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DOE OSTI2020

Radiological Recovery Logistics Tool - 20161

Argonne is building and testing a tool, the Radiological Recovery Logistics Tool (RRLT), that can be used during the response and recovery from a radiological or nuclear incident to effectively allocate appropriate commercial and public works equipment to mitigate, remove, and contain radiological contamination. The requirements for this tool - as well as development of the resulting software - is overseen by a steering committee of stakeholders from DHS's National Urban Security Technology Laboratory (NUSTL), the Federal Emergency Management Agency (FEMA), and the Environmental Protection Agency (EPA). One essential requirement is for RRLT to support the efficient and appropriate allocation of resources for a radiological response. Subsequent discussions between ANL and stakeholders have solidified the nature of this support to include identification of the types of resources to be allocated. The study reported in this paper has both factored fundamental concepts and connections out of this identification process and created a Knowledge Base detailing support goals, response scenarios, and efficacy information on dozens of equipment types. In short, RRLT will dynamically apply these findings to situational conditions surrounding contamination incidents. RRLT's Domain, the model of elements, ideas and relationships with which the tool will work, draws concepts from technical reports and stakeholder vocabularies to connect response goals and scenarios to types of equipment that offer utility towards those goals in those scenarios. RRLT's Knowledge Base will contain details on dozens of equipment types and facilitate the operator's discovery and consumption of these details most pertinent to a dynamically selected subset of goals. The core of its Domain Model is based on a report authored by this team. This report [1] contains a comprehensive list of proposed equipment to accomplish various missions or scenarios that might arise after a large-scale radiological contamination incident in an urban environment or critical infrastructure. The report divides potential response and recovery efforts into five support goals: Survey and monitoring of the contaminated area; Mitigation of received dose to first responders: Decontamination (gross and final) of buildings, vehicles, roadways, parks, and other surfaces: Waste management of solid waste generated during recovery operations: and Containment of wastewater and other waste generated during the response and recovery phases. RRLT's development is driven by use cases. A use case is an intention with which a user approaches the software. Use cases are grouped into delivery increments to schedule development, testing, and presentation to stakeholders. This model partitions the system into seven increments: User Arrival and Authentication, Search and Navigation, Equipment Recommendation, Plan Management, Content Management, and Expanded Access. Once a user 15 authenticated, RRLT will present the user with a dashboard that allows them to explore or search RRLT's content. The dashboard will also include a 'Plan' panel for collecting decisions and relevant observations about an incident at hand to facilitate development of an equipment list. RRLT will offer three general modes of access to items in the knowledge base: - Keyword search for direct discovery of items, - Navigation along predetermined paths from recovery goal towards equipment types, and - Interactive guidance towards equipment types by an autonomous software agent: the Equipment Recommendation Wizard. This presentation will detail progress in the development of the RRLT and also discuss opportunities for those interested in providing feedback on its content and functionality. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Persistent Current Simulation for CCT Testing Magnet Used in EIC

The Electron-Ion Collider (EIC), a powerful new facility to be built in the United States at the U.S. Department of Energy's Brookhaven National Laboratory in collaboration with Thomas Jefferson National Accelerator Facility, will explore the most fundamental building blocks of nearly all visible matter. Here, there are many different types of superconducting magnets near the interaction region (IR) of EIC. Due to space constraints and special lattice requirements, Tapered CCT (canted-cosine theta) magnets have been used for EIC. At beam injection, the magnetic field is only ~5.5% of the maximum operating field. Considerable field errors will be generated from persistent current in superconducting strands even using very fine filament for those superconductors. A tapered CCT demonstrator magnet has been built and tested successfully at BNL since July 2020 to evaluate the key technologies for future tapered CCT magnets. In October 2023, BNL team also measured the persistent current in this demonstrator magnet. To validate the persistent current simulation methods for CCT magnets in EIC, this paper used a full 3D Opera Model and measured magnetization data from superconducting strand for the simulation. Simulation results showed reasonable agreement with recent measurement results.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Deep exclusive meson production as a probe to the puzzle of Λ hyperon polarization

In the 1970s, an unexpected transverse Λ polarization in unpolarized proton-beryllium collisions was discovered, which initiated extensive studies on spin phenomena in high-energy physics. Over the past five decades, similar transverse Λ polarization has been observed across various collision systems, including lepton-hadron deep-inelastic scattering, hadron-hadron collisions, and electron-positron collisions. Despite numerous promising theoretical models, the fundamental mechanism underlying this polarization phenomenon remains inconclusive to this day. However, in both longitudinally and transversely polarized lepton-hadron and hadron-hadron collisions, it is found that the Λ hyperon is polarized with respect to the initial parton spin direction. How the Λ hyperon acquires its spin has become one of the most crucial questions to address in order to resolve this puzzle. In this paper, I propose to use an exclusive process that can be measured at the Electron-Ion Collider, the deep exclusive meson production, to explicitly test the mechanism of Λ polarization. The outcomes of this experimental measurement are anticipated to unveil the dominant mechanism by which Λ obtains its spin, eliminating many of the ambiguities that have been encountered in previous studies. Finally, experimental challenges and requirements are discussed. Published by the American Physical Society 2024

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Measurement of Nuclear Dependence in Inclusive Antineutrino Scattering

One of the fundamental questions in physics is the matter-antimatter asymmetry of the Universe, explored through charge-parity violation searches in neutrino oscillation experiments. Next-generation oscillation experiments like DUNE need to constrain the systematic uncertainties arising from our understanding of (anti)neutrino-nucleus scattering to within a few percent to achieve their physics goals. MINERvA, a dedicated (anti)neutrino-nucleus scattering experiment, plays a crucial role in constraining these uncertainties. This thesis presents MINERvA's first high-statistics direct measurement of nuclear dependence in charged-current inclusive antineutrino scattering on carbon, hydrocarbon, iron, and lead as a function of antimuon transverse momentum, $p_{\text{T}}$, and Bjorken~$x$. The analysis utilises interactions with a mean antineutrino energy of approximately~6~GeV, with reconstructed antimuons having a scattering angle of less than 17$^\circ$ relative to the antin eutrino beam and an antimuon energy of 2--20 GeV. The measured per-nucleon differential cross-sections are reported with a precision of 7--9\%, while the cross-section ratios of carbon, iron, and lead to hydrocarbon have uncertainties of 5\% or less. The cross-sections for iron and lead indicate strong suppression at low $p_{\text{T}}$ and Bjorken~$x$, and an enhancement at high $p_{\text{T}}$. These effects are observed to be more pronounced with the increasing size of the target nucleus and are not reproduced by the underlying simulation prediction. Comparisons to alternative models used in current (anti)neutrino interaction generators show some improvements in modelling over the base prediction model, yet they are still unable to fully reproduce the observed nuclear dependence in this analysis. Importantly, the analysis provides a direct test of nuclear effects in inclusive antineutrino scattering, with major contributions from resonant pion production, deep inelastic scattering, and the transition region between these channels, which will be significant in DUNE. This measurement also represents one of the largest antineutrino datasets in this energy regime analysed to date.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2021

Assessing subtle variations in the actinyl oxo reactivity through characterization of neptunyl complexes. Final Report

Formation of the actinyl cation, [An(V,VI)O 2 ] n+ (n = 1,2), imparts unique chemical properties to the lighter actinide elements (U, Np, and Pu) that has yet to be fully understood. The axial O atoms (oxo) of the [An(VI)O 2 ] 2+ are considered weak Lewis bases that exhibit only meager interact with other metal cations and regarded as poor hydrogen acceptors for nearby water molecules. Oxo atoms of [An(V)O 2 ] + should engage in stronger bonding interactions due to a higher degree of Lewis basicity, but the actual interactions have yet to be fully explored. Intermolecular interactions can impact radionuclide separations, corrosion of spent fuel, and mobility of actinides in environmental systems; there is, therefore, a critical need to understand how the subtle difference in electronic properties of the An(V) and An(VI) metal center influence actinyl chemistry. The objective of this proposal was to determine the chemical components that influence the intermolecular interactions occurring between neptunyl ([Np(V)O 2 ] + and [Np(VI)O 2 ] 2+ ) cations and neighboring species. My overall hypothesis was that the intermolecular attraction that occurs between the neptunyl oxo atoms and neighboring species (H atoms, low-valent cations, actinyl cations) is primarily controlled by the electronic properties of the actinyl cation, but can be further influenced by the electron donating properties of the equatorial ligands. The hypothesis was tested through the following research objectives: (1) Determine the fundamental differences in H-bonding between Np(V)O 2+ and Np(VI)O 2 2+ and neighboring donor molecules; (2) Identify the major differences in bonding between low-valence metal cations and neptunyl oxo groups, and (3) Assess the impact of the equatorial ligand on the formation of cation-cation interactions within molecular species. Major outcomes of the research include: (1) More precisely identifying oxo interactions (actinyl-cation; actinyl-actinyl, actinyl-hydrogen) and the factors that impact the vibrational modes for actinyl cation; (2) Identification of H-bonding modes for the [An(V,VI)O 2 ] n+ (n = 1,2), with direct H-bonding interactions to the oxo group of the Np(V)O 2+ cation more prevalent than in hexavalent species and recognition of the importance of H-bonding networks, that can impart bond asymmetry and activation of vibrational modes with the actinyl moiety; (3) Delineation of the importance of charge density for engaging the cation-oxo interaction for both pentavalent and hexavalent species; (4) Determining the importance of sterics and ligand binding in formation of specific actinyl-actinyl interactions and the resulting vibrational modes associated with this bonding motify and (5) Understanding how the functionalization of the ligand can impact redox stability of neptunyl cations. Deliverables from this work include 11 peer-reviewed manuscripts and 13 (including six by graduate students) oral/poster presentations.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Fallout Cloud Regimes

The U.S. Department of Defense (DOD), Department of Energy (DOE), and other organizations maintain operational nuclear explosion and atmospheric dispersion models to provide critical guidance on the expected effects of an accidental or deliberate explosion of a nuclear weapon (in this paper simply referred to as “device”). To be effective, these models must represent, as accurately as possible, the complex interactions of the blast, fire, and residual radiological hazards with the environment and population. One hundred atmospheric nuclear tests that form the basis for many models were conducted at the Nevada Test Site (NTS) (now referred to as the Nevada Nuclear Security Site, NNSS) in a dry desert environment. Other environments should be studied, but have less data available and are beyond the scope of the work presented in this paper. The debris clouds produced by the NTS tests, frequently called “mushroom clouds,” are familiar, with common structural elements such as a buoyant cap connected to a skirt of raised dust at the desert surface by a thin, dirt-filled stem. The film scanning project at LLNL has investigated historical film records of nuclear weapons tests. Here, we summarize findings showing that the mushroom cloud behavior for historic U.S. tests conducted in Nevada, has similar characteristics based on the distance of the device from the ground surface or Height of Burst (HOB), scaled by the energy release, or yield, of the device. This scaled height is referred to as the scaled-height-of-burst (SHOB). The findings discussed below show that mushroom clouds look and behave similarly when detonated at the same SHOB. The amount of residual radiation that is produced by a nuclear detonation is proportional to the yield. But, the amount of that residual radiation that actually becomes local fallout is strongly dependent on the SHOB and the type of surface over which the detonation occurs. In order to develop a more comprehensive model that predicts the fraction of the residual radiation that becomes local fallout, it is convenient to define a series of regimes based on SHOB values in which all detonations that occur within a given regime can be modeled using the same algorithms. The purpose of this paper is to provide a framework for defining different regimes, and, in a qualitative way, a basic understanding of the fundamental characteristics of each of these regimes.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

DOE OSTI2024

Nucleon Structure Studies at Jefferson Lab and the Electron Ion Collider

The research programs of Thomas Jefferson Laboratory (JLab) and the future Electron- Ion Collider (EIC) focus on one of the main goals of strong interaction studies : understanding the structure of nucleons in terms of the quarks and gluons composing them. Their structure is encoded in functions such as Generalized Parton Distributions (GPDs), which describe how quarks and gluons’ transverse position and longitudinal momentum are distributed inside nucleons. GPDs allow to obtain three-dimensional pictures of nucleons and to understand some of their fundamental properties, such as their internal pressure or the emergence of their spin from the dynamics of the partons composing them. At JLab and the EIC, electron beams are used to probe nucleons. Measurement of reactions such as Deeply Virtual Compton Scattering (DVCS) allows access to GPDs. The first longitudinally polarized-target experiment of the CLAS12 program at Jlab took place in 2022-2023. Combining polarized electron beams and nucleon targets, this experiment offers unique access to observables that allow the measurement of different types of GPDs. In particular, the DVCS beam- and target-spin asymmetries for protons and neutrons in deuterium will be measured for the first time. They give access to kinds of GPDs that are still poorly known, and the comparison between proton and neutron data will allow the extraction of the flavor dependence of the structure of nucleons. Specific analysis methods have been implemented to work with a polarized nuclear target and are presented in this thesis. These methods allow to obtain preliminary results for the asymmetries, waiting for the complete statistics to be available. In the long term, the experimental program for the EIC has been established with a strong emphasis on the measurement of the structure of nucleons at high energy. Measurements of reactions such as DVCS impose strict requirements on the electromagnetic calorimeter that will allow to measure the energy of the scattered electrons and photons. This calorimeter, which is under development, will be based on scintillating crystals read by Silicon Photomultipliers (SiPMs). A new type of glass-based scintillating material was tested, evaluating the possibilities to meet the technical requirements concerning their light yield and resistance to radiation damage in particular. Several models of SiPMs have been characterized, demonstrating they can operate over the vast energy range necessary to address the physics case at the EIC and providing guidelines for developing their readout electronics.

Pilleux, Noemie↗

DOE OSTI2025

Computational Fluid Dynamics Analysis of the Molten Salt Tritium Transport Experiment Test Section

Tritium, a radionuclide produced through neutron capture by lithium and other elements (beryllium and fluoride) in molten salts, presents unique challenges to radionuclide release. This is true for both fusion energy breeder blankets and molten salt fission reactors. The fundamental understanding of tritium transport is crucial to the safe design and operation of these reactors. The Molten Salt Tritium Transport Experiment (MSTTE), currently under construction at Idaho National Laboratory, aims to investigate tritium transport phenomena using a forced-convection fluoride salt loop. This loop is designed to study various transport mechanisms, such as permeation through metals and gas-liquid interactions, and is intended to support future research on tritium extraction units. A critical aspect of the MSTTE loop design is ensuring a fully developed velocity profile before the fluid reaches the permeation test section where measurements are made. This study employs computational fluid dynamics to model the salt flow behavior within the MSTTE permeation test section. A realizable k-ε turbulent model with enhanced wall treatment is used to simulate the single-phase, vertical upward flow of molten salt FLiNaK under isothermal conditions. The simulation results indicated flow distortion and underdeveloped profiles at all planned flow rates within the test section due to the 85-deg sharp bend. To address this issue, a reduced diameter with a reducer and expander and a flow conditioner are investigated to achieve fully developed flow. The analysis showed that the flow conditioner successfully corrected the flow profile, achieving fully developed behavior at a flow rate of 50 liters per minute (LPM). In conclusion, this research enhances our understanding of flow dynamics in molten salt systems and contributes to optimizing tritium transport control technologies.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2026

Experimental investigation of a closed vapour box module for a divertor-like configuration in Magnum-PSI

Efficient management of extreme heat fluxes in the divertor region to extend the lifetime of the components remains a critical challenge for the realization of nuclear fusion-based power plants. Among the alternative concepts explored for the divertor region, the use of liquid metals, particularly lithium, is of interest due its ability to dissipate the incoming plasma heat flux through the vapour shielding effect (VS). In this work, we experimentally investigated a ‘closed’ configuration of a dedicated Vapour Box Module (VBM) in the linear plasma device Magnum-PSI. The goal of the experiments is to simulate the vapour box divertor environment conditions and assess its performance in terms of power mitigation and redistribution and lithium confinement. Initial testing without Li demonstrated the efficacy of a closed VBM structure in inducing detachment via neutral gas accumulation. Apertures which enabled non-condensing gas to be effectively pumped while ensuring lithium condensed on the inner surfaces were therefore added. With a lithium capillary porous structure target used, lithium is directly vaporized by the plasma, forming a dense lithium vapour cloud that interacts with the incoming plasma. This resulted in a significant reduction of the target temperature of at least 48%, together with a temperature locking effect, a phenomenon typically observed in the VS regime. Lithium vapour confinement within the VBM was strongly correlated with the wall temperature. Relatively cold walls promoted Li re-condensation and therefore improved Li confinement, although with the expected trade-off of increased hydrogenic retention on lithium-wetted surfaces. As the wall temperature increased, the confinement efficiency decreased, consistent with reduced Li re-condensation and thermally activated Li–H chemistry and remobilization at the walls. Diagnostic measurements through embedded thermocouples and calorimetry revealed that lithium vaporization and re-condensation processes also playedsignificant roles in plasma power dissipation. The results advance the case for a closed divertor chamber with direct lithium evaporation from the strike-points as a viable method to manage divertor heat fluxes in future fusion reactors.

Romano, Fabio [Dutch Institute for Fundamental Ene↗

DOE OSTI2022

Test of lepton universality in beauty-quark decays

The standard model of particle physics currently provides our best description of fundamental particles and their interactions. The theory predicts that the different charged leptons, the electron, muon and tau, have identical electroweak interaction strengths. Previous measurements have shown that a wide range of particle decays are consistent with this principle of lepton universality. This article presents evidence for the breaking of lepton universality in beauty-quark decays, with a significance of 3.1 standard deviations, based on proton–proton collision data collected with the LHCb detector at CERN’s Large Hadron Collider. The measurements are of processes in which a beauty meson transforms into a strange meson with the emission of either an electron and a positron, or a muon and an antimuon. If confirmed by future measurements, this violation of lepton universality would imply physics beyond the standard model, such as a new fundamental interaction between quarks and leptons.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Effects of renormalon scheme and perturbative scale choices on determinations of the strong coupling from e + e − event shapes

We study the role of renormalon cancellation schemes and perturbative scale choices in extractions of the strong coupling constant α s ( m Z ) and the leading nonperturbative shift parameter Ω 1 from resummed predictions of the e + e − event shape thrust. We calculate the thrust distribution to N L 3 L ′ resummed accuracy in soft-collinear effective theory (SCET) matched to the fixed-order O ( α s 2 ) prediction, and perform a new high-statistics computation of the O ( α s 3 ) matching in , although we do not include the latter in our final α s fits due to some observed systematics that require further investigation. We are primarily interested in testing the phenomenological impact sourced from varying amongst three renormalon cancellation schemes and two sets of perturbative scale profile choices. We then perform a global fit to available data spanning center-of-mass energies between 35–207 GeV in each scenario. Relevant subsets of our results are consistent with prior SCET-based extractions of α s ( m Z ) , but we are also led to a number of novel observations. Notably, we find that the combined effect of altering the renormalon cancellation scheme and profile parameters can lead to few-percent-level impacts on the extracted values in the α s − Ω 1 plane, indicating a potentially important systematic theory uncertainty that should be accounted for. We also observe that fits performed over windows dominated by dijet events are typically of a higher quality than those that extend into the far tails of the distributions, possibly motivating future fits focused more heavily in this region. Finally, we discuss how different estimates of the three-loop soft matching coefficient c S ˜ 3 can also lead to measurable changes in the fitted { α s , Ω 1 } values. Published by the American Physical Society 2024

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2020

Measurement of quark- and gluon-like jet fractions using jet charge in PbPb and pp collisions at 5.02 TeV

The momentum-weighted sum of the electric charges of particles inside a jet, known as jet charge, is sensitive to the electric charge of the particle initiating the parton shower. This paper presents jet charge distributions in $ \sqrt{s_{\mathrm{NN}}} $ = 5.02 TeV lead-lead (PbPb) and proton-proton (pp) collisions recorded with the CMS detector at the LHC. These data correspond to integrated luminosities of 404 μb$^{−1}$ and 27.4 pb$^{−1}$ for PbPb and pp collisions, respectively. Leveraging the sensitivity of the jet charge to fundamental differences in the electric charges of quarks and gluons, the jet charge distributions from simulated events are used as templates to extract the quark- and gluon-like jet fractions from data. The modification of these jet fractions is examined by comparing pp and PbPb data as a function of the overlap of the colliding Pb nuclei (centrality). This measurement tests the color charge dependence of jet energy loss due to interactions with the quark-gluon plasma. No significant modification between different centrality classes and with respect to pp results is observed in the extracted quark- and gluon-like jet fractions.[graphic not available: see fulltext]

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2024

The Uranium-Containing and Thorium-Containing Anions Studied by Photoelectron Spectroscopy

An in-depth knowledge of actinide chemistry is fundamental to many aspects of nuclear science and technology, including the synthesis and processing of materials and the remediation of waste disposal sites. Among the actinides, the chemical bonding behaviors of actinium and thorium resemble those of the transition metals; the 5f-electrons of protactinium, uranium, neptunium, and plutonium often play important roles in their bonding; and among the still heavier elements, their bonding tends to mimic the lanthanide elements in terms of electron shielding and their f-electron contributions. Bonding that involves 5f-electrons, however, is especially important, in part because of the significance of uranium and plutonium, but also because these elements are among the few where f-electron participation in bonding is relatively common. This work focused on studying uranium-containing and thorium-containing anions in the gas phase using negative ion photoelectron spectroscopy. Since this technique directly probed valence electrons, it was uniquely positioned to address open questions regarding molecular bonding and electron configurations. A particularly important issue concerned how bonding in actinide-containing molecules was affected by modifications to their actinide atoms’ environment, i.e., due to their interaction with ligands. A closely related question was how actinide atoms’ suborbitals were qualitatively reordered and their energies quantitatively shifted as a result of their ligated environments. These were especially relevant issues in regard to uranium due to it having multiple possible oxidation states (OS) and the potential for 5f electron participation in bonding. The effects of ligands on oxidation states and 5f-orbital energies in uranium bonding was expected to be pronounced. Both ligands and excess electrons were seen as probes of actinide atoms within actinide-containing molecules. Our strategy for advancing knowledge of chemical bonding in the actinide-containing species utilized the synergy between experiments and theory, where in some cases experimental results validated theory and where in others computational results assisted in interpreting experiments. Calculations on actinide systems are terrifically challenging due to large spin-orbit interactions, relativistic effects, and just the sheer number of electrons involved. Even in the simplest species, e.g., U and U2, the most sophisticated, modern calculations carried out by the most experienced theorists often only approximate experimentally-measured values, such as electron affinities. For theory to provide confident predictions that can be used to solve real problems it needed an iterative and ultimately corrective mechanism by which its methods can develop further. Experiments can be used to identify when theory has failed; whereupon the subsequent process of using the experiment-theory interplay can be used to find the cause of the failure. Upon fixing it in one case, different test species can be proposed and studied by the experiment-theory combination to determine whether the problem has been corrected. Thus, experiments not only measure the values of molecular properties, they also provide navigational 3 beacons that keep computations off the reefs in an otherwise dark sea with few reference points. Experimental measurements in the actinide field are not only important, they are in actuality essential to computational progress. While it was not always possible to compare the theoreticallydetermined quantity of interest directly with the same experimentally-measured observable, it was usually possible to compare consequential properties that are both calculable and measurable. In the work completed here electron affinities and electronic state spacings were often sensitive consequential parameters. Reasonable agreement between measured and computational values signaled that a calculation that was very likely to be on-track. We had established collaborative relationships with five computational groups, all of which have expertise in computational actinide chemistry. Their PI’s are L. Cheng, D. Dixon, L. Gagliardi, K. Peterson, and B. Vlaisavljevich. Our close interaction with our theory partners led to us suggesting systems to them and them to us. This reciprocal interaction between our experimental and their computational results was among the most important strengths of this work and was a thread woven throughout. Even though anion photoelectron spectroscopic studies are conducted on anions, much of the information that they provide, pertains to the electronic structure of the neutral counterparts of those anions; among these are electron affinities and electronically excited state spacings. Our experimental tools included several specialized ion sources for forming the anionic species of interest, a mass spectrometer for identifying and mass-selecting them, and an anion photoelectron spectrometer for determining their electron affinities (EA) and characterizing the electronic states of the selected anions’ neutral counterparts. Anion photoelectron spectroscopy is conducted by crossing a mass-selected beam of anions with a fixed-frequency laser beam and energy-analyzing the resultant photodetached electrons. The photodetachment process is governed by the energyconserving relationship: hν = EBE + EKE, where hν is the photon’s energy, EBE is the electron binding (photodetachment transition) energy, and EKE is the electron’s kinetic energy. In our apparatus mass-selection is accomplished via time-of-flight mass spectrometry (TOF-MS), electron energy analysis is achieved with either a magnetic bottle or by velocity mapped imaging. Photodetachment of electrons from anions is implemented via either Nd:YAG or excimer lasers. The photodetachment transition energy, i.e., the EBE, between the ground vibrational and electronic state of an anion and the ground vibrational and electronic state of that anion’s neutral counterpart is the adiabatic electron affinity (EA) of that neutral molecule. Likewise, photodetachment transitions between the ground vibrational and electronic state of an anion and the various electronically-excited states of that anion’s corresponding neutral map the electronic spectrum of that neutral species, i.e., the spectral spacings in the photoelectron spectrum are a mirror image of the neutral’s electronic spectrum. It was, of course, crucial to be able to form the anionic species of interest. There, we had a particularly broad field of anion sources from which to choose. These included several variants of pulsed laser vaporization (LV), laser photoemission, infrared desorption plus photoemission, pulsed arc discharge (PACIS), electrospray ionization (ESI), and Rydberg electron transfer (RET). Each of these anion sources were readily combined with, i.e., connected to, the anion photoelectron spectroscopic portion of our apparatus as described above. Among the sources that utilize lasers, visible light for LV sources as well as IR for desorption sources are provided by Nd:YAG lasers. Ultraviolet photons are provided by both Nd:YAG and excimer lasers, whereas the excitation wavelengths for RET experiments come from two Nd:YAG-pumped dye lasers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Next Generation Noble Liquid Detectors

The research program here combines Generic and Directed R\&D for Liquid Noble Gas detectors for neutrino physics and dark matter. In neutrino physics and dark matter research, we are addressing some of the most fundamental questions in particle physics today by studying these tiny particles in the electron family. To study them, detectors must be large, high precision, and ideally have the ability to collect detailed information from both charge and light from neutrino and dark matter interactions. Precision detection combined with large scales can be challenging. Liquid Argon detectors mitigate some of these challenges given the nature of its interaction medium and it’s relatively inexpensive cost per ton. Significant progress has been made in the last 15 years in developing these kinds of detectors to be built and operated at large scales. However there are still challenges and new ideas in moving these detectors from ton scale to kiloton scale. To be able to get the most out of these kinds of detectors directed questions with respect to specific components running and colleting data in the detectors must be understood. As well, new ideas on how to best combine charge and light measurements may lead to new ways to learn new things with these detectors. Experimental test stands to conduct this work, as is done in this proposal, to accomplish both of these goals are critical to address both of these questions. In the test stand enabled under this grant at Yale University’s Wright lab, new developments in efficient small scale setups were developed, instrumentation developed for running and future experiments (the SBND experiment at Fermilab at present, the DUNE experiment in the future) were and will be tested, and new ideas for charge and light determination for new measurements are under study. The long term impact of this work in neutrino physcis is both for the short and long baseline programs originating at Fermi National Accelerator Laboratory. At long baselines, the US flagship DUNE experiment will measure neutrino properties through neutrino oscillations using a beam originating at Fermilab and a massive LArTPC detector sited about a mile underground at the Sanford Underground Research Facility in Lead, South Dakota. Studies here on the high voltage for thes detectors, and ongoing work on charge and light production and collection in the TPC are relevant for the design and data taking of this and other LArTPC detectors to enable them to best measure the neutrinos created at Fermilab that then pass through the detector in South Dakota. What we learn in these detectors may ultimately change the course of how we understand neutrino’s impact in the early universe. What we learn about how to improve this detection technology and develop new ideas in Lar detectors in general may impact both future neutrino experiments and dark matter experiments.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2022

Direct observation of the dead-cone effect in quantum chromodynamics

In particle collider experiments, elementary particle interactions with large momentum transfer produce quarks and gluons (known as partons) whose evolution is governed by the strong force, as described by the theory of quantum chromodynamics (QCD). These partons subsequently emit further partons in a process that can be described as a parton shower, which culminates in the formation of detectable hadrons. Studying the pattern of the parton shower is one of the key experimental tools for testing QCD. This pattern is expected to depend on the mass of the initiating parton, through a phenomenon known as the dead-cone effect, which predicts a suppression of the gluon spectrum emitted by a heavy quark of mass m Q and energy E, within a cone of angular size m Q /E around the emitter. Previously, a direct observation of the dead-cone effect in QCD had not been possible, owing to the challenge of reconstructing the cascading quarks and gluons from the experimentally accessible hadrons. We report the direct observation of the QCD dead cone by using new iterative declustering techniques to reconstruct the parton shower of charm quarks. This result confirms a fundamental feature of QCD. Furthermore, the measurement of a dead-cone angle constitutes a direct experimental observation of the non-zero mass of the charm quark, which is a fundamental constant in the standard model of particle physics.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2020

The Quantum Nature and Mass of the Neutrino. FY20 Annual Laboratory Continuation Progress Report

Over the last 100 years we have learned a much about the neutrino, but there remain interesting questions about this weakly interacting particle. In particular, at LLNL we are developing experiments to measure the mass and the quantum nature of the neutrino. The 2015 long range plan recommended tonne-scale neutrinoless double beta decay experiments as the top new project priority and this experiment will target the quantum nature of the neutrino. The LLNL team is motivated and focused on developing the best technology for this experiment which is a liquid xenon time project chamber called nEXO. On a longer time scale, LLNL is also developing technology to measure the neutrino mass with tritium decay experiments. Work on nEXO at LLNL started in 2015 with an LDRD and program development funds to develop the nEXO concept, publish sensitivity predictions, explore alternatives and risks, and to build a credible project team and this effort is on going. In addition, we received research funding from DOE-SC NP and LLNL manages pre-conceptual R&D for the nEXO collaboration a portion of which is executed at LLNL. The Project 8 effort is solely funded by LLNL LDRD, and ends this year. A second LDRD effort is focused on repurposing cyclotron radiation emission spectroscopy for eV-scale X-ray detection. This second effort, while separated from Project 8, still has scientific and technical commonalities with Project 8. The funding for this X-ray detection effort will continue for one more year. LLNL has a long history of building large projects, science projects and time projection chambers, but nEXO is in fact the first project of this scale that LLNL is prepared to lead for DOE-SC NP.We have the tools, skills, people and motivation to make nEXO a reality. The current program development dollars are used to prepare the nEXO concept for down select and CD1. These internal LLNL dollars pay for a number of things including project staff to organize the nEXO collaboration for the various reviews that lie ahead, to develop the draft plans and structure to manage the project as well as setting up an external advisory committee. The current LDRD is exploring alternatives that effect the risk profile as well as possible performance improvements. The DOE-SC NP base funding is targeted at simulation and analysis of the nEXO concept in preparation for the down select and refinement of the understanding of the detector as well as scientific effort on the large xenon test stand (LXTS) that will burn down one of the largest risks to the nEXO project. Lastly, LLNL is leading the pre-conceptual R&D effort and managing the funds for the nEXO collaboration. The results of this effort are reported elsewhere, but the scope of this executed at LLNL will be reported here and is primarily the engineering and construction of the LXTS experiment. The primary technical contribution of LLNL to the Project 8 concept is the formation and study of atomic tritium. Atomic tritium is necessary for Project 8 to reach the ultimate sensitivity. LLNL has considerable experience with tritium and is well suited for this crucial work. Although the focus of this work is strictly fundamental science, there has already been one significant spinoff to develop a new means to measure radio xenon in the air

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2025

Observation of the distribution of nuclear magnetization in a molecule

Precise experimental control and interrogation of molecules and calculations of their structure are enriching the investigation of nuclear and particle physics phenomena. Molecules containing heavy, octupole-deformed nuclei, such as radium, are of particular interest. Here, we report precision laser spectroscopy measurements and theoretical calculations of the structure of the radioactive radium monofluoride molecule 225 Ra 19 F. Our results reveal fine details of the short-range electron-nucleus interaction, indicating the high sensitivity of this molecule to the distribution of magnetization, within the radium nucleus. Here, these results provide a stringent test of the description of the electronic wave function inside the nuclear volume, highlighting the suitability of these molecules for investigating subatomic phenomena.

Nuclear structure↗

DOE OSTI2024

DECOVALEX-2023: Task D Final Report

Task D of DECOVALEX-2023 is focused on the simulation of the coupled thermal hydraulic-mechanical (THM) behaviour in the full-scale engineered barrier system (EBS). The Horonobe EBS experiment is the demonstration of the full-scale EBS in the underground research laboratory (URL) (performed by JAEA in the Horonobe URL in Japan). Task D consisted of the three steps, a preliminary step (Step 0), simulation of the laboratory tests (Step 1) and simulation of the in-situ full-scale EBS experiment (Step 2). Since the Horonobe EBS experiment demonstrates the vertical emplacement option of the EBS, the experiment gallery is also backfilled with the backfill material. Therefore, interaction between the EBS and the backfill material can also be demonstrated, such as deformation (change of density) of the buffer material. The underground water in the Horonobe URL is saline. This fact adds chemical processes to THM behaviour. For example, mechanical properties (such as swelling pressure of the buffer material and backfill material) and hydraulic properties (such as permeability of the buffer material and backfill material) change depending on the water chemistry. Task D was therefore a challenging Task focused on not only the relatively simple THM behaviour but also complex THM behaviour including chemical processes. Six research teams (BGR, CAS, JAEA, KAERI, SNL and Taipower) participated the Task D. BGR, CAS, JAEA, KAERI and Taipower research teams selected a THM approach, while the SNL research team selected a TH approach. Step 1 involved the simulation of laboratory test results and was important to check the numerical codes developed by the research teams. Step 1 was divided into four sub steps. The simulation results through the Step 1 identified the parameters for simulation of the Step 2. Basic parameters of the materials (buffer material, backfill material, rock mass, concrete, sand) were provided by JAEA. Special parameters which research team needed were identified by back analysis of Step 1. Most notably the mechanical behaviour of swelling and displacement depended on the applied model (elastic model or elastoplastic model). Parameters such as Young’s modulus were found to need smaller values than characterised in the fundamental laboratory test results (Step 1-1, 1-2) for the elastic model. Although laboratory experiments are usually simple, test results contained some error. For example, if the saturation level is 100 % or higher, it should be considered an error. This situation was presented in the Step 1-3. A possible reason is that the buffer material is a mixture of bentonite and silica sand. When a specimen is cut to measure volume or weight, sand grains will affect the measurement data. In Step 2, boundary conditions such as temperature on the surface of the simulated overpack, heater power of the electrical heaters installed in the simulated overpack, injection pressure and inflow rate of the test water, were applied. The outer boundary conditions can be selected using measured data (injection pressure and inflow rate of the test water that is controlled by the injection systems installed in the sand layer around the buffer material and in the boundary between backfill material and concrete support). Since such measured data has some noise, research teams developed their own simplified boundary conditions. Inner boundary conditions can be selected using measured data as heater power and temperature on the surface of the simulated overpack. These data also contain some noise, so research teams developed their own simplified developed boundary conditions. Task D validated various approaches thorough the simulation of the in-situ full scale EBS system including backfill of the gallery: variations in the coupling processes (THM or THC), analysis codes, and boundary conditions. Temperature distribution in the buffer material was simulated well by all research teams. This means thermal behaviour is not sensitive to the simulation approaches. Although the water content distribution on the outside of the buffer material was well simulated by all research teams, the simulation results differ from the measured values inside the buffer material (at the centre and inside, near the simulated overpack). The buffer material is made from tap water, but in the in-situ experiment, saline groundwater infiltrates the buffer material. Therefore, the selection of the hydraulic parameters of the buffer material greatly affects the simulation results of the re saturation behaviour of the buffer material. In the Horonobe EBS experiment, measured values suitable for validating the simulation results were not obtained near the simulated overpack. When simulating the pressure and deformation of the buffer material, the measurement data is easily affected by the installation conditions of the measurement sensors, so verifying the measurement data itself remains an issue. Mechanical simulation results differ depending on whether they are considered as elastic or elastoplastic phenomena. The accuracy of measured in-situ data can be assessed by detailed analysis comparing sampling specimen analysis and measured data. The Horonobe EBS experiment is scheduled to be dismantled in the future (FY2026 and 2027). This detailed dismantling investigation will finally confirm the measured data.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗