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Comprehensive Analysis of the Relative Dispersion of Droplet-Size Distributions and Their Relationships to Key Physical Fog Processes Under Different Aerosol Conditions and Evolutionary Stages

The relative dispersion of cloud and fog droplets has significant impacts on aerosol indirect effects, radiative transfer, and microphysical processes. However, previous studies have been mostly concerned with clouds, with limited studies on fog, particularly those that examine the combined influences of all key physical processes and their roles during fog evolution. As such, this study aims to conduct a comprehensive investigation by examining the relationships between relative dispersion and other microphysical variables, as well as the underlying microphysical and dynamic processes, based on field fog campaigns in polluted and clean conditions. In polluted fog, droplet concentrations are higher, leading to smaller droplets and increased dispersion. The correlation between dispersion and droplet volume-mean radius is positive in the polluted fog, but shifts to negative in clean fog. Here, we attribute the difference to various microphysical processes like aerosol activation, condensation, collision-coalescence, and entrainment-mixing. In polluted fog, high aerosol concentrations, low supersaturations, and strong turbulence (entrainment-mixing) provide suitable conditions for the simultaneous occurrence of droplet condensation and aerosol activation, resulting in a positive correlation between dispersion and volume-mean radius, especially during the fog formation stage. In contrast, during the mature stage in clean fog, condensation is dominant with weak aerosol activation leading to a negative correlation between relative dispersion and volume-mean radius. The collision-coalescence process is more active in the mature stage, increasing radii and leading to the negative correlation between dispersion and volume-mean radius. This result sheds new light on understanding the relative dispersion and mechanisms in fog under different aerosol backgrounds.

54 ENVIRONMENTAL SCIENCES

New approach to QCD final-state evolution in processes with massive partons

We present an algorithm for massive parton evolution which is based on the differentially accurate simulation of soft-gluon radiation by means of a nontrivial azimuthal angle dependence of the splitting functions. The kinematics mapping is chosen such as to reflect the symmetry of the final state in soft-gluon radiation and collinear splitting processes. We compute the counterterms needed for a fully differential next-to-leading order matching and discuss the analytic structure of the parton shower in the next-to-leading logarithmic limit. We implement the new algorithm in the numerical code Alaric and present a first comparison to experimental data. Published by the American Physical Society 2024

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

The U.S. DOE ARM User Facility Establishes a New Site for Studies of Land–Aerosol–Cloud Interactions in the Southeastern United States

The U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) user facility has established a new site in the Bankhead National Forest (BNF) in northern Alabama that will gather data on how clouds, the land surface, and aerosols interact at a hierarchy of scales important to understanding and simulating the Earth system. Starting its operations in October 2024, the BNF site provides a multi-year opportunity for scientists to unravel complex land-atmosphere interactions. A suite of ground-based sensors, elevated tower-based instrumentation, and aerial facilities will enable scientists to investigate those interactions from within the canopy to the clouds. The Southeastern United States was recommended by the DOE ARM and its collaborators in the broader community as an important region to address their common scientific questions given the region’s abundant surface-forced convective clouds and mesoscale convective systems that pose ongoing challenges in Earth system models. The region is also home to significant terrain complexity and land-use heterogeneity that will unleash new understanding of anthropogenic and biogenic aerosol processes, boundary-layer aerosol-cloud interactions, and the interactions between the terrestrial ecosystem and coupled aerosol-cloud-radiation processes.

Aerosols

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

Defect Generation and Evolution in Irradiated Epitaxial Films and Heterostructures of Fe 3 O 4 and Cr 2 O 3

Abstract The functionality of nuclear structural materials, sensors, and microelectronics in harsh environments such as radiation relies on understanding defect generation and evolution processes in oxide layers. The initial radiation response of epitaxial thin films of Fe 3 O 4 (111), Cr 2 O 3 (0001), and Fe 3 O 4 (111)/Cr 2 O 3 (0001) heterostructures deposited on Al 2 O 3 (0001) by oxygen‐assisted molecular beam epitaxy and irradiated with 200 keV He + is characterized. X‐ray diffraction and X‐ray absorption near edge spectroscopy showed that the Cr 2 O 3 layers underwent significant lattice expansion and disordering under irradiation, whereas the Fe 3 O 4 layers do not exhibit noticeable changes. In contrast, positron annihilation spectroscopy revealed an evolution of cation vacancy point defects in the Fe 3 O 4 layers into larger vacancy clusters with increasing irradiation, while the cation vacancies in Cr 2 O 3 remained primarily as single vacancies and small clusters. The results suggest that the Fe 3 O 4 lattice can utilize the free volume of the larger vacancy clusters to relax but the small vacancies in the Cr 2 O 3 lattice do not facilitate relaxation. Comparing defect concentrations in the single layer films versus the heterostructure suggests that point defects may cross the interface from Fe 3 O 4 into Cr 2 O 3 . Together, these results enhance the understanding of the initial defect evolution mechanisms in oxide layers in harsh irradiation environments.

36 MATERIALS SCIENCE

Characterization of a CMOS camera based film digitization platform for gated x-ray imaging diagnostics at the National Ignition Facility

Hardened gated x-ray detectors use photographic film as the data recording medium due to its low sensitivity to the high-yield neutron environments at the National Ignition Facility (NIF). The photographic film is digitized with a Photometric Data Systems (PDS) microdensitometer, which measures the film’s optical density. The PDS scanner is able to measure a dynamic range of 0–5 OD; however, raster scanning the film is time consuming and maintenance of the instrument is challenging due to legacy technology. Since film usage at NIF is expected to continue in the foreseeable future, a digitization platform that is faster and more maintainable would benefit the NIF’s current and future operations. Here, this work presents the characterization of the digital transitions (DT) atom, a CMOS camera-based digitization platform that records film data in a single image capture very quickly and has widely available user support. The preliminary results suggest that the DT atom is able to reconstruct exposures accurately enough to be a competitive alternative to the PDS Scanner.

47 OTHER INSTRUMENTATION

Radiation image reconstruction and uncertainty quantification using a Gaussian process prior

We propose a complete framework for Bayesian image reconstruction and uncertainty quantification based on a Gaussian process prior (GPP) to overcome limitations of maximum likelihood expectation maximization (ML-EM) image reconstruction algorithm. The prior distribution is constructed with a zero-mean Gaussian process (GP) with a choice of a covariance function, and a link function is used to map the Gaussian process to an image. Unlike many other maximum a posteriori approaches, our method offers highly interpretable hyperparamters that are selected automatically with the empirical Bayes method. Furthermore, the GP covariance function can be modified to incorporate a priori structural priors, enabling multi-modality imaging or contextual data fusion. Lastly, we illustrate that our approach lends itself to Bayesian uncertainty quantification techniques, such as the preconditioned Crank–Nicolson method and the Laplace approximation. The proposed framework is general and can be employed in most radiation image reconstruction problems, and we demonstrate it with simulated free-moving single detector radiation source imaging scenarios. We compare the reconstruction results from GPP and ML-EM, and show that the proposed method can significantly improve the image quality over ML-EM, all the while providing greater understanding of the source distribution via the uncertainty quantification capability. Furthermore, significant improvement of the image quality by incorporating a structural prior is illustrated.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Spatial Correlations of the Poisson Model for Radiation Transport

Characterizing the relationship between bulk physical properties and mixing in randomly heterogeneous media is a central challenge across many areas of science and engineering. A benchmark model for such studies is the Poisson model, a random tessellation of space by a Poisson process of hyperplanes. In radiation transport studies, the lack of exact expressions for the Poisson model’s spatial multipoint functions has led to approximate methods being used, introducing unquantified sources of error. Here, we recently introduced an exact solution for the Poisson model’s multipoint functions and closely related conditional probability functions (CPFs), providing a new opportunity to understand and reduce these sources of error. In this paper, we enable a more rigorous investigation of radiation transport in stochastic media by applying the recently introduced exact solution for the Poisson model’s CPFs. This paper consists of three main contributions. First, we introduce a unified framework for CPFs of the Poisson model, encompassing the recently introduced exact CPFs as well as the previously introduced atomic mix, nearest-neighbor, and combination CPFs. This framework also includes existing pruning techniques for the approximate CPFs, such as angular exclusion, as well as a novel form of angular exclusion suitable for the exact CPFs. Second, we use the exact CPFs to characterize the spatial regions where each approximate three-point CPF is most accurate, thereby explaining the observed hierarchy of accuracy among the approximate models. Finally, we evaluate material transmittance, reflectance, and flux in a three-dimensional test problem using conditional point sampling, demonstrating the relationship between CPF accuracy and transport simulation accuracy.

Poisson model

Cloud-atmosphere impacts on the central Arctic surface energy budget (Final Report)

This project investigated how clouds and atmosphere-sea ice interactions shape the central Arctic surface energy budget using observations from the MOSAiC expedition and coordinated model experiments. Analyses focused on three themes. First, a new method applied to thermistor string data revealed that snow thermal conductivity is systematically higher than assumed in most models, strongly influencing conductive heat flux and sea ice growth, especially under clear skies. Second, a full annual cycle of surface energy budget observations, combined with detailed cloud microphysical retrievals, demonstrated how cloud regimes regulate radiative, turbulent, and conductive fluxes, driving seasonal contrasts in sea ice energy balance: in winter, radiative forcing elicits strong turbulent and conductive responses, while in summer excess energy is primarily partitioned into surface melt. Third, these observations were used to evaluate and improve regional and global forecast models. While some models captured key Arctic cloud-radiation states, most exhibited persistent deficiencies in representing liquid-containing clouds, snow-on-sea-ice processes, and flux responses to radiative forcing. Together, these results provide unprecedented benchmarks for understanding coupled Arctic processes, improve parameterizations of snow, sea ice, and cloud interactions, and highlight critical pathways by which atmospheric variability drives sea ice change in a rapidly evolving Arctic system. Lastly, the project was a resounding success, resulting in 38 peer-reviewed publications and dozens of presentations, while also supporting an early career scientist.

54 ENVIRONMENTAL SCIENCES

Impacts of Ionizing Radiation on Sulfur Chloride Compounds for Advanced Fuel Cladding Decontamination Processes

Tripling the nation’s nuclear energy capacity is a critical component for significantly increasing energy production and reducing energy costs for American families and businesses. Achieving this vision requires fuel cycle technologies that maximize resource utilization while minimizing radioactive waste generation. Advanced sulfur chloride–based chlorination technologies are being developed to enable efficient recycling of fuel cladding materials, which account for a significant fraction of used nuclear fuel. However, the impacts of ionizing radiation on the longevity and performance of these sulfur chloride compounds are not well established. Here, we will explore the effects of gamma and electron-beam irradiation on the chemical composition of select sulfur chloride reagents, specifically sulfur monochloride (S2Cl2) and thionyl chloride (SOCl2), and the impacts of pre-irradiation on the chlorination yield/chemical dissolution of surrogate aluminum alloy 6061 (AA6061-T6) materials.

38 - RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCL

Vertically Resolved Analysis of the Madden-Julian Oscillation Highlights the Role of Convective Transport of Moist Static Energy

We simulate the Madden-Julian oscillation (MJO) over an aquaplanet with uniform surface temperature using the multiscale modeling framework (MMF) configuration of the Energy Exascale Earth System Model (E3SM-MMF). The model produces MJO-like features that have a similar spatial structure and propagation behavior to the observed MJO. To explore the processes involved in the propagation and maintenance of these MJO-like features, we perform a vertically resolved moist static energy (MSE) analysis for the MJO (Yao et al., 2022, https://doi.org/10.1175/jas-d-20-0254.1). Unlike the column-integrated MSE analysis, our method emphasizes the local production of MSE variance and quantifies how individual physical processes amplify and propagate the MJO's characteristic vertical structure. We find that radiation, convection, and boundary layer (BL) processes all contribute to maintaining the MJO, balanced by the large-scale MSE transport. Furthermore, large-scale dynamics, convection, and BL processes all contribute to the propagation of the MJO, while radiation slows the propagation. Additionally, we perform mechanism-denial experiments to examine the role of radiation and associated feedbacks in simulating the MJO. We find that the MJO can still self-emerge and maintain its characteristic structures without radiative feedbacks. This study highlights the role of convective MSE transport in the MJO dynamics, which was overlooked in the column-integrated MSE analysis.

54 ENVIRONMENTAL SCIENCES

Predicting Radiation-Induced Plutonium Redox Chemistry using Multi-scale Modeling Methods

Over the the last 70 years plutonium (Pu) has been integral in the development of several technologies that have changed the world, yet our fundamental understanding of its chemistry is still far from complete. This is a testament to this element’s unique and complex properties, such as its ability to coexist as multiple oxidation states in aqueous solution. Careful manipulation of plutonium oxidation states is essential in the study and utilization of its rich chemistry. To achieve this level of control, a comprehensive mechanistic understanding of radiation-induced plutonium redox chemistry is critical due to the unavoidable exposure of plutonium to ionizing radiation fields, both inherent and from in-process applications. For this reason, we have developed an experimentally evaluated multi-scale computer model for the prediction of gamma radiation-induced Pu(IV) redox chemistry in concentrated nitric acid solutions (1.0, 3.0, and 6.0 M). Under these acidic, aqueous solution conditions, cobalt-60 gamma irradiation afforded negligible net change in the steady-state oxidation state distribution of Pu(IV). Multi-scale calculations, which are in excellent agreement with experimental data, indicate that this observation is due to radiation-induced redox cycling between Pu(IV) and Pu(III), as achieved by the reduction of Pu(IV) by radiolytic nitrous acid and hydrogen peroxide, and the oxidation of Pu(III) by nitrate and hydroxyl radicals. These radiation-induced redox processes are augmented by plutonium’s inherent disproportionation reactions.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA

Synthesis, Processing, and Use of Isotopically Enriched Epitaxial Oxide Thin Films

Isotopic engineering has emerged as a key approach to study the nucleation, diffusion, phase transitions, and reactions of materials at an atomic level. It aims to uncover mass transport pathways, kinetics, and operational and failure mechanisms of functional materials and devices. Understanding these phenomena leads to deeper insights into important physical processes, such as the transport of ions in energy conversion and storage devices and the role of active sites and supports during heterogeneous catalytic reactions. Likewise, isotopic engineering is being pursued as a means of modifying functionality to enable future technological applications. In this Account, we summarize our recent work employing isotope labeling (e.g., 18 O 2 and 57 Fe) during thin film synthesis and postgrowth processing to reveal growth mechanisms, defect chemistry, and elemental diffusion under working and extreme conditions. Isotope-resolved analysis techniques with nanometer-scale spatial resolution, such as time-of-flight secondary ion mass spectrometry and atom probe tomography, facilitate the accurate quantification of isotopic placement and concentration in our well-defined heterostructures with precisely positioned, isotope-enriched layers. By measuring the nanometer-scale redistribution between natural abundance and isotopically enriched oxygen layers during the deposition of Fe 2 O 3 and Cr 2 O 3 by molecular beam epitaxy, we identified intermixing processes driven by surface adatoms occurring both at the film growth surface and within the first few layers below the surface. Further insights into synthesis mechanisms were gained by studying the tungsten oxide thin films grown by evaporating WO 3 powder in the presence of background 18 O 2 , revealing minimal incorporation of background oxygen during the film formation process. Thermal and radiation-enhanced diffusion in epitaxial Fe and Cr oxides were precisely tracked using 18 O and 57 Fe tracer layers incorporated into model epitaxial oxide thin films. This approach has allowed us to access thermal diffusion behavior at lower temperatures than previously measured, revealing a potential changeover in diffusion mechanism. Understanding radiation-enhanced diffusion in model oxides that represent the surface layers on the structural components of nuclear reactors informs our understanding of their corrosion behavior under irradiation. Isotopic labeling can also provide unique insights into the surface exchange reactions and defect chemistry of electrocatalysts. For instance, tracking the change in 18 O concentration at the surface of an epitaxial LaNiO 3 thin film after the electrocatalytic oxygen evolution reaction revealed the participation of lattice oxygen, confirming a hypothesis that had been proposed previously. Lastly, we highlight a new direction wherein we perform in situ processing studies utilizing isotopic tracers in conjunction with model epitaxial thin films within the atom probe tomography instrument. Additionally, this Account illustrates the great potential of isotopic engineering to enable fundamental mechanistic insights into physical processes and engineer functional properties in epitaxial films, heterostructures, and superlattices.

36 MATERIALS SCIENCE

A machine learning framework for accurate and robust analysis of radiation detector pulses

The microscopic properties of atomic nuclei are used to study various scientific questions. They are essential for understanding the fundamental forces of nature and the chemical evolution of the universe. Detecting decay radiation from radioactive nuclei makes it possible to probe these fundamental nuclear properties. Detector waveform traces may contain additional information about the radiation. Generally, advanced signal processing techniques are needed to extract this additional information, often involving fitting the waveform with model response functions using non-linear least-squares optimization with second-order gradient methods. While this is a powerful technique, it is also computationally expensive, leading to slow processing time, which scales with the volume of data. To address this problem, we have developed a machine learning (ML) approach that infers the characteristics of traces from a model detector response function. In particular, we are interested in classifying whether a single recorded trace consists of one or two pulse constituents and estimating the pulse parameters. Furthermore, our proposed ML method can precisely extract the pulses’ parameters, such as energy and timing information, and accurately classify the pulse multiplicity of a trace. Unlike non-learning-based approaches, our ML approach uses neural networks that are significantly faster at inference, as they do not require any optimization during this stage.

Curve fitting

RCEMIP-II: mock-Walker simulations as phase II of the radiative–convective equilibrium model intercomparison project

Abstract. The radiative–convective equilibrium (RCE) model intercomparison project (RCEMIP) leveraged the simplicity of RCE to focus attention on moist convective processes and their interactions with radiation and circulation across a wide range of model types including cloud-resolving models (CRMs), general circulation models (GCMs), single-column models, global cloud-resolving models, and large-eddy simulations. While several robust results emerged across the spectrum of models that participated in the first phase of RCEMIP (RCEMIP-I), two points that stand out are (1) the strikingly large diversity in simulated climate states and (2) the strong imprint of convective self-aggregation on the climate state. However, the lack of consensus in the structure of self-aggregation and its response to warming is a barrier to understanding. Gaining a deeper understanding of convective aggregation and tropical climate will require reducing the degrees of freedom with which convection can vary. Therefore, we propose phase II of RCEMIP (RCEMIP-II) that utilizes a prescribed sinusoidal sea surface temperature (SST) pattern to provide a constraint on the structure of convection and move one critical step up the model hierarchy. This so-called “mock-Walker” configuration generates features that resemble observed tropical circulations. The specification of the mock-Walker protocol for RCEMIP-II is described, along with example results from one CRM and one GCM. RCEMIP-II will consist of five required simulations: three simulations with the same three mean SSTs as in RCEMIP-I but with an SST gradient and two additional simulations at one of the mean SSTs with different values of the SST gradients. We also test the sensitivity to the imposed SST gradient and the domain size. Under weak SST gradients, unforced self-aggregation emerges across the entire domain, similar to what was found in RCEMIP. As the SST gradient increases, the convective region narrows and is more confined to the warmest SSTs. At warmer mean SSTs and stronger SST gradients, low-frequency variability in the convective aggregation emerges, suggesting that simulations of at least 200 d may be needed to achieve robust equilibrium statistics in this configuration. Simulations with different domain sizes generally have similar mean statistics and convective structures, depending on the value of the SST gradient. The prescribed SST boundary condition is the only difference in the set-up between RCEMIP-II and RCEMIP-I, which enables comparison between the two; however, we also welcome participation in RCEMIP-II from models that did not participate in RCEMIP-I.

Geology

Reconciling calculations and measurements of inverse bremsstrahlung absorption

It was recently shown that the use of Coulomb logarithms appropriate for bremsstrahlung radiation (rather than transport processes) along with corrections for the Langdon effect and ion screening reproduced measurements of collisional absorption in well-characterized underdense plasmas [D. Turnbull et al., Phys. Rev. Lett. 130, 145103 (2023)]. However, it was recognized at the time that the use of the standard absorption-reduction factor from Langdon's seminal paper was inconsistent with the use of Coulomb logarithms that are thermally averaged over a Maxwellian electron-velocity distribution function. A more accurate approach would be to average over the expected super-Gaussian distribution function while accounting for the Gaunt factor's velocity dependence, which somewhat mitigates the Langdon effect; however, at that time, this theory matched the data less well. This conflict is now eliminated with the additional insight that the ionization state of our mid-Z ion species (when present) was lower than had been assumed, as evidenced by the Thomson-scattering data and time-dependent Cretin simulations. We are now able to show that an improved treatment of the Langdon effect provides the best match to data. Otherwise, the prior conclusions remain unchanged. We also show an example of the substantial expected impact to the absorption rate in calculations of indirect-drive hohlraums.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY