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At least 127 records · Page 7

DESI 2024: Constraints on physics-focused aspects of dark energy using DESI DR1 BAO data

Baryon acoustic oscillation data from the first year of the Dark Energy Spectroscopic Instrument (DESI) provide near percent-level precision of cosmic distances in seven bins over the redshift range z=0.1–4.2. Here, this paper is the follow-up to the original DESI BAO cosmology paper [A. G. Adame et al. (DESI Collaboration), arXiv:2404.03002], which considered the conventional w 0 w a cold dark matter (CDM) model. We use the novel DESI data, together with other cosmic probes, to constrain the background expansion history using some well-motivated physical classes of dark energy. In particular, we explore three physics-focused behaviors of dark energy from the equation of state and energy density perspectives: the thawing class (matching many simple quintessence potentials), emergent class (where dark energy comes into being recently, as in phase transition models), and mirage class [where phenomenologically the distance to cosmic microwave background (CMB) last scattering is close to that from a cosmological constant Λ despite dark energy dynamics]. All three classes fit the data at least as well as Λ ⁢CDM, and indeed can improve on it by Δ⁢χ 2 ≈ –5 to –17 for the combination of DESI BAO with CMB and supernova data while having one more parameter. The mirage class does essentially as well as w 0 ⁢w a CDM and exhibits moderate to strong Bayesian evidence preference with respect to Λ⁢ CDM. These classes of dynamical behaviors highlight worthwhile avenues for further exploration into the nature of dark energy.

79 ASTRONOMY AND ASTROPHYSICS↗

Robustness of the Galactic Center excess morphology against masking

The Galactic Center excess (GCE) remains an enduring mystery, with leading explanations being annihilating dark matter or an unresolved population of millisecond pulsars. Analyzing the morphology of the GCE provides critical clues to identify its exact origin. We investigate the robustness of the inferred GCE morphology against the effects of masking, an important step in the analysis where the gamma-ray emission from point sources and the galactic disk are excluded. Using different masks constructed from Fermi point source catalogs and a wavelet method, we find that the GCE morphology, particularly its ellipticity and cuspiness, is relatively independent of the choice of mask for energies above 2–3 GeV. The GCE morphology systematically favors an approximately spherical shape, as expected for dark matter annihilation. Compared to various stellar bulge profiles, a spherical dark matter annihilation profile better fits the data across different masks and galactic diffuse emission backgrounds, except for the stellar bulge profile which provides a similar fit to the data. Modeling the GCE with two components, one from dark matter annihilation and one tracing the Coleman bulge, we find this two-component model outperforms any single component or combinations of dark matter annihilation and other stellar bulge profiles. Uncertainty remains about the exact fraction contributed by each component across different background models and masks. Furthermore, when the Coleman bulge dominates, its corresponding spectrum lacks characteristics typically associated with millisecond pulsars, suggesting that it mostly models the emission from other sources instead of the GCE that is still present and spherically symmetric.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Modification of conventional peak shapes to accurately represent spectral asymmetry: High-Resolution X-ray photoelectron spectra of [C 4 C 1 Pyrr][NTf 2 ] and [C 8 C 1 Im][NTf 2 ] ionic liquids

X-ray photoelectron spectroscopy (XPS) is one of the most widely used techniques for surface characterization. Analysis of XPS data is challenging and requires the analyst to fit the data with synthetic line shapes to reach physically meaningful interpretations. Experimental spectral envelopes, however, are complex and display asymmetric features that are often ignored or attributed to additional chemical components. The high-resolution XPS spectra of [C 4 C 1 Pyrr][NTf 2 ] and [C 8 C 1 Im][NTf 2 ] all exhibit a degree of asymmetry which is systematically observed at the higher binding energy side of photoemission envelopes. Here, we present the development of a refined fitting procedure for XPS spectra of these ionic liquid-based systems which include (a) Shirley background offset necessary to account for the insulator-like region and (b) spectral asymmetry in C 1s and N 1s regions. Further, Shirley and trapezoid components are applied to compensate for inelastic scattering taking place during electron transitions as high as 7.8 eV above the start of the fitting region in C 1s high-resolution spectrum. To demonstrate the fitness of this model, we present an analysis of a 2:1 mixture of [C 4 C 1 Pyrr][NTf 2 ]: [C 8 C 1 Im][NTf 2 ].

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Evolving radon diffusion through earthen barriers at uranium waste disposal sites

Field measurements of Rn-222 fluxes from the tops and bottoms of compacted clay radon barriers were used to calculate effective Rn diffusion coefficients (D Rn ) at four uranium waste disposal sites in the western United States to assess cover performance after more than 20 years of service. Values of D Rn ranged from 7.4 × 10 -7 to 6.0 × 10 -9 m 2 /s, averaging 1.42 × 10 -7 . Water saturation (S W ) from soil cores indicated that there was relatively little control of D Rn by S W , especially at higher moisture levels, in contrast to estimates from most steady-state diffusion models. Further, this is attributed to preferential pathways intrinsic to construction of the barriers or to natural process that have developed over time including desiccation cracks, root channels, and insect burrows in the engineered earthen barriers. A modification to some models in which fast and slow pathway D Rn values are partitioned appears to give a good representation of the data; 4% of the fast pathway was needed to fit the data regression. For locations with high S w and highest D Rn (and fluxes) at each site, the proportion of fast pathway ranged from 1.7% to 34%, but for many locations with lower fluxes, little if any fast pathway was needed.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

A comparison of model validation approaches for echo state networks using climate model replicates

As global temperatures continue to rise, climate mitigation strategies such as stratospheric aerosol injections (SAI) are increasingly discussed, but the downstream effects of these strategies are not well understood. As such, there is interest in developing statistical methods to quantify the evolution of climate variable relationships during the time period surrounding an SAI. Feature importance applied to echo state network (ESN) models has been proposed as a way to understand the effects of SAI using a data-driven model. This approach depends on the ESN fitting the data well. If not, the feature importance may place importance on features that are not representative of the underlying relationships. Typically, time series prediction models such as ESNs are assessed using out-of-sample performance metrics that divide the times series into separate training and testing sets. However, this model assessment approach is geared towards forecasting applications and not scenarios such as the motivating SAI example where the objective is using a data driven model to capture variable relationships. Here, in this paper, we demonstrate a novel use of climate model replicates to investigate the applicability of the commonly used repeated hold-out model assessment approach for the SAI application. Simulations of an SAI are generated using a simplified climate model, and different initialization conditions are used to provide independent training and testing sets containing the same SAI event. The climate model replicates enable out-of-sample measures of model performance, which are compared to the single time series hold-out validation approach. For our case study, it is found that the repeated hold-out sample performance is comparable, but conservative, to the replicate out-of-sample performance when the training set contains enough time after the aerosol injection.

54 ENVIRONMENTAL SCIENCES↗

Impact of Precipitation Parameters on the Specific Surface Area of PuO 2

Controlling the properties of PuO 2 through processing is of vital importance to environmental transport and fate, production of nuclear fuels, nuclear forensic analyses, stockpile stewardship, and storage of nuclear wastes applications. A number of processing conditions have been identified to control final product properties, including specific surface area (SSA), residual carbon content, adsorption of volatile species, morphology, and particle size. In this paper, a novel approach is developed for the prediction of PuO 2 SSA via the synthetic route of Pu(IV) oxalate precipitation followed by calcination. The proposed model utilizes multivariate regression methodology and leave one out formalism to link Savannah River Site (SRS) precipitation and calcination production data to the SSA of the final product. A comparison among the models provides insight into the accuracy and ability to identify variations amongst the processing data. Additionally, the models may also be used to fit new data outside of the parameters explored in a production facility. Finally, the trained model was compared to a similarly trained conventional model form to illustrate the influence of precipitation parameters on the prediction of the final SSA. The models presented here attempt to provide new methods for more accurate prediction of the PuO 2 product properties in a production scale environment for key environmental and nuclear applications.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

When more data hurts: Optimizing data coverage while mitigating diversity-induced underfitting in an ultrafast machine-learned potential

Machine-learned interatomic potentials (MLIPs) are becoming an essential tool in materials modeling. However, optimizing the generation of training data used to parametrize the MLIPs remains a significant challenge. This is because MLIPs can fail when encountering local environments too different from those present in the training data. The difficulty of determining a priori the environments that will be encountered during molecular dynamics simulation necessitates diverse, high-quality training data. Here, this study investigates how training data diversity affects the performance of MLIPs using the Ultra-Fast force field (UF 3 ) to model amorphous silicon nitride. We employ expert and autonomously generated data to create the training data and fit four force field variants to subsets of the data. Our findings reveal a critical balance in training data diversity: insufficient diversity hinders generalization, while excessive diversity can exceed the MLIP's learning capacity, reducing simulation accuracy. Specifically, we found that the UF 3 variant trained on a subset of the training data, in which nitrogen-rich structures were removed, offered vastly better prediction and simulation accuracy than any other variant. By comparing these UF 3 variants, we highlight the nuanced requirements for creating accurate MLIPs, emphasizing the importance of application-specific training data to achieve optimal performance in modeling complex material behaviors.

ab initio molecular dynamics↗

Thermoelastic properties of zircon: Implications for geothermobarometry

Abstract A thermal-pressure equation of state has been determined for zircon (ZrSiO4) that characterizes its thermoelastic behavior at metamorphic conditions. New pressure-volume (P-V) data from a “Mud Tank” zircon have been collected from 1 bar to 8.47(1) GPa using X-ray diffraction, and elastic moduli were measured from room temperature up to 1172 K by resonance ultrasound spectroscopy. These data were fitted simultaneously with temperature-volume (T-V) data from the literature in EosFit7c using a new scaling technique. The parameters of a third-order Birch-Murnaghan EoS with a Mie-Grüneisen-Debye model for thermal pressure have compressional EoS parameters K0T = 224.5(1.2) GPa, K0T' = 4.90(31) with a fixed initial molar volume V0 = 39.26 cm3/mol and thermal parameters γ0 = 0.868(15), q = 2.37(80), and ΘD = 848(38) K. EoS parameters that describe the variation of unit-cell parameters with pressure and temperature were determined using an isothermal-type EoS. This new EoS confirms that zircons are stiffer than garnets and exhibit a much lower thermal expansion. This results in steep isomekes between zircon and garnets, which makes zircon trapped as inclusions in garnets at metamorphic conditions a good piezothermometer.

Geochemistry & Geophysics↗

Exploring the Whole Set of Accurate Sparse Interpretable Models

In data science applications, there are often many models that fit the data well. This phenomenon was called the Rashomon Effect by Leo Breiman. The set of good models is called the Rashomon Set, and the goal of this project is to locate, store, and study the Rashomon sets for classes of interpretable models, including decision trees and generalized additive models.

97 MATHEMATICS AND COMPUTING↗

A Perspective on Traditional and Data Driven Electrochemical Modeling and Analysis

To understand the behavior of electrochemical systems, we need to reduce the dimensionality of the measured current-voltage-time (I-V-t) data by fitting models, thus enabling us to analyze and compare the governing physics. Traditionally, the process for this is an 'expert first' approach: defining the model and its explicit assumptions based on inductive reasoning or empirical observation, fitting small portions of the I-V-t data where assumptions are most valid or carefully designing experiments to enforce key assumptions, and then interpreting the model parameters. However, modern data-driven methods enable a new paradigm: a 'data first' approach, where the latent behaviors governing the system's measured response are identified directly using machine-learning models that optimize both model structure and parameters from the I-V-t data, guaranteeing that the learned model explains as much of the observed system response as possible. After model identification, the model can then be interrogated by an expert to connect observed behaviors with underlying physics. This talk will review several different types of electrochemical analysis (electrochemical impedance, differential voltage-capacity, electrochemical kinetics) and compare the traditional and data-driven methods for analyzing the data.

42 ENGINEERING↗

Encoding nonlinear and unsteady aerodynamics of limit cycle oscillations using nonlinear sparse Bayesian learning

This article investigates the applicability of a recently proposed, nonlinear sparse Bayesian learning (NSBL) algorithm to identify and estimate the complex aerodynamics of limit cycle oscillations. NSBL provides a semi-analytical framework for determining the data-optimal sparse model nested within a (potentially) over-parameterized model. This is particularly relevant to nonlinear dynamical systems where modelling approaches involve the use of physics-based and data-driven components. In such cases, the data-driven components, where analytical descriptions of the physical processes are not readily available, are often prone to overfitting, meaning that the empirical aspects of these models will often involve the calibration of an unnecessarily large number of parameters. While an overparameterized model may fit the observed data well, such models may be inadequate for making predictions in regimes that are different from those wherein the data were recorded. In view of this, it is desirable to not only calibrate the model parameters, but also identify the optimal compromise between data fit and model complexity. In this article, we exhibit the optimal model discovery for an aeroelastic system wherein the structural dynamics are well-known and described by a differential equation model, coupled with a semi-empirical aerodynamic model for laminar separation flutter, resulting in low-amplitude limit cycle oscillations (LCO). To illustrate the performance of the algorithm, in this article, we use synthetic data and demonstrate the ability of the algorithm to correctly rediscover the optimal model and model parameters, given a known data-generating model. The synthetic data are generated from a forward simulation of a known differential equation model with parameters selected so as to mimic the dynamics observed in wind-tunnel experiments. Subsequently, we demonstrate the performance of the algorithm for model selection using noisy LCO data from wind tunnel experiments. As there is no ground truth available for the experimental data case, we provide a comparison between NSBL and Bayesian model selection to validate the results, and demonstrate the use of NSBL as an efficient alternative to traditional methods.

97 MATHEMATICS AND COMPUTING↗

Light Detecting and Ranging (LIDAR) for in-situ heliostat optical error assessment

A system and method for optical assessment of a heliostat includes obtaining a point cloud data representing an image of the heliostat; isolating the data; filtering and fitting the filtered heliostat data to a bounding box; translating the heliostat data to a plane to aid in segmentation; segmenting a plurality of facets of the heliostat fitting each of the segmented facets to a respective plane; generating normal vectors characterizing each of the plurality of facets; and calculating a canting angle associated with each respective facet of the plurality of facets. A heliostat with mirrored facets and a scanner are provided. The scanner captures point cloud data representing the heliostat, which is segmented for each facet. Normal vectors characterize the facets and a canting angle is calculated for the respective facet.

Small, Daniel E.↗

Surface analysis insight note: Differentiation methods applicable to noisy data for determination of sp2‐ versus sp3‐hybridization of carbon allotropes and AES signal strengths

The derivatives of the spectra are commonly used for quantification in Auger Electron Spectroscopy (AES) spectra, while the derivative of the KLL C Auger line has proven to be valuable in obtaining a measure of the relative proportions of sp 2 ‐ and sp 3 ‐hybridization using the D‐parameter in both AES and X‐ray Photoelectron Spectroscopy (XPS). Differentiation of X‐ray Photoelectron Spectroscopy (XPS) and Auger Electron Spectroscopy (AES) spectra by numerical means is presented and illustrated for polymeric, such as PEEK and Nylon, as well as for graphitic materials including highly ordered pyrolytic graphite and graphene oxide. The most commonly available Savitzky–Golay method is explained mathematically and developed through the case of constructing a 5‐point quadratic polynomial convolution kernel suitable for differentiating spectra of adequate signal to noise. The concept of differentiation of spectra where signal to noise is less than adequate is also developed. Two alternative strategies to Savitzky–Golay differentiation are presented, which fit curves to data that allow derivatives to be obtained where Savitzky–Golay would otherwise fail. These alternative methods involve constructing a parametric curve that fits data over the entire energy interval of interest. Derivatives of spectra are then obtained by differentiating these parametric curves directly. A comparison of results for different materials for which specific sp 2 ‐ vs sp 3 ‐hybridized carbon proportions are of interest is used to emphasize the importance of characterizing methods used to differentiate spectra and understanding the characteristics of instrumentation used to measure spectra. The case for using Principal Component Analysis noise reduction with C KLL spectra is made for spectra collected from a heterogeneous graphene oxide sample.

Fairley, Neal↗

Measurement of neutrino oscillations using neutrino and antineutrino beams in the NOvA experiment

NOvA is a long-baseline accelerator neutrino oscillation experiment using the NuMIneutrino beam from Fermilab. Its main physics goals are to probe the 3-flavour oscillationparameters: neutrino mass hierarchy, CP-violating phase dcp and octant of .23 mixingangle by observing electron neutrino appearance and muon neutrino disappearance. Twofunctionally identical detectors are placed off-axis from the centre of the NuMI beam.The near detector at Fermilab is 100 m underground, and the far detector is locatedon the surface at Ash River, 810 km away from the beam source. The initial neutrinobeam spectra are measured using the near detector data and the oscillation parametersare extracted by fitting the observed data to the predicted neutrino spectrum in the fardetector.This thesis is centered around how to improve the sensitivity of |.m232| and .23 measurementsin the muon neutrino disappearance analysis. NOvA will take data for about12 years. The operation of the NOvA experiment for each year costs tens of millions ofdollars, thus it is valuable to maximise the sensitivity of the analysis. Three samples ofmuon neutrino events are studied in this thesis to improve the analysis sensitivities. First,higher energy muon neutrinos are investigated by extending the energy range in NOvA’scurrent standard analysis. Second, for the sample of events used in NOvA’s existing analysis,a new energy estimator which has been developed to improve the neutrino energy resolution is considered. Furthermore, in addition to binning the events as function ofenergy and hadronic energy fraction, three particle identifiers are introduced to separateneutrino events by signal purity to reduce the effects from backgrounds. Third, an additionallower purity sample of muon neutrino charged current (CC) events that look similarto neutral current events and have not been included in NOvA’s existing analyses havebeen studied.This thesis reanalyses NOvA’s data used in the 2020 analysis, corresponding to anexposure of 13.60×1020 protons on target (POT) in the neutrino beam mode recordedfrom February 6, 2014 to March 20, 2020, and 12.50×1020 protons on target in theantineutrino beam mode recorded between June 29, 2016 to February 26, 2019. Thisthesis has implemented a fit to Asimov fake data, generated where sin2 .23 = 0.59 and.m232 = 2.5 × 10-3 eV2. These sensitivity studies show that the uncertainty range of|.m232| at 1 s in the new analysis is reduced by 5.5% and the significance of maximaldisappearance rejection improves by 7.7%, compared to the standard analysis. This isequivalent to adding 11-16% more data. The best fit values of the oscillation parametersfrom fitting to the far detector (FD) data with the new analysis are found to besin2 .23 = 0.568+0.025-0.043 (sin2 .23 = 0.454+0.046-0.026) and .m232 = 2.399+0.055-0.070 × 10-3 eV2 (.m232= -2.427+0.055-0.067 × 10-3 eV2) for the normal (inverted) hierarchy. The difference in thebest fit for sin2 .23 (.m232) between the new analysis and NOvA’s 2020 analysis is around2% (1.4%). The uncertainty range at 1 s for .m232 decrease by 8% (4%) for the normalhierarchy (inverted hierarchy) compared to the standard analysis. The uncertainty rangefor sin2 .23 is close to the standard analysis. This thesis also implements the fit from combiningelectron neutrino appearance and muon neutrino disappearance. The combinedanalysis shows that the best fit values are very close to the standard analysis. However,the uncertainty range of .m232 at 1 s is reduced by 3.7% using the new analysis. The maximaldisappearance significance is not improved in the new analysis, but the new analysisslightly improves the rejection of the disfavoured octant.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Evolving efforts to maintain and improve XPS analysis quality in an era of increasingly diverse uses and users

Based on literature analysis, X-ray photoelectron spectroscopy (XPS) use continues to increase exponentially. This increased use is accompanied by anecdotal reports and systematic analyses indicating a growing presence of significantly flawed data analyses. Recognition of this problem within the surface analysis community has increased with an understanding that both inexperienced users and increased use of XPS outside the surface analysis community contribute to the problem. The XPS community has initiated several efforts to help address the problem, which is not unique to XPS. This paper describes some of the specific problems identified and some of the community efforts intended to address them. Here, we describe activities focused on three specific issues: (i) requests for detailed guides and protocols and bite-sized versions of information for non-experts, (ii) incomplete data and analysis reporting, and (iii) the high rate of peak fitting problems. A 2019 survey identified the need for guides, protocols, and standards to assist XPS users. One set of such guides has been published, and another is being assembled. Providing incremental bites of useful information is the goal of a series of papers on specific challenges to surface analysis with example solutions has been initiated as Notes and Insights papers in Surface and Interface Analysis. Examination of XPS-containing papers finds that information to establish the credibility and reproducibility of XPS results is often very incomplete. Unfortunately, ISO and ASTM standards require an amount of parameter reporting that seems excessive and unrealistic for many research publications. Initial approaches to develop and distribute a graded approach to parameter reporting are briefly described. Multiple efforts are underway to address the high rate of problems associated with photoelectron peak fitting. These include guides to peak fitting, guides to peak identification and fitting for specific elements, and the development of a peak fitting social network. The fitting social network is designed to facilitate interactions between new and experienced XPS users; analysts trying to fit XPS data (for publication or other reasons) can ask questions and establish dynamic conversations. Encouraging and enabling high-quality XPS analysis and reporting requires several different types of effort from all members of the surface and interface analysis community.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Plutonium Speciation and Oxidation State Distributions in the Presence of Citrate

We explored the speciation and kinetics of the Pu(VI)-citrate and Pu(III)-citrate systems (pH m = 2.5–11.0, I = 0.1 M NaCl, T = 23 °C, O 2 (g) < 2 ppm) using ultraviolet–visible–near-infrared (UV–vis–NIR) spectrophotometry, solvent extraction, and PHREEQC modeling. Formation constants were determined for PuO 2 (HcitH)(aq) (log K° 1,1 = 1.09 ± 0.05) and PuO 2 (HcitH)(citH) 3– (log K° 1,2 = -0.20 ± 0.07), and evidence for (PuO 2 ) m (citH –k ) n (OH) x 2m(3+k)n–x was identified under alkaline conditions. Pu(VI) species were found to be less stable in the presence of citrate than in the absence of citrate (t ≤ 168 days); the rate of reduction increased with increasing pH. Further, the direct reduction of Pu(VI) to Pu(IV) was required to fit experimental data in the presence of citrate but did not improve the fit for Pu in the absence of citrate. We also observed increased Pu(III) stability in the presence of citrate (t ≤ 293 days), with higher concentrations of Pu(III) favored at lower pH. Finally, we provide evidence of a radiolysis-driven mechanism for the citrate-mediated reduction of plutonium that involves electron transfer from the oxidative breakdown of citrate. Our work highlights the need to investigate the redox effect of organic ligands on plutonium oxidation states under repository-relevant conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Results on elastic cross sections in proton–proton collisions at $\sqrt{s}$ = 510 GeV with the STAR detector at RHIC

We report results on an elastic cross section measurement in proton–proton collisions at a center-of-mass energy $\sqrt{s}$ = 510 GeV, obtained with the Roman Pot setup of the STAR experiment at the Relativistic Heavy Ion Collider (RHIC). The elastic differential cross section is measured in the four-momentum transfer squared range 0.23 ≤ −t ≤ 0.67 GeV 2 . This is the only measurement of the proton-proton elastic cross section in this t range for collision energies above the Intersecting Storage Rings (ISR) and below the Large Hadron Collider (LHC) colliders. We find that a constant slope B does not fit the data in the aforementioned t range, and we obtain a much better fit using a second-order polynomial for B(t). This is the first measurement below the LHC energies for which the non-constant behavior B(t) is observed. The t dependence of B is also determined using six subintervals of t in the STAR measured t range, and is in good agreement with the phenomenological models. The measured elastic differential cross section dσ/dt agrees well with the results obtained at $\sqrt{s}$ = 540 GeV for proton–antiproton collisions by the UA4 experiment. We also determine that the integrated elastic cross section within the STAR t-range is σ$^{fid}_{el}$ = 462.1 ± 0.9(stat.) ± 1.1(syst.) ± 11.6(scale) μb.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗