichment in these types of samples within 4-8hrs of collection with 5-10% uncertainty.

98 - NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL↗

Reassessment of PHDS Fulcrum40h High Purity Germanium (HPGe) Detector System Performance

This report presents a comprehensive evaluation of the updated PHDS Fulcrum40h High Purity Germanium (HPGe) detector system, benchmarking its performance, usability, and software capabilities against the current National Nuclear Security Administration (NNSA) Nuclear Emergency Support Team (NEST) HPGe Detector System Requirements Document. Systematic measurements were conducted using a single Fulcrum40h detector to assess key parameters including gamma efficiency and resolution, neutron detection efficiency, gamma pulse-pileup response, and gamma-to-neutron crosstalk. The Fulcrum40h system, acquired in August 2022, has undergone recent updates by PHDS to address deficiencies identified following the initial NEST requirements release. The results provide critical insights into the detector’s operational capabilities and compliance with NNSA NEST standards.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Evaluation of simulated HPGe detector efficiencies in OpenMC compared to MCNP

In late 2023, the open-source radiation transport code OpenMC introduced a pulse-height tally (PHT) feature, enabling users to track the total energy deposited by individual photons in OpenMC cells. This function represents an important improvement of the OpenMC code because it allows users to simulate the response function of a gamma detector without relying on closed-source alternatives. Despite this, limited work has been published evaluating OpenMC as a radiation transport code for simulating gamma spectroscopy experiments. This study attempts to demonstrate the usefulness of OpenMC in this space by directly comparing its PHT output to MCNP (a trusted industry-standard Monte Carlo code). In the first half of this study, a radiation transport experiment is described in which a detector with a complex internal geometry is exposed to various gamma-emitting isotopes ( 133 Ba, 137 Cs, and 60 Co) over a range of distances. The setup of this experiment was modeled in MCNP with sufficient detail to capture the efficiency characteristics of a high purity germanium (HPGe) detector for the primary gammas of each isotope. After good agreement between the MCNP model and experiment was achieved, an identical model was produced in OpenMC to allow direct comparison between the full energy peak (FEP) values produced in OpenMC and MCNP. The results show strong agreement between OpenMC and MCNP across the full range of tested energies, with each model’s FEP values typically within 2% of each other and most FEP areas within 4% of experimental data. Worse agreement was seen between the Monte Carlo codes and experiment below 300 keV (an expected result). For the 662 keV line of 137 Cs, both codes were found in poor agreement with experiment and each other over the full range of distances tested (possibly indicating an error with the 137 Cs experimental data). Ignoring the anomalous results of the 662 keV line, all other data show good qualitative and quantitative agreement between MCNP and OpenMC. This result demonstrates the accuracy of OpenMC’s PHT feature for spectroscopic applications in which detector efficiency is a primary concern.

07 - ISOTOPES AND RADIATION SOURCES↗

Detector Calibration to Quantify Random Summing in HPGe Spectroscopy

While calibrating a High Purity Germanium (HPGe) Radiation Detector for Xenon-133 (133Xe) the process of random summing occurs which leads to excess counts in the 160.6keV peak from random summing of the 81keV photons at the 162keV energy. Multiple samples of 133Xe with varying levels of radioactivity were assayed to determine a relationship between the occurrence of random summing and the net area of the 160.6keV peak. When the calculated efficiencies in the 160.6keV peak were compared to the theoretical efficiency obtained from a multi-energy calibration at 160.6keV, the amount of random summing could be estimated as excess observed efficiency and correlated to the sample activity. While a trend is apparent in the data, the mechanisms that contribute to the trend are still being studied so the data can be accurately correlated.

07 ISOTOPE AND RADIATION SOURCES↗

Applications of HPGe-detected high energy gamma rays toward quantifying neutron emission rates and 234 U enrichment in UF 6 cylinders

This study presents a 234 U enrichment meter that uses high energy gamma and neutron count rate as measured by a portable, high-purity germanium gamma ray detector. Twenty-one 30B cylinders containing UF 6 of varying origin were analyzed with an HPGe detector for high-energy gamma ray and neutron counts. Excellent correlations (R 2 0.95) between various regions of 3.0 MeV gamma rays, neutron count rate, and uranium enrichment were found. These neutron and high-energy gamma data are used to create calibration-dependent enrichment meters for 234 U. The 234 U enrichment calculated from the neutron count rate and 4 – 6 MeV gamma count rate is more accurate than methods that rely on the 120.9 keV peak which is strongly attenuated inside commercial sized UF 6 cylinders. These neutron and high-energy gamma enrichment calculators can also be used to determine a 235 U enrichment, assuming mass-based enrichment from natural uranium, but the results are not as accurate as the traditional 185.7 keV peak enrichment meter.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Characterization of the First Prototype of the L1K65n Differential-Output Charge-Sensitive Preamplifier ASIC for High-Performance, Low-Background HPGe Detector Readout

Next-generation neutrinoless double-beta (0νββ) decay searches require a large detector/isotope mass and very low radioactive backgrounds. The upcoming LEGEND-1000 experiment (Large Enriched Germanium Experiment for Neutrinoless double-beta Decay) constitute a ton-scale array of several hundred high-purity germanium (HPGe) detectors enriched in 76Ge, the isotope of interest. It aims to reach a sensitivity beyond 10 28 years on the 0νββ decay half-life of 76Ge, necessitating an order of magnitude reduction in background with respect to the state of the art. This will require the implementation of a dedicated application specific integrated circuit (ASIC) preamplifier that will significantly lower background contribution compared to the conventional low-mass front end (LMFE) employed in the Majorana Demonstrator and LEGEND-200 experiments while maintaining or improving energy resolution and other performance parameters. Features include a high (9 MeV) dynamic range with noise low enough to achieve a trigger threshold of <1 keV, a single power supply to reduce background-inducing cabling, and a differential output to maintain signal integrity over several meters of transmission line. The chip would be optimized to operate in liquid argon (87 K) and be able to do so reliably for ten years. Following on from an earlier 180-nm prototype, we have developed a differential-output charge-sensitive preamplifier ASIC fabricated in a 65-nm process, 1×2 mm in size, that addresses these needs. Here, we present recent results from the successful testing and characterization of the first version of this device.

ASIC↗

$$\alpha $$-event characterization and rejection in point-contact HPGe detectors

Abstract P-type point contact (PPC) HPGe detectors are a leading technology for rare event searches due to their excellent energy resolution, low thresholds, and multi-site event rejection capabilities. We have characterized a PPC detector’s response to $$\alpha $$ α particles incident on the sensitive passivated and p $$^+$$ + surfaces, a previously poorly-understood source of background. The detector studied is identical to those in the Majorana Demonstrator experiment, a search for neutrinoless double-beta decay ( $$0\nu \beta \beta $$ 0 ν β β ) in $$^{76}$$ 76 Ge. $$\alpha $$ α decays on most of the passivated surface exhibit significant energy loss due to charge trapping, with waveforms exhibiting a delayed charge recovery (DCR) signature caused by the slow collection of a fraction of the trapped charge. The DCR is found to be complementary to existing methods of $$\alpha $$ α identification, reliably identifying $$\alpha $$ α background events on the passivated surface of the detector. We demonstrate effective rejection of all surface $$\alpha $$ α events (to within statistical uncertainty) with a loss of only 0.2% of bulk events by combining the DCR discriminator with previously-used methods. The DCR discriminator has been used to reduce the background rate in the $$0\nu \beta \beta $$ 0 ν β β region of interest window by an order of magnitude in the Majorana Demonstrator and will be used in the upcoming LEGEND-200 experiment.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Assessment of PHDS Fulcrum40h and Ortec Detective-X High Purity Germanium (HPGe) Detector System Performance

This report provides a summary of measurement results used to compare the performance of the PHDS Fulcrum40h and Ortec Detective-X High Purity Germanium (HPGe) detector systems. Specifically, the measurement data collected was used to assess each detector system for gamma efficiency and resolution, gamma angular response and efficiency for an in-situ surface distribution, neutron efficiency, gamma pulse-pileup response, and gamma to neutron crosstalk.

42 ENGINEERING↗

Application of Indirect Quantification of 133mXe to Calibration of HPGe Detector

The INL Noble Gas Laboratory provides intercomparison samples for the noble gas analysis laboratories as part of the CTBTO PrepCom IMS. Xe-133m is one of the four relevant radionuclides in nuclear explosion monitoring. Without commercially available Xe-133m calibration standards laboratories must create and improve calibration methods. Improvements in calibration methods at the INL NGL benefit the CTBTO PrepCom through better certified values for Xe-133m intercomparison samples. Calibration of High Purity Germanium detectors for Xe-133m quantification is complicated by the coexistence of Xe-133 in samples under analysis. Xe-133 is typically produced in larger quantities, has higher gamma emission probabilities, and its gammas are detected more efficiently than Xe-133m. Xe-133m activity of samples can be indirectly inferred through the 133:133m activity ratio of a batch of material, and the Xe-133 counts in the assay of a small aliquot of the same material. This indirect quantification method can be leveraged to perform detector calibrations for quantification of Xe-133m. Calibrations can be performed by inferring the Xe-133m to certify the sample, and direct counting to determine detector efficiency. A comparison of method results will be shown.

133mXe↗

Effects of magnetic fields on HPGe tracking detectors

Here, we present a study of magnetic fields effects on the position resolution and energy response of hyper-pure germanium detectors. Our results provide realistic estimates of the potential impact on the resolving power of tracking-arrays from (fringe) magnetic fields present when operating together with large spectrometers. By solving the equations of motion for the electron and holes in the presence of both electric and magnetic fields, we analyzed the drift trajectories of the charge carriers to determine the deviations in the positions at the end point of the trajectories, as well as changes in drift lengths affecting the energy resolution and peak shift due to trapping. Our results show that the major effect is in the deviation of the transverse (to the electric field direction) position and suggest that, if no corrective action is taken in the pulse-shape and tracking data analysis procedures, a field strength ≳ 0.1 T will start to impact the intrinsic position resolution of 2 mm (RMS). At fields above ~1 T, the degradation of the energy response becomes observable.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Machine Learning technique for isotopic determination of radioisotopes using HPGe γ-ray spectra

γ-ray spectroscopy is a quantitative, non-destructive technique that may be utilized for the identification and quantitative isotopic estimation of radionuclides. Traditional methods of isotopic determination have various challenges that contribute to statistical and systematic uncertainties in the estimated isotopics. Furthermore, these methods typically require numerous pre-processing steps, and have only been rigorously tested in laboratory settings with limited shielding. Here, in this work, we examine the application of a number of machine learning based regression algorithms as alternatives to conventional approaches for analyzing γ-ray spectroscopy data in the Emergency Response arena. This approach not only eliminates many steps in the analysis procedure, and therefore offers potential to reduce this source of systematic uncertainty, but is also shown to offer comparable performance to conventional approaches in the Emergency Response Application.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Cumulative fission yields of short-lived fission products from 235 U and 239 Pu measured by HPGe gamma-ray spectroscopy

In this study, we present a preliminary investigation focused on determining cumulative fission yields for short-lived fission products. Our analysis involves examining gamma spectra from the irradiated samples of 235 U and 239 Pu using the High Flux Isotope Reactor. The motivation stems from the observed discrepancy in the antineutrino energy spectrum within the range of 5 to 7 MeV. While several hypotheses have been proposed, a thorough analysis of fission yields provides an additional way of gaining insight into this unexplained phenomenon. Our study suggests that the measured gamma rays from 100 Nb, 140 Cs and 95 Sr are consistent with the expected values. However, 93 Rb, 96 Y, 97 Y and 142 Cs cannot be quantified due to insufficient statistics, interference from other gamma rays and the Compton scattering background. Additionally, the calculated cumulative fission yields based on the measured 140 Cs and 95 Sr are found to be consistent with the JEFF3.3 fission yield library. In conclusion, the present work shows that the potential of improving gamma-ray spectroscopy in the fission yields as a means to improve our understanding of the antineutrino spectrum.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Dense autoencoders, clustering techniques, and semi-supervised learning for HPGe $γ$-spectra

Classifying high-resolution gamma spectra by their isotopic content is an essential task in nuclear forensics and other applications. Traditional analysis methods are often time-intensive, but machine learning (ML) may help analysts quickly process many spectra. Such methods tend to rely on abundant, well-labeled data for training. Historical gamma data exists in various fields but is not uniformly useful for supervised ML due to inconsistent labeling. Here, to address some of these challenges, we present a method to classify and organize unlabeled data from high-purity germanium detectors using an autoencoding neural network (autoencoder). We trained dense autoencoders to compress gamma data into latent representations that enable efficient data characterization. By clustering the encoded spectra or lower-dimensional mappings of them, we identified and removed portions of over-abundant data categories, resulting in a more balanced dataset and improved autoencoder performance. This encoding and clustering pipeline also enabled the organization of spectra into self-consistent categories. Finally, we found that encoded representations showed potential as inputs for semi-supervised learning of nuclide identification (NID) labels, achieving an average F1 score of 0.85 ± 0.03 when mapping encodings to a set of 65 isotope labels.

Autoencoders↗

On the determination of iridium in diverse geological samples employing HPGe-coincidence/NaI(Tl)-anticoincidence spectrometry

This paper reports the Ir content of a variety of geological samples determined by the high-purity Ge-coincidence/NaI(Tl)-anticoincidence gamma-ray spectrometry (henceforth referred to as coincidence/anticoincidence technique) and by the conventional INAA. The advantages of this technique are: (1) the Ir content of the samples is obtained (ppm to a fraction of ppb ranges) not only by the 468.1 keV peak as in the conventional INAA but also by the 784.6 keV and 920.9 keV sum peaks, which gives more confidence in the values obtained; and (2) it is well suited for the samples with high Compton background for which it is difficult to measure the Ir content by the conventional INAA technique. The practical sensitivity of this technique depends on the sample matrix. Under present experimental conditions, it varied from 0.1 ng for Mn nodules and 0.004 ng for Libyan Desert Glass. Iridium values obtained on small (about 1 microg) olivine grains demonstrate the potential application of this new technique to microsamples. The principle and methodology of this new technique as well as its advantages and disadvantages over the conventional INAA are discussed.

Murali, A. V.↗