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DOE OSTI2025

A Fast Framework for Generating Radioactive Mixture Spectra and Its Application to Remote High-Performance Mixture Identification

Remote detection of radioactive materials in mixtures using handheld or portal detectors remains a challenge because of factors such as low concentration, environmental interference, sensor noise, and other complications. This work introduces a fast framework for generating realistic mixture spectra. Moreover, we present mixture isotope identification using data generated by the fast framework. Researchers have examined a range of conventional and recent algorithms within the fields of machine learning and deep learning. An application to uranium enrichment-level prediction has been included. Extensive simulation experiments validated the efficacy of the proposed framework.

GADRAS↗

DOE OSTI2020

MRDIS Case Study

The Mobile Radiation Detection and Identification System (MRDIS) is a large mobile scanner that inspects containers in transit from cargo ships for radiological materials. The MRDIS platform operates as a two-part system with one MRDIS using a plastic Polyvinyl Toleune (synthetic polymer) for primary detection and another MRDIS that uses spectroscopic detectors for secondary isotopic identification. MRDIS can operate either independently or as part of a team, depending on the needs of the port. MRDIS is controlled by a human operator, who searches the computer monitor for any traces of radiological materials when the containers pass through the center of the system. Each MRDIS can also feed data into a central system or collect data on its own for additional material analysis. The system integrates radiation detection, radioisotope identification, an optical character recognition system, occupancy/speed sensors, wireless communications, and data processing capabilities to discern what specific radiological materials are of particular interest. In addition, Sandia engineers created a detailed set of requirements for subsequent models, allowing for faster implementation of additional detection systems.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Application of SAMMY for Non-Destructive Characterization of Irradiated Samples Using Neutron Transmission Measurements at VENUS

This report presents the application of SAMMY (Larson 2008), an R-matrix Bayesian fitting system, for analyzing neutron transmission data to enable non-destructive isotopic identification. Transmission measurements were conducted at the VENUS (Bilheux et al. 2023) beamline of the Spallation Neutron Source (SNS) using samples with unknown or partially characterized compositions. Through the application of SAMMY’s R-matrix Bayesian fitting capabilities to the measured transmission spectra and comparison against evaluated nuclear data libraries, isotopic constituents can be quantitatively determined based on their characteristic neutron resonance signatures. This methodology demonstrates significant potential for applications in nuclear safeguards, forensics, and post-irradiation examination.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Uranium measurements in the field using high-resolution cadmium zinc telluride detectors

A new generation of cadmium zinc telluride (CZT) detectors has become available and is being evaluated by the International Atomic Energy Agency (IAEA) for safeguards verifications in the field. The new CZT detector, model M400, is a room temperature spectrometer manufactured by H3D, Inc. The M400 demonstrates superior energy resolution, effective isotope identification capabilities, and convenient usability features when tested in a controlled laboratory environment. These characteristics define the M400 as a potential platform for IAEA field detection applications, which could become suitable for nuclear material characterization (e.g., enrichment verification) and nuclear safeguards missions. The capabilities of gamma spectrometry codes including Fixed energy, Response function Analysis with Multiple efficiencies (FRAM) from Los Alamos National Laboratory, CZT for Uranium (CZTU) from Lawrence Livermore National Laboratory, and Gamma Detector Response and Analysis Software (GADRAS) from Sandia National Laboratories were adapted for M400 spectra, and the performance of the codes has been validated. This was reported in a prior work. To further validate the performance of the high-energy resolution CZT detector and the isotopic analysis codes, a field measurement campaign consisting of uranium hexafluoride (UF 6 ) cylinder measurements was conducted at a fuel fabrication facility. A total of 34 Type 30B cylinders containing UF6 were measured using three different M400 CZT detectors. Each detector was outfitted with a custom rectangular collimator and shield made out T-Flex®, a tungsten-impregnated polymer. Measurements were performed at three different locations of the cylinder, ensuring that the measurement geometry satisfied the infinite thickness criterion. The spectra from the M400 CZT were analyzed using the code General Enrichment Meter (GEM). For analyzing the gamma-ray spectra from UF 6 cylinder, the GEM code is the appropriate tool since it relies only on the gamma-ray emissions from 235 U and not from other isotopes. Results from the spectral analysis were compared with the known abundance of 235 U in the cylinders, as well as with the International Target Values 2020 (ITV2020). The suitability of the different underlying techniques used by the various codes for UF 6 analysis is discussed. The challenges of measuring UF 6 contained in cylinders and mitigation strategies are highlighted.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2020

Discriminating Uranium Isotopes Based on Fission Signatures Induced by Delayed Neutrons

The use of active interrogation to induce delayed neutron emission is a well-established technique for the characterization of special nuclear materials. Delayed neutrons have isotope-characteristic spectral and temporal signatures, which provide the basis for isotope identification. However, in bulk materials that contain an appreciable fissile (e.g., 235 U or 233 U) fraction, such as highly enriched uranium (HEU), delayed neutrons have a high probability of inducing additional fissions. As a result, the overall delayed neutron signature consists of two distinct components: the “primary” delayed neutrons (emitted directly by fission fragments) and the “secondary prompt” fission neutrons produced in fission induced by primary delayed neutrons. These prompt products differ from “primary” delayed neutrons both in their energy spectra and in the presence of coincident radiation released by the parent fission event. The presence and relative quantity of prompt products from delayed fission depend on the cross section of the material in the energy range of delayed neutrons, which may differ significantly between isotopes, thus providing an exploitable means for isotope differentiation. Here, we demonstrate two experimental approaches for discriminating between 235 U and 238 U isotopes based on the measurement of delayed neutron-induced fission products. First, HEU and depleted uranium objects are differentiated through the detection of high-energy prompt neutrons from delayed fission using both recoil-based organic liquid scintillators and thermalization spectra from a custom-built capture-gated composite detector. Secondly, coincident radiation measurements are used as the basis for discrimination by comparing the overall rates and time evolution of fission events when delayed neutrons are present.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2025

Characterization of the Multi-Coincident Bismuth Germanate Oxide Spectrometer at the Nuclear Counting Facility

A multi-detector γ-ray spectroscopy system including 3 high-purity germanium (HPGe) detectors has been developed at the Nuclear Counting Facility at Lawrence Livermore National Laboratory. This system operates not only in conventional singles γ-ray detection mode but also incorporates features like coincidence and anti-coincidence techniques. These advanced detection modes can significantly enhance the system’s sensitivity, making it a powerful tool for isotope identification and quantification, especially for complex samples with high background and overlapping peaks. In this re port, we present a comprehensive performance characterization of the Multi-Coincident Bismuth Oxide Spectrometer (MCBOS) using a variety of sample types, including 60 Co, 48 Sc, and mixed fission product samples. Each sample provides unique tests for the MCBOS capabilities. Additionally, a GEANT4 model of the MCBOS has been generated to aid with the characterization of the system.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

A decay database of coincident γ–γ and γ–X -ray branching ratios for in-field spectroscopy applications

Current fieldable spectroscopy techniques often use single detector systems heavily impacted by interferences from intense background radiation fields. These effects result in low-confidence measurements that can lead to misinterpretation of the collected spectrum. To help improve interpretation of the fission products and short-lived radionuclides produced in a composite sample, a coincidence-database is being developed in support of a robust portable and X-ray coincidence detector system concurrently under development at the Pacific Northwest National Laboratory for in-field deployment. Hitherto, no database exists containing coincident γ–γ and γ–X-ray branching-ratio intensities on an absolute scale that will greatly enhance isotopic identification for in-field applications. As part of this project, software has been developed to parse all radioactive-decay data sets from the Evaluated Nuclear Structure Data File (ENSDF) archive to enable translation into a more useful JavaScript Object Notation (JSON) formats that more readily supports query-based data manipulation. The coincident database described in this work is the first of its kind and contains coincidence γ–γ and γ–X-ray intensities and their corresponding uncertainties, together with auxiliary metadata associated with each decay data set. The new JSON format provides a convenient and portable means of data storage that can be imported into analysis frameworks with relatively low overhead allowing for meaningful comparison with measured data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2026

A Coincident CdTe Detector Array for Enhanced Nuclear Process Monitoring

Nuclear fuel cycle aqueous separation processes desire improved real-time material characterization and process monitoring techniques; gamma coincidence spectroscopy has the potential to meet this need in these high throughput and high radiation environments based on its ability to reduce background noise, thereby enhancing detection limits and improving isotopic identification accuracy. A detector array composed of three CdTe detectors was designed to surround a chemical processing pipe in a reprocessing facility and evaluate the feasibility of passively assaying the nuclear materials flowing though this measurement point. This array uses commercial off the shelf components that are radiation hard and highly efficiency at low energies relevant to actinide photon signatures. Detector efficiency characterizations, coincidence detection, and potential configuration improvements are presented here.

Good, Erin C.↗

DOE OSTI2020

Nuclear Data Sheets for A=190

The evaluated experimental data are presented and evaluated for 15 known nuclides of mass 190 (Hf, Ta, W, Re, Os, Ir, Pt, Au, Hg, Tl, Pb, Bi, Po). This work supersedes earlier full evaluations of A=190 by 2003Si05, 1990Si09, 1982Le22 and 1973Sc42. For 190Hf, only the isotopic identification has been made, with no information about the half-life of the ground state or its decay properties. For 190 Ta, only one excited state as an isomer has been identified, but with no knowledge about its decay properties. For 190 W, 190 Re, 190 Bi and 190 Po, available spectroscopic data are scarce. Here, the decay schemes of 190 Ta, 190 W, 190 Au, 190 Hg, 190 Au isomer decay, 190 Tl (both the activities), 190 Pb, and 190 Bi (both the activities) are considered incomplete by the evaluators. At present, extensive level structures, both the low-spin and high-spin, are known for 190 Os, 190 Ir, 190 Pt, 190 Au, 190 Hg, 190 Tl and 190 Pb, but data for level lifetimes, and γ-ray transition probabilities are generally lacking.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

Nuclear Structure and Decay Data for A=149 Isobars

Here, experimental nuclear structure and decay data are evaluated for all the 17 known nuclides of mass 149 (Xe, Cs, Ba, La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb). Detailed compiled and evaluated spectroscopic information is presented for each reaction and decay dataset, and recommended values are provided for level properties, α, β and γ radiations, and other spectroscopic parameters, based on an evaluation of all the available experimental data for A=149 isobaric nuclides. Although large amounts of nuclear spectroscopic data are available for nuclides of A=149, yet large gaps in knowledge exist, as described below. For the lowest atomic number nuclide 149 Xe, only the isotopic identification has been made, with no data for its ground-state half-life. For 149 Cs, 149 Tm and 149 Yb information is available for only the respective ground states. For 149 Ba, 149 La and 149 Er, limited data exist for excited states. Many of the decay schemes of radioactive nuclei of A=149 are considered as incomplete, either due to large energy differences between the highest observed excited states in daughter nuclides and the respective Q-values, or due to the lack of confirmed γ-ray data, as listed below: 149 Cs → 149 Ba, 149 Ba → 149 La, 149 La → 149 Ce, 149 Ce → 149 Pr, 149 Pr → 149 Nd, 149 Tb(4.17 min) → 149 Gd, 149 Ho(21.0 s and 56 s) → 149 Dy, 149 Er(4 s and 9.6 s) → 149 Ho, and 149 Tm → 149 Er. No data exist for the decay of 149 Yb to 149 Tm. Data for half-lives of the excited states in this mass chain are generally lacking as given below by the number of excited levels of known half-life / approximate number of known levels in a nuclide: 2/17 for 149 Ba, 0/18 for 149 La, 3/53 for 149 Ce, 3/44 for 149 Pr, 17/110 for 149 Nd, 9/90 for 149 Pm, 10/210 for 149 Sm, 2/125 for 149 Eu, 6/270 for 149 Gd, 5/200 for 149 Tb, 3/80 for 149 Dy, 3/90 for 149 Ho, and 3/14 for 149 Er. This work supersedes earlier evaluations of A=149 nuclides published by 2004Si16, 1994Si18, 1985Sz01 and 1976Ho17.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2026

Stable and tunable MeV $$\gamma$$-ray generation via dual-laser inverse Thomson scattering from a laser-plasma accelerator

Abstract Inverse Thomson scattering from laser-plasma accelerators offers a pathway to compact, tunable MeV $$\gamma$$ -ray sources for reduced-dose radiography and enhanced performance in nuclear resonance fluorescence (NRF)-based isotope identification. However, photon yield and spectral quality are often limited by constraints on interaction geometry and scatter-laser tunability. Here we demonstrate a MeV $$\gamma$$ -ray source based on a dual-laser inverse Thomson scattering configuration driven by a 100-TW laser-plasma accelerator. Electron beams tunable from 122 to 204 MeV with $$<5$$ mrad divergence and $$<1$$ mrad pointing stability generate $$\gamma$$ rays with peak energies from 276 keV to 1.2 MeV and yields up to $$2\times 10^{7}$$ photons per shot. By independently controlling the interaction position and the scatter-pulse duration, we experimentally match the scatter pulse to the walk-off-limited interaction length. Extending the scatter pulse to 200 fs increases photon production by approximately $$15\%$$ while maintaining operation in the linear Thomson regime, thereby preserving narrow spectral bandwidth and controlled radiation divergence. Radiographic characterization demonstrates MeV-level penetration and $$\approx 0.1$$ mm spatial resolution, while stable operation is sustained over multi-hour timescales across multiple days. These results show that interaction-length optimization provides a scalable strategy for improving photon yield, spectral control, and operational stability in compact laser-plasma-accelerator-driven $$\gamma$$ -ray sources.

Tsai, Hai-En↗

DOE OSTI2021

InterSpec v. 1.0.8

SAND2021-4823 O InterSpec decodes and displays gamma radiation data from a variety of handheld, laboratory, and fixed installation detector types. Once loaded, InterSpec provides a means to interactively analyze the data via a peak-based methodology. InterSpec assists with isotope identification and determines the source strength and shielding characteristics of the measured item. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525.

Johnson, William↗

DOE OSTI2021

InterSpec v. 1.0.9

Johnson, William↗

DOE OSTI2020

Nuclear Interdiction Through Relocatable Detectors

The NNSA Office of Nuclear Smuggling Detection and Deterrence (NSDD) has investigated a set of minimal-infrastructure radiation detection systems as alternatives to fixed Radiation Portal Monitors (RPMs) for nuclear interdiction applications. These versatile and relocatable systems can improve nuclear security in missions or locations that do not warrant or support a standard fixed radiation detection system. Over 2019, a variety of relocatable detectors were characterized at the Interdiction Technologies Integration Laboratory at Pacific Northwest National Laboratory (PNNL). Evaluated detectors were diverse in their size and capabilities, ranging from backpack-sized systems to lane-spanning cargo scanning portals. Both spectroscopic and non-spectroscopic pedestrian and vehicle detection systems were characterized against uranium and plutonium sources. Signatures from the sources were modulated by both shielding and distance to quantify the performance of the relocatable systems as signal strength was decreased. Findings showed that relocatable spectroscopic detectors with isotope identification capabilities could reduce nuisance alarm rates compared to conventional fixed installation, gross-counting, radiation portal monitors. In vehicle scanning applications, detection ability generally trended with detection volume, regardless of spectral capability. In pedestrian scanning applications, several smaller backpack-sized detector systems were found to be more sensitive to detecting material than pedestrian portal monitors. The results of this characterization effort have helped inform the deployment of versatile equipment to improve nuclear security missions.

relocatable detectors, Nuclear Security↗

DOE OSTI2021

Surface Functionalization of Black Phosphorus with Nitrenes: Identification of P=N Bonds Using Isotopic Labeling

Abstract: Surface functionalization of two-dimensional crystals is a key path to tuning their intrinsic physical and chemical properties. However, synthetic protocols and experimental strategies to directly probe chemical bonding in modified surfaces are scarce. Introduced here is a mild, surface-specific protocol for the surface functionalization of few-layer black phosphorus nanosheets using a family of photolytically generated nitrenes (RN) from the corresponding azides. By embedding spectroscopic tags in the organic backbone, a multitude of characterization techniques are employed to investigate in detail the chemical structure of the modified nanosheets, including vibrational (infrared, Raman), Xray (emission, photoelectron), CPMAS NMR, and UV-vis spectroscopy. To directly probe the functional groups introduced on the surface, R fragments were selected such that in conjunction with vibrational spectroscopy, 15N-labeling experiments, and DFT methods, diagnostic P=N vibrational modes indicative of iminophosphorane units on the nanosheet surface could be conclusively identified.

Walz, Kendall↗

DOE OSTI2020

Identification of the New Isotope 244 Md

In an experiment performed at Lawrence Berkeley National Laboratory’s 88-inch cyclotron, the isotope Md 244 was produced in the Bi 209 ( Ar 40 , 5 n ) reaction. Decay properties of Md 244 were measured at the focal plane of the Berkeley Gas-filled Separator, and the mass number assignment of A = 244 was confirmed with the apparatus for the identification of nuclide A . The isotope Md 244 is reported to have one, possibly two, α -decaying states with α energies of 8.66(2) and 8.31(2) MeV and half-lives of 0.4 – 0.1 + 0.4 and ~ 6 s , respectively. Furtermore, first evidence of the α decay of Bk 236 was observed and is reported.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2024

Isotopic gamma lines for identification of shielding materials

Identifying the constituting materials of concealed objects is crucial in a wide range of sectors, such as medical imaging, geophysics, nonproliferation, national security investigations, and so on. Existing methods face limitations, particularly when multiple materials are involved or when there are challenges posed by scattered radiation and large areal mass. Here we introduce a novel brute-force statistical approach for material identification using high spectral resolution detectors, such as HPGe. The method relies upon updated semianalytic formulae for computing uncollided flux from source of gamma radiation, shielded by a sequence of nested spherical or cylindrical materials. These semianalytical formulae make possible rapid flux estimation for material characterization via combinatorial search through all possible combinations of materials, using a high-resolution HPGe counting detector. An important prerequisite for the method is that the geometry of the objects is known (for example, from X-ray radiography). We demonstrate the viability of this material characterization technique in several use cases with both simulated and experimental data in spherical geometry.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

DOE OSTI2022

First experiment at the Super Heavy Element Factory: High cross section of Mc 288 in the Am 243 + Ca 48 reaction and identification of the new isotope Lr 264

Here, we present results of the first experiment aimed at the synthesis of Mc isotopes in the 243 Am+ 48 Ca reaction performed at the new gas-filled separator DGFRS-2 online to the new cyclotron DC280 at the Super Heavy Element Factory at JINR. Fifty-five new decay chains of 288 Mc and six chains assigned to 289 Mc were detected. The α decay of 268 Db with an energy of 7.6–8.0 MeV, half-life of 16$^{+6}_{-4}$h, and a branch of 55$^{+20}_{-15}$% was registered for the first time, and a new spontaneously fissioning isotope 264 Lr with a half-life of 4.9$^{+2.1}_{-1.3}$h was identified. The cross section for the 243 Am( 48 Ca,3n) 288 Mc reaction was measured to be 17.1$^{+6.3}_{-4.7}$ pb, which is the largest value for the known superheavy nuclei at the island of stability.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗