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DOE OSTI2024

Observational evidence for Criegee intermediate oligomerization reactions relevant to aerosol formation in the troposphere

Criegee intermediates are reactive intermediates that are implicated in transforming the composition of Earth’s troposphere and in the formation of secondary organic aerosol, impacting Earth’s radiation balance, air quality and human health. Yet, direct identification of their signatures in the field remains elusive. Here, from particulate and gas-phase mass-spectrometric measurements in the Amazon rainforest, we identify sequences of masses consistent with the expected signatures of oligomerization of the CH 2 OO Criegee intermediate, a process implicated in ozonolysis-driven aerosol formation. In this study, we assess the potential contributions of oligomerization through laboratory ozonolysis experiments, direct kinetic studies of Criegee intermediate reactions, and high-level theoretical calculations. Global atmospheric models built on these kinetics results indicate that Criegee intermediate chemistry may play a larger role in altering the composition of Earth’s troposphere than is captured in current atmospheric models, especially in areas of high humidity. However, the models still capture only a relatively small fraction of the observed signatures, suggesting considerable underestimates of Criegee intermediate concentrations and reactivity and/or the dominance of other, presently uncharacterized, oxidation mechanisms. Resolving the remaining uncertainties in emission inventories and the effects of atmospheric water vapour on key chemical reactions will be required to definitively assess the role of Criegee intermediate oligomerization reactions.

58 GEOSCIENCES↗

DOE OSTI2020

Benched: Upgrading and Updating the Los Alamos Benchmark Suite for the 21st Century [Slides]

The presentation begins by stating that most organizations make choices to handle specific things when preparing input files for validation, such as which elemental abundance data to use, how to decompose specific elements, and setting calculation precision. It also discusses the consequences, which include differing calculation results between different organizations for the same case, even when using the same code. This is illustrated by the intercomparison exercise and input files that are prepared by one organization and are not necessarily correct for another. The presentation explains that the Los Alamos Benchmark Suite is a centralized repository of high-quality benchmark models currently under development at LANL. The objectives of the new repository are to remain up to date with the latest ICSBEP revision, to have a formal review and revision process, to (eventually) be an open-source repository, and to provide new tools for improved input and output file generation and review.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

Interannual variability and trends of summertime PM2.5-based air quality in the Intermountain West

Abstract Summertime air quality is a growing public health concern in the populated region of Northern Utah. Whereas winter air pollution is highly linked with local atmospheric temperature inversions associated with upper atmospheric high-pressure and radiational cooling in valleys, the relationship between climate factors and the frequency of poor air quality during summer is still unknown. Analyzing the last 20 years of data, we demonstrated that summertime unhealthy days (as defined by PM2.5 air quality index level) in Northern Utah highly correlate with the number of dry-hot days, wildfire size, and an upper atmospheric ridge over the Northwestern United States. The persistent atmospheric ridge enhances lightning-caused fire burned areas in northwestern states and then transports the wildfire smoke toward Northern Utah. Similarly, climate model simulations confirm observational findings, such as an increasing trend of the upper atmospheric ridge and summertime dry days in the northwestern states. Such metrics developed in this study could be used to establish longer-term monitoring and seasonal forecasting for air quality and its compounding factors, which is currently limited to forecasting products for only several days.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Post-DTL Beam Delivery

Ensuring that the beam delivered from the upgraded Front-End (FE) meets the Key Performance Parameters (KPPs) at each user facility is critical to the success of the LANSCE Accelerator Modernization Project (LAMP). For a high-intensity, multi-user facility like LANSCE, compliance with beam loss and radiation thresholds is as important as the charge delivered to each target. While early LAMPF/LANSCE operations relied on iterative tuning to minimize losses from beam halo and tail particles, the new FE may introduce different beam distributions and loss modes—making predictive modeling essential. To manage this, the F2E (Front-End to End) effort is developing detailed particle-tracking models that reflect realistic beamline conditions, including halo formation and expected diagnostic readings. These "snapshot" simulations aim to benchmark live machine performance at a given moment. This will help quantify how beam quality from the new FE will propagate downstream through the facility. Only by validating these models can we confidently assess and mitigate the potential impacts of the LAMP FE on beam delivery. Post-DTL, the beam splits to serve five major user facilities. Historically, low-energy beam transport has been modeled using TRACE, and higher-energy sections with TRANSPORT. These have now been unified into MAD-X format and validated with codes such as Elegant, pyOrbit, XSuite, Impact-Z, and HPSim. The primary focus now is on accurate modeling of full particle distributions (including beam halo) as they traverse the accelerator and beamlines to each experimental station. All models are at various stages of validation with empirical data.

43 PARTICLE ACCELERATORS↗

DOE OSTI2026

PIE-Enabled Study of Aqueous Corrosion & Zr Hydriding in Cr-Coated Cladding: M3GV-23PN0101132

Chromium-coated zirconium alloy cladding is under investigation as an accident-tolerant fuel (ATF) concept to extend performance to higher burnups via improved oxidation resistance and reduced hydrogen pickup. However, hydrothermal corrosion behavior and hydrogen transport mechanisms governing in-service hydriding of these coatings remain poorly understood. In a collaborative study between Pacific Northwest National Laboratory (PNNL), Idaho National Laboratory (INL), and the University of Huddersfield, cold spray (CS) and physical vapor deposition (PVD) Cr-coated Optimized ZIRLO™ cladding samples were characterized after exposure to PWR-simulated water chemistry under both in-core (neutron irradiation) and out-of-core (aqueous-only) conditions at the MIT Research Reactor. Multi-scale characterization was performed independently at PNNL and INL to evaluate coating integrity, microstructural evolution, Cr/Zr interface chemistry, and hydride formation. Both laboratories observed a consistent divergence in hydriding behavior: out-of-core CS Cr-coated cladding exhibited elevated hydride concentrations exceeding those of uncoated cladding, whereas in-core CS samples showed substantially suppressed hydriding. In-core specimens also displayed irradiation-specific features, including nanoscale voids within the Cr coating and radiation-induced segregation clusters in the Zr substrate. CS coatings retained an interdiffusion-free Cr/Zr bond with no intermetallic layer, whereas PVD coatings exhibited inferior quality with visible cracks and pores. An automated image-based hydride quantification method systematically overestimated bulk hydrogen content relative to inert gas fusion measurements, underscoring the need for standardized sample preparation and reference standards. Interpretation of hydride nucleation and growth is complicated by the open inner-diameter of the specimens, which provides additional hydrogen pathways. The results motivate further foundational studies to support predictive models of hydrothermal corrosion and hydrogen transport in unirradiated and irradiated Cr-coated cladding.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

High Quality Doping of GaN Through Transmutation Processing

This project led to several outstanding achievements: - Computational modeling of nuclear reactions, including estimates of the production ratio and doping concentration using TALYS 1.96 based on nuclear reactions in GaN induced by gamma-ray and protons. For photonuclear transmutation doping, simulations proved that Zn/Ge ratio with 40 MeV is higher than the other energies. - Proton transmutation doping was shown to be a potential nuclear source to fabricate p-type gallium-based semiconductor materials, examined during new irradiations with Oak Ridge National Laboratory and Brookhaven National Laboratory (in 200 MeV H - –Linac). - Patent disclosure to the University of Missouri-Columbia about healing effects in GaN by radiations. - Zn-doped p-type GaN through photonuclear transmutation doping process. - The PIs made an oral presentation on the p-type characteristics of Zn-doped GaN at the Materials Research Society Fall meeting in Boston. - The last irradiation process was in progress in collaboration with Argonne National Laboratory.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Gravitational Waves from Rapid Structure Formation on Microscopic Scales before Matter-Radiation Equality

We propose a new scenario for the formation of asteroid-mass primordial black holes (PBHs). Our mechanism is based on the annihilation of the string-wall network associated with thebreaking of a U(1) global symmetry into a discrete ZN symmetry. If the potential hasmultiple local minima (N > 1) the network is stable, and the annihilation is guaranteed by a biasamong the different vacua. The collapse of the string-wall network is accompanied bycatastrogenesis, a large production of pseudo-Goldstone bosons (pGBs) — e.g. axions,ALPs, or majorons — gravitational waves, and PBHs. If pGBs rapidly decay into products thatthermalize, as predicted e.g. in the high-quality QCD axion and heavy majoron models, they do notcontribute to the dark matter population, but we show that PBHs can constitute 100% of the darkmatter. The gravitational wave background produced by catastrogenesis with heavy unstable axions,ALPs, or majorons could be visible in future interferometers.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

An interlaboratory collaboration to determine consensus 231 Pa/ 235 U model ages of a uranium certified reference material for nuclear forensics

Application of the 231 Pa/ 235 U radiochronometer for nuclear forensic investigations is challenged by a lack of certified reference materials with 231 Pa/ 235 U model purification dates. The Japan Atomic Energy Agency, Los Alamos National Laboratory, and Lawrence Livermore National Laboratory completed an interlaboratory study measuring 231 Pa/ 235 U model ages of New Brunswick Laboratory CRM U100. Results from independent laboratories were combined to calculate a consensus 231 Pa/ 235 U model purification date for CRM U100 of March 26, 1959 ± 237 days. This 231 Pa/ 235 U consensus date for CRM U100 may be used by the nuclear forensic community for quality control of 231 Pa/ 235 U radiochronometry measurements of unknown materials.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2022

A Machine Learning Framework to Predict Images of Edge-on Protoplanetary Disks

The physical structure and properties of protoplanetary disks are typically derived from spatially resolved disk images. Edge-on disks in particular provide an important view point on the vertical structure and degree of settling of disks. Such analyses rely on radiative transfer (RT) calculations that are generally computationally intensive due to the high optical depth of disks. Here we present a machine learning framework that has the potential to dramatically speed up the forward modeling process by approximating the results of RT calculations. This framework, trained on an initial set of RT calculations, utilizes an autoencoder neural network to enable the generation of synthetic scattered light images of edge-on disks directly from a set of physical parameters. We demonstrate that this framework generates synthetic images 2–3 orders of magnitude faster than using RT calculations. These machine learning-generated images appear to approximate the RT images well, in particular preserving their size and shape. We also find a strong correlation between the latent space representations of the generated disk images and several of their associated physical parameters. Finally, we discuss potential changes to the framework, such as methods to further improve the image quality, extending the framework to multiple wavelengths, and inverting the process to infer physical parameters from observed images. Overall, these new tools have the potential to enable a more efficient and uniform analysis of edge-on disk properties and the initial conditions of planet formation.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

Climate and air pollution implications of potential energy infrastructure and policy measures in India

India is a rapidly developing economy with interrelated air quality, sustainable development, and climate change mitigation goals. There are unique challenges to achieving each of these goals as well as potential tradeoffs among them. This study examines the implications of possible future energy, climate, and air pollution control policies and measures in India through 2050. We take a scenario approach using the GCAM global energy-climate-land model combined with the Hector simple climate model and the TM5-FASST air quality source-receptor model to examine energy, climate and air quality outcomes. Reducing use of traditional biomass in buildings can reduce primary carbonaceous particulate emissions well below 2015 levels. However, policies that are more ambitious than current plans would likely be required to reduce SO 2 and NO x emissions well below 2015 levels. Among single policy cases considered, pricing of greenhouse gas (GHG) emissions and expansion of natural gas infrastructure have the largest impacts on overall energy system changes relative to the reference scenario. Ambitious air pollution control and GHG policies lead to the largest reductions in air pollution concentrations and radiative forcing, respectively. However, ambitious air pollution control and GHG policies differ in the extent to which they support or impede other policy objectives. Forcing increases due to reduced aerosols from ambitious air pollution policies can be mitigated, at least in part, by applying air pollution control and GHG policies together.

India↗

DOE OSTI2025

Measuring the muon content of inclined air showers using AERA and the water-Cherenkov detectors of the Pierre Auger Observatory

We present a novel approach for assessing the muon content of air showers with large zenith angles on a combined analysis of their radio emission and particle footprint. We use the radiation energy reconstructed by the Auger engineering radio array (AERA) as an energy estimator and determine the muon number independently with the water-Cherenkov detector array of the Pierre Auger Observatory, deployed on a 1500 m grid. We focus our analysis on air showers with primary energy above 4 EeV to ensure full detection efficiency. Over approximately ten years of accumulated data, we identify a set of 40 high-quality events that are used in the analysis. The estimated muon contents in data are compatible with those for iron primaries as predicted by current-generation hadronic interaction models. This result can be interpreted as a deficit of muons in simulations as a lighter mass composition has been established from X max measurements. This muon deficit was already observed in previous analyses of the Auger Collaboration and is confirmed using hybrid events that include radio measurements for the first time.

Abdul Halim, A. [Adelaide U.]↗

DOE OSTI2026

CoURAGE KAZR b1 Processing: Corrections, Calibrations, and Processing Report

The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) User Facility supports atmospheric and earth system research through a comprehensive network of fixed and mobile observatories. These facilities provide long-term and intensive campaign-based observations of clouds, aerosols, precipitation, radiation, and meteorological state variables. ARM observations are designed to improve the physical understanding and numerical representation of atmospheric processes in earth system models, with particular emphasis on cloud-radiation interactions and precipitation processes. The Coast-Urban-Rural Atmospheric Gradient Experiment (CoURAGE) deploys one of the ARM Mobile Facilities (AMF) to the Mid-Atlantic region surrounding Baltimore, Maryland, for the period 1 December 2024 through 30 November 2025. This deployment focuses on characterizing atmospheric structure, cloud properties, and precipitation processes across strong land-use and surface heterogeneity gradients associated with urban, rural, and coastal (Chesapeake Bay) environments. The CoURAGE deployment complements the Baltimore Social-Environmental Collaborative (BSEC), a DOE Urban Integrated Field Laboratory (UIFL), by providing high-quality atmospheric observations needed to connect urban surface processes, emissions, and meteorology to cloud and precipitation responses. In addition to the central urban site, ancillary observing sites were deployed to rural Maryland northwest of Baltimore and to an island site in Chesapeake Bay. These measurements further complement a long-term atmospheric observatory operated in Beltsville, Maryland, by Howard University in collaboration with the Maryland Department of the Environment. Together, these assets form a four-node regional atmospheric observatory network representing Baltimore and its three primary surrounding environments—urban, rural, and coastal/bay. This coordinated observational strategy enables investigation of spatial gradients in boundary-layer structure, cloud occurrence, precipitation evolution, and aerosol-cloud interactions across complex surface regimes. Within this network, vertically pointing cloud radars play a critical role by providing continuous, high-resolution measurements of cloud and precipitation vertical structure.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Incorporating new evaluation on angular distributions and energy spectra of neutron-induced charged particle reactions into the next ENDF library release (Technical Progress Report)

This project aims to provide the improved Evaluated Nuclear Data File (ENDF) using the newly measured data as well as the latest nuclear reaction model for calculating angular distributions and energy spectra on neutron-induced charged particle reactions through the collaboration of Korea Atomic Energy Research Institute (KAERI) and Los Alamos National Laboratory (LANL). The LANL group will provide the experimental data for angular distributions and spectra of (n,p) and (n,α) on several structural materials such as Fe, Ni and Zn isotopes using the Low Energy Neutron-induced Charged-particle (Z) Chamber (LENZ) instrument at Los Alamos Neutron Science Center (LANSCE). The KAERI group will provide the improved evaluated nuclear library which is based on the LANL experimental data, and further will predict angular distributions and spectra of (n,p) and (n,α) reactions on unmeasured nuclides, such as Cr, Mn, Co, Cu and so on. For the first year of this project, we planned to analyze (n,p) and (n,α) reactions for 54,56 Fe and perform new measurements on those reactions for 58,60 Ni isotopes with the LENZ instrument at LANSCE. For improving our evaluation quality, we have studied reaction models to reproduce LANL’s experimental angular distributions and energy spectra using the full Hauser-Feshbach model code, CoH3 with no approximations used. As the first year’s deliverables, we provided the experimental (n,p) and (n,α) reaction cross sections for 54,56 Fe and incorporate new evaluation on angular distributions and energy spectra of neutron-induced charged particle reactions into the current ENDF/B-VIII.0.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

VA EDH Data Curation Documentation FY22-Q2, Rev. 2

The health and well-being of the Nation’s men and women who have served in uniform is the highest priority for the U.S. Department of Veterans Affairs (VA). VA is committed to providing timely access to high-quality, recovery-oriented, evidence-based mental health care that anticipates and responds to Veterans’ needs and supports the reintegration of returning Service members into their communities. VA is working to eliminate suicide among all Veterans by developing and implementing innovative suicide prevention approaches and resources. Health outcomes, such as suicide are typically modeled as a function of genetics and environment, where environment refers to factors beyond medical, e.g., air quality, access to transportation and food, homelessness status, etc. Mental health outcomes for each individual are considered to be associated with multiple stressors that fall under a variety of categories socioeconomic, economic, physical environment. Understanding the relationships between these stressors, covariates and health outcomes, requires curated, standardized data that can be input into the VA’s Recovery Engagement and Coordination for Health - Veterans Enhanced Treatment (REACH VET) or other health outcomes model. Environmental Determinants of Health (EDH) as defined by the World Health Organization (WHO) is clean air, stable climate, adequate water, sanitation and hygiene, safe use of chemicals, protection from radiation, healthy and safe workplaces, sound agricultural practices, health-supportive cities and built environments, and a preserved nature are all prerequisites for good health.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2022

VA EDH Data Curation Documentation (FY22-Q3, Rev.2)

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2022

VA EDH Data Curation Documentation FY22-Q4

The health and well-being of the Nation’s men and women who have served in uniform is the highest priority for the U.S. Department of Veterans Affairs (VA). VA is committed to providing timely access to high-quality, recovery-oriented, evidence-based mental health care that anticipates and responds to Veterans’ needs and supports the reintegration of returning Service members into their communities. VA is working to eliminate suicide among all Veterans by developing and implementing innovative suicide prevention approaches and resources. Health outcomes, such as suicide are typically modeled as a function of genetics and environment, where environment refers to factors beyond medical, e.g., air quality, access to transportation and food, homelessness status, etc. Mental health outcomes for each individual are considered to be associated with multiple stressors that fall under a variety of categories socioeconomic, economic, physical environment. Understanding the relationships between these stressors, covariates, and health outcomes, requires curated, standardized data that can be input into the VA’s Recovery Engagement and Coordination for Health - Veterans Enhanced Treatment (REACH VET) or other health outcomes model. Environmental Determinants of Health (EDH) as defined by the World Health Organization (WHO) is clean air, stable climate, adequate water, sanitation and hygiene, safe use of chemicals, protection from radiation, healthy and safe workplaces, sound agricultural practices, health-supportive cities and built environments, and a preserved nature are all prerequisites for good health.

99 GENERAL AND MISCELLANEOUS↗

DOE OSTI2023

VA EDH Data Curation Documentation FY23-Q2

The health and well-being of the Nation’s men and women who have served in uniform is the highest priority for the U.S. Department of Veterans Affairs (VA). VA is committed to providing timely access to high-quality, recovery-oriented, evidence-based mental health care that anticipates and responds to Veterans’ needs and supports the reintegration of returning Service members into their communities. Since its creation, VA has been working to eliminate suicide among all veterans by developing and implementing innovative suicide prevention approaches and resources. Health outcomes, such as suicide are typically modeled as a function of genetics and environment, where environment refers to factors beyond medical, e.g., air quality, access to transportation and food, homelessness status, etc. Mental health outcomes for each individual are considered to be associated with multiple stressors that fall under a variety of categories including socioeconomic, economic, physical environment. Understanding the relationships between these stressors, covariates and health outcomes requires curated, standardized data that can be input into the VA’s Recovery Engagement and Coordination for Health, Veterans Enhanced Treatment (REACH VET) or other health outcomes model. Environmental Determinants of Health (EDH) as defined by the World Health Organization (WHO) is clean air, stable climate, adequate water, sanitation and hygiene, safe use of chemicals, protection from radiation, healthy and safe workplaces, sound agricultural practices, health-supportive cities and built environments, and a preserved nature are all prerequisites for good health.

99 GENERAL AND MISCELLANEOUS↗

DOE OSTI2023

VA EDH Data Curation Documentation FY23-Q3

The health and well-being of the Nation’s men and women who have served in uniform is the highest priority for the U.S. Department of Veterans Affairs (VA). VA is committed to providing timely access to high-quality, recovery-oriented, evidence-based mental health care that anticipates and responds to Veterans’ needs and supports the reintegration of returning Service members into their communities. Since its creation, VA has been working to eliminate suicide among all veterans by developing and implementing innovative suicide prevention approaches and resources. Health outcomes, such as suicide are typically modeled as a function of genetics and environment, where environment refers to factors beyond medical, e.g., air quality, access to transportation and food, homelessness status, etc. Mental health outcomes for each individual are considered to be associated with multiple stressors that fall under a variety of categories including socioeconomic, economic, physical environment. Understanding the relationships between these stressors, covariates and health outcomes requires curated, standardized data that can be input into the VA’s Recovery Engagement and Coordination for Health, Veterans Enhanced Treatment (REACH VET) or other health outcomes model. Environmental Determinants of Health (EDH) as defined by the World Health Organization (WHO) refers to clean air, stable climate, adequate water, sanitation and hygiene, safe use of chemicals, protection from radiation, healthy and safe workplaces, sound agricultural practices, health-supportive cities and built environments, and a preserved nature are all prerequisites for good health.

97 MATHEMATICS AND COMPUTING↗