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DOE OSTI2021

Electrochemical Manipulation and Radiolytic Evaluation of Organic Phase Neptunium

Presentation for Seed LDRD proposal presentation: This Seed LDRD research proposes to test an innovative approach to precisely control the oxidation state distribution of neptunium (Np) under used nuclear fuel (UNF) reprocessing conditions using novel electrochemical methods. Current UNF reprocessing technologies are not financially viable in the US, requiring significant scientific and technological innovation to improve cost efficiency. Reducing the number of process cycles is one avenue for increasing cost efficiency, of which resolving the challenge associated with isolating Np is critical. Under envisioned process conditions, Np is present in a mixture of extractable (Np(IV) and Np(VI)) and inextractable (Np(V)) oxidation states, the distribution of which is dependent on several factors, including ionizing radiation dose, that change throughout a reprocessing scheme. Consequently, Np unintentionally partitions into various UNF reprocessing phases and product streams, ultimately increasing the number of process cycles to isolate UNF components. Here, we propose to employ novel, high surface area, optically transparent, Ligand Modified tin-doped indium oxide Electrodes (LMES). These LMEs bind Np, and therefore enable concurrent generation and spectroscopic characterization of Np oxidation states in organic solutions. These proof-of-concept experiments will: (i) facilitate optimization of the proposed electrochemical system conditions for Np oxidation state manipulation; (ii) identify the accessible electrochemical window for Np complexes in the organic phase; (iii) report characteristic optical spectra for each accessible complexed Np oxidation state; and (iv) determine the lifetime and partitioning of a given atypical Np oxidation state in the organic phase in the presence and absence of ionizing radiation fields. The data gathered by this Seed LDRD will provide support for the design of an electrochemical process concept for the precise manipulation of Np oxidation states in UNF reprocessing solvent systems, with the intention of providing advanced control over Np mass transfer, and thus greater process efficiency and economy.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2020

Report from the Inaugural Meeting on the Opportunities at the SEEMS Facility

An Inaugural Meeting on the Opportunities at the SEEMS Facility was held at the Spallation Neutron Source (SNS) on June 11 - 12, 2019. It focused on the second of the user communities - industrial and academic researchers. Indeed, the SEEMS design concept started with a Spallation Neutron Source (SNS) study conducted for the Federal Aviation Administration (FAA) that examines test facility options for providing neutron radiation simulating that in the atmosphere originating from cosmic rays and solar particles. The study was stimulated by earlier work calling for neutron radiation facilities with increased capacity and capabilities to meet current and future needs. Regulators, aircraft producers and avionics equipment suppliers recognize the growing urgent need for SEE testing in prototypical radiation fields. Industry standards formalizing procedures to assure that critical systems are robust against SEE phenomena have been issued. Regulatory bodies including the Federal Aviation Administration (FAA) and the European Union Aviation Safety Agency (EASA) now requiring that updated standards are met for aircraft certification.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2025

Radiation Characterization Summary: Godiva IV Critical Assembly Environments at the In-Core, Top Hat, 1m, and 2m Irradiation Locations

This document presents the facility-recommended characterization of the neutron, prompt gamma ray, and delayed gamma ray radiation fields at the Godiva IV critical assembly at the National Criticality Experiments Research Center (NCERC). The environments assessed include the In-Core location, a location on the Top Hat, 1m away from the assembly, and 2m away from the assembly. The neutron, prompt gamma ray, and delayed gamma ray energy spectra, uncertainties, and covariance matrices are presented as well as radial and axial neutron and gamma ray fluence profiles on the Top Hat surrounding the critical assembly. Recommended constants are given to facilitate the conversion of various dosimetry readings into radiation metrics desired by experimenters. Representative pulse operations are presented with conversion examples.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Shock wave formation in radiative plasmas

The temporal evolution of weak shocks in radiative media is theoretically investigated in this work. The structure of radiative shocks has traditionally been studied in a stationary framework. Their systematic classification is complex because layers of optically thick and thin regions alternate to form a radiatively-driven precursor and a temperature-relaxation layer, between which the hydrodynamic shock is embedded. In this work, we analyze the formation of weak shocks when two radiative plasmas with different pressures are put in contact. Applying a reductive perturbative method yields a Burgers-type equation that governs the temporal evolution of the perturbed variables including the radiation field. The conditions upon which optically thick and thin solutions exist have been derived and expressed as a function of the shock strength and Boltzmann number. Below a certain Boltzmann number threshold, weak shocks always become optically thick asymptotically in time, while thin solutions appear as transitory structures. The existence of an optically thin regime is related to the presence of an overdense layer in the compressed material. Scaling laws for the characteristic formation time and shock width are provided for each regime. The theoretical analysis is supported by FLASH simulations, and a comprehensive testcase has been designed to benchmark radiative hydrodynamic codes.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

CAAS-3S Radiation Testing for Y-12 and UPF with Godiva-IV

The Y-12 National Security Complex and the Uranium Processing Facility (UPF) selected the Mirion CAAS-3S as the Criticality Accident Alarm System for UPF and for Y-12 facilities replacing their legacy CAAS as part of efforts to extend the facility lifespans. As part of this process, the CAAS-3S system was exposed to a high radiation dose and dose rate during reactor testing with the Godiva-IV fast burst reactor. The reactor testing was designed around preliminary analyses that determined Y-12 and UPF requirements, and simulations of the radiation field within the reactor facility were used to determine reactor operating parameters, CAAS equipment locations, and the design of a neutron shield wall. This paper presents the design and results of the testing, and discusses how the test results were interpreted by criticality safety engineers at Y-12 and UPF.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Analyses of Dose Rates for Second Inner Reflector Plug Replacement at Spallation Neutron Source

The Inner Reflector Plug (IRP) is a central component of the Spallation Neutron Source (SNS) target monolith, which houses the liquid mercury target and four liter-sized neutron moderator units. It is exposed to high-level radiation fields during routine operation and builds up significant activity. The IRP needs to be replaced due to moderator neutron poison and decoupler burn-out, which is used for shaping neutron pulses. The first IRP exchange took place in March 2018 and next one, which is IRP2, is planned to be replaced during the facility maintenance period in the end of December 2025, beginning of January 2026 calendar year. The replacement of IRP is a complex task due to its location in the area receiving high irradiation, being under significant amount of shielding, and size, which requires removal in segments. For planning the replacement workflow to help to reduce radiation exposure to workers dose rates for each stage of extraction/replacement operation are predicted.

42 ENGINEERING↗

DOE OSTI2021

A fully kinetic model for orphan gamma-ray flares in blazars

ABSTRACT Blazars emit a highly variable non-thermal spectrum. It is usually assumed that the same non-thermal electrons are responsible for the IR-optical-UV emission (via synchrotron) and the gamma-ray emission (via inverse Compton). Hence, the light curves in the two bands should be correlated. Orphan gamma-ray flares (i.e. lacking a luminous low-frequency counterpart) challenge our theoretical understanding of blazars. By means of large-scale two-dimensional radiative particle-in-cell simulations, we show that orphan gamma-ray flares may be a self-consistent by-product of particle energization in turbulent magnetically dominated pair plasmas. The energized particles produce the gamma-ray flare by inverse Compton scattering an external radiation field, while the synchrotron luminosity is heavily suppressed since the particles are accelerated nearly along the direction of the local magnetic field. The ratio of inverse Compton to synchrotron luminosity is sensitive to the initial strength of turbulent fluctuations (a larger degree of turbulent fluctuations weakens the anisotropy of the energized particles, thus increasing the synchrotron luminosity). Our results show that the anisotropy of the non-thermal particle population is key to modelling the blazar emission.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

Angular-spatial hp -adaptivity for radiative transfer with discontinuous Galerkin spectral element methods

Radiative transfer is important for many science and engineering applications, and numerical simulations of radiative transfer can be challenging. For instance, the radiation field is seven-dimensional – three spatial, two angular, one wavelength, and one temporal – and often features steep gradients. Therefore, memory usage is a key issue. To reduce memory, some past work has investigated the use of adaptive mesh refinement (AMR), typically for either the spatial or angular coordinate, and typically for only h -adaptivity. Here, we propose the use of AMR for the spatial and angular coordinates together, and the use of h - and p -adaptivity together as hp -AMR for the potential for further memory savings. We implemented the proposed method for several test cases in two spatial and one angular dimension, with the discontinuous Galerkin spectral element method. These test cases featured highly anisotropic angular radiation, with or without steep spatial gradients. Our primary findings from these test cases were: (1) Angular hp -adaptivity can deliver the radiation solution with the same accuracy as, and with much less computational memory than, uniform angular h - or p -refinements, or angular h -adaptivity alone. This is most obvious when the incoming radiation is highly anisotropic, in which case the savings can be orders of magnitude. (2) Full spatial-angular hp -adaptivity is more efficient in solution representation, compared to solely spatial or solely angular -adaptivity. This is most evident when steep gradients are present in both the spatial and angular distribution. These results suggest that adaptive spatial- hp angular-refinement may perform well in large-scale seven-dimensional applications.

Adaptive refinement↗

DOE OSTI2026

Impact of Nd ions on the chemical kinetic behavior of radiolytic transients in molten LiCl-KCl-NdCl3 salt mixtures

Pyrochemical reprocessing technologies can be used to recover valuable materials from used nuclear fuel (UNF), such as uranium. However, other critical materials, such as fission product neodymium, are challenging to recover from molten chloride eutectic mixtures (LiCl-KCl) due to the presence of multivalent states (Nd2+/Nd3+), disproportionation reactions, and re-dissolution in the molten chloride salt. Understanding, predicting, and controlling these processes is further complicated by the presence of ionizing radiation fields, for which little is known on the interaction of neodymium ions with the radiolytic transients (es– and Cl2.–) in molten LiCl-KCl salt mixtures. Here, chemical kinetics, from integrated electron pulse irradiation and transient absorption spectroscopy, are presented for the reaction of Nd3+ ions with es– and Cl2.– as a function of temperature (400–600 ?).

36 - MATERIALS SCIENCE↗

DOE OSTI2021

Gamma Radiolysis of Biphasic Acetohydroxamic Acid (AHA) Solvent Systems

Acetohydroxamic acid (AHA) has been proposed as a substitute for uranium(IV) and hydrazine as a plutonium complexant and neptunium reductant for simplified, single-cycle used nuclear fuel reprocessing flowsheets. However, the chemical behavior of AHA in an intense multi-component radiation field is poorly understood, especially under representative biphasic reprocessing solvent system conditions. In response to this critical knowledge gap, this study has investigated the gamma radiolytic integrity of AHA in aqueous nitric solutions in contact with an organic phase, comprising current and future reprocessing ligands (TBP, DEHBA, and DEHiBA) dissolved in n-dodecane diluent. Our data show negligible effect of the organic phase on the radiolytic behavior of AHA compared to complementary single-phase experiments.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2021

Radiolytic evaluation of acetohydroxamic acid (AHA) under biphasic (n-dodecane and TBP/DEHBA/DEHiBA) used nuclear fuel reprocessing conditions

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2023

Lyman continuum leaker candidates among highly ionised, low-redshift dwarf galaxies selected from He II

Contemporary research suggests that the reionisation of the intergalactic medium (IGM) in the early Universe was predominantly realised by star-forming (proto-)galaxies (SFGs). Due to observational constraints, our knowledge on the origins of sufficient amounts of ionising Lyman continuum (LyC) photons and the mechanisms facilitating their transport into the IGM remains sparse. Recent efforts have thus focussed on the study of local analogues to these high-redshift objects. We aim to acquire a set of very low-redshift SFGs that exhibit signs of a hard radiation field being present. A subsequent analysis of their emission line properties is intended to shed light on how the conditions prevalent in these objects compare to those predicted to be present in early SFGs that are thought to be LyC emitters (LCEs). We used archival spectroscopic SDSS DR12 data to select a sample of low-redshift He II 4686 emitters and restricted it to a set of SFGs with an emission line diagnostic sensitive to the presence of an active galactic nucleus, which serves as our only selection criterion. We performed a population spectral synthesis with FADO to reconstruct these galaxies’ star-formation histories (SFHs). Utilising the spectroscopic information at hand, we constrained the predominant ionisation mechanisms in these galaxies and inferred information on interstellar medium (ISM) conditions relevant for the escape of LyC radiation. Our final sample consists of eighteen ionised, metal-poor galaxies (IMPs). These low-mass (6.2 ≤ log(M * /M ⊙ ) ≤ 8.8), low-metallicity (7.54 ≤log(O/H) + 12 ≤ 8.13) dwarf galaxies appear to be predominantly ionised by stellar sources. We find large [OIII] 5007/[OII] 3727 ratios and [SII] 6717,6731/Hα deficiencies, which provide strong indications for these galaxies to be LCEs. At least 40% of these objects are candidates for featuring cosmologically significant LyC escape fractions ≳10%. The IMPs’ SFHs exhibit strong similarities and almost all galaxies appear to contain an old (> 1 Gyr) stellar component, while also harbouring a young, two-stage (~10 Myr and < 1 Myr) starburst, which we speculate might be related to LyC escape. The properties of the compact emission line galaxies presented here align well with those observed in many local LCEs. In fact, our sample may prove as an extension to the rather small catalogue of local LCEs, as the extreme ISM conditions we find are assumed to facilitate LyC leakage. Notably, all of our eighteen candidates are significantly closer (z < 0.1) than most established LCEs. If the inferred LyC photon loss is genuine, this demonstrates that selecting SFGs from He II 4686 is a powerful selection criterion in the search for LCEs.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

Indium Tin-Doped Oxide Interactions with Solvent Radiolysis Products

Transparent conductive oxides (TCOs), such as indium tin-doped oxide (ITO), are ubiquitous as components of electronics and are ideal electrode substrates for catalysis, energy transformation reactions, and energy storage applications. Recently, researchers have recognized their effectiveness as electrode materials for manipulating actinide oxidation states in solution. Despite their popularity as electrode materials, prior studies focused extensively on the direct radiolysis of TCO materials in air and rarely examined these effects within a solution, limiting our fundamental understanding of the interactions between solvent radiolysis products and these substrates in high radiation environments. Here, in this study, we characterize the effects of solvent radiolysis products—arising from the gamma irradiation of water, aqueous nitric acid solutions, and n-dodecane—on the composition, surface speciation, and band structure of ITO thin films on a glass substrate as a function of absorbed dose using UV-visible spectroscopy, scanning electron microscopy, photoelectrochemistry, and X-ray photoelectron spectroscopy. Our work demonstrates that mesoporous thin film electrodes of ITO exposed to gamma radiation in each solvent accumulate defects and exhibit solvent and dose dependent changes to their surface and interfacial properties. These electrodes maintain their electrochemical function and improve their photoelectrochemical performance up to at least 100 kGy of accumulated gamma dose, confirming their utility in solvents exposed to ionizing radiation fields.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2025

A Behavioral Robotics Approach to Radiation Mapping Using Adaptive Sampling

Radiation mapping is a desirable task to automate because of the inherent risks involved and its tedious nature. A novel system was designed to address this by combining various existing technologies, utilizing behavior-based robotics and Bayesian optimization. The system uses a quadruped robot equipped with a manipulator and gamma detector to take measurements at locations that are selected based on the uncertainty of a surrogate model used to estimate the true radiation field. The robot uses input from the world with depth cameras to avoid collisions with the robot’s body, and unreachable points for the end effector are addressed by both allowing for a soft collision with the environment to occur, prompting the system to abandon that point, and varying the exploration tendency of the optimization based on consecutive collisions. This approach provides unique traversability and adaptability over other strategies in the literature. Experiments were performed by placing a Cesium-137 source on the ground and varying geometric setups and an optimization parameter demonstrating the adaptability to diverse environments and the increased robustness resulting from the designed behavior. The results additionally demonstrate that dynamically adjusting the optimization algorithm’s exploration tendency based on the arm’s collision history improves the system’s ability to navigate cluttered environments and construct accurate radiation maps without getting stuck in unreachable areas.

Adams, Joel↗

DOE OSTI2020

Irradiation Assessment of a Lightweight Industrial Robot - Towards Faster, Safer and Sooner Waste Decommissioning - 20317

Robotic systems have been successfully applied in the nuclear industry for several decades as a safe approach to minimize the exposure dose of human operators. As nuclear waste management and decommissioning gathers pace, there is an emerging interest integrating modern off-the-shelf industrial robots in nuclear robotic systems which make use of complex electronics and software to improve functionality over traditional machines. The use of the industrial robots will significantly increase the pace of development of automated waste management systems at a reduced cost, and although these off-the-shelf robots are proven robust in typical industrial environments, performance in radioactive environments is less clear. This paper investigates the performance degradation of a lightweight industrial robot (KUKA iiwa 7 LBR 800) in a controlled radiation field, aiming to simulate conditions in highly radioactive nuclear waste handling facilities. The degradation of the industrial robot's performance is identified while measuring the air kerma dose-tolerance of sensitive components, via a systematic experimental methodology. The experience from this experiment has demonstrated the significant capabilities of industrial robots, which tolerated a large gamma dose of 164 Gy before a system failure. Future tests are planned, aiming to enable faster, safer and sooner waste management and decommissioning using complex robotic systems. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2021

A Multiwavelength Look at the GJ 9827 System: No Evidence of Extended Atmospheres in GJ 9827b and d from HST and CARMENES Data

GJ 9827 is a bright star hosting a planetary system with three transiting planets. As a multiplanet system with planets that sprawl within the boundaries of the radius gap between terrestrial and gaseous planets, GJ 9827 is an optimal target to study the evolution of the atmospheres of close-in planets with a common evolutionary history and their dependence from stellar irradiation. Here we report on the Hubble Space Telescope (HST) and CARMENES transit observations of GJ 9827 planets b and d. We performed a stellar and ISM characterization from the ultraviolet HST spectra, obtaining fluxes for Lyα and Mg ii of F(Lyα) = (5.42{sub −0.75}{sup +0.96}) × 10{sup −13} erg cm{sup −2} s{sup −1} and F(Mgii) = (5.64 ± 0.24) × 10{sup −14} erg cm{sup −2} s{sup −1}. We also investigated a possible absorption signature in Lyα in the atmosphere of GJ 9827b during a transit event from HST spectra, as well as Hα and He i signature for the atmosphere of GJ 9827b and d from CARMENES spectra. We found no evidence of an extended atmosphere in either of the planets. This result is also supported by our analytical estimations of mass loss based on the measured radiation fields for all three planets of this system, which led to a mass-loss rate of 0.4, 0.3, and 0.1 planetary masses per Gyr for GJ 9827b, c, and d, respectively. These values indicate that the planets could have lost their volatiles quickly in their evolution and probably do not retain an atmosphere at the current stage.

47 OTHER INSTRUMENTATION↗

DOE OSTI2026

A non-intrusive framework using acoustic signals and deep learning for boiling diagnostics in visual-limited environments

Accurate monitoring of boiling heat transfer is critical for safeguarding high-power systems operating in environments where conventional optical diagnostics are hindered by radiation fields or restricted visual accessibility. This study presents a non-intrusive framework that integrates hydroacoustic sensing with deep learning to infer near-wall boiling characteristics and enable predictive thermal assessment without visual access. In a prototypical subcooled flow-boiling facility representative of the Isotope Production Facility (IPF) at Los Alamos, hydrophones capture boiling-induced acoustic emissions that are transformed into background-removed Short-Time Fourier Transform (STFT) spectrograms. A convolutional neural network (CNN) then regresses heat flux, wall superheat, and key bubble parameters directly from these spectrograms. The CNN achieved predictive accuracy under nominal conditions and demonstrated robustness and generalization under acoustic noise for Signal-to-Noise Ratios (SNRs) down to approximately 0 dB. When integrated into an ANSYS CFX wall-boiling model, the acoustically inferred parameters reproduced boiling curve and critical heat flux (CHF) values consistent with image-based benchmarks. Furthermore, the model retained reliable performance under moderate variations in bulk temperature, flow rate, and hydrophone placement, confirming its generalizability across practical boundary conditions. These results demonstrate the feasibility of hydroacoustic-based deep learning as a viable path toward real-time, radiation-tolerant boiling diagnostics and predictive thermal safety assessment in inaccessible systems such as the IPF.

42 ENGINEERING↗

DOE OSTI2026

Comparison of the performance of TLD, OSL and RPL personal dosimetry systems to the American National Standard Institute (ANSI) test categories

The Laboratory Accreditation Program (LAP) tests the capability and performance of the United States Department of Energy's (USDOE) facilities to accurately measure and quantify the whole-body and extremity radiation equivalent doses to the occupational workers. The dosimetry methods used in personal dosimetry can be Thermoluminescence (TL), Optically Stimulated Luminescence (OSL) and Radiophotoluminescence (RPL), among other techniques available. Currently, the TL (LiF:Mg,Ti) and OSL (Al 2 O 3 :C) dosimetry systems are DOELAP-accredited for occupational dose measurements and regulatory reporting. In this study, the performance of a beryllium oxide (BeO) OSL dosimetry system and of a silver-doped phosphate glass RPL dosimetry system is compared against the performance of an accredited LiF:Mg,Ti TL dosimetry system. The bias and standard deviation in each of the performance test categories are compared between these three systems for exposures to photons, beta, and mixed radiation fields with the criteria established by the American National Standard Institute (ANSI) and Health Physics Society (HPS) N13.11-2022 standard. The practical implementation of the dosimetry program and its equivalency to the occupational personal equivalent dose H p (0.07) and H p (10) measurements were evaluated. The TL, OSL and RPL dosimetry systems passed the ANSI performance test criteria for H p (0.07) and H p (10) occupational dose measurements and met the DOELAP accreditation requirements.

61 RADIATION PROTECTION AND DOSIMETRY↗