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At least 1,405 records · Page 78

Benchtop Autonomous Electrochemical Characterization System for Combinatorial Thin-Film Solid Oxide Electrodes

The design of materials for electrochemical energy conversion is complicated by a vast search space of candidate materials and multifaceted property requirements: multicarrier conductivity, stability, and catalytic activity are all necessary but rarely intersect. Although self-driving laboratories are rapidly rising to address such material optimization problems, the required infrastructure for integrated, large-scale robotic facilities can be cost-prohibitive. Here we develop and evaluate a closed-loop measurement system for efficient screening of proton-conducting oxide electrodes for ceramic fuel cells and electrolyzers, building on top of an existing benchtop instrument and integrating techniques for rapid impedance measurement and automated analysis. This system exemplifies a “minimum viable” self-driving implementation that can deliver substantial benefits with relatively simple infrastructure. Combinatorial thin-film microelectrode libraries are characterized with a recently developed joint time-domain and frequency-domain impedance measurement technique, which provides an order-of-magnitude acceleration relative to conventional impedance spectroscopy. The distribution of relaxation times is extracted from impedance data and analyzed without human intervention. These results feed an active learning and Bayesian optimization process that learns to predict electrochemical impedance as a function of material composition, measurement temperature, oxygen partial pressure, and electrical bias, which further reduces the screening time by tenfold with optimized experimental sequences. We apply this system to Ba⁡(Co,Fe,Zr,Y)⁢O 3−𝛿 combinatorial libraries and evaluate its effectiveness for learning material property trends and optimizing expensive-to-evaluate properties such as activation energy. This offers insights into key methodological aspects of practical autonomous experimentation, including surrogate model validation, cost-aware acquisition functions, and high-throughput data interpretation. Our results demonstrate the efficacy of the system for rapidly gathering information, but also highlight real-world experimental challenges of thin-film degradation and numerical instability in surrogate models.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Accelerated Aging in Electrolytic Capacitors for Prognostics

The focus of this work is the analysis of different degradation phenomena based on thermal overstress and electrical overstress accelerated aging systems and the use of accelerated aging techniques for prognostics algorithm development. Results on thermal overstress and electrical overstress experiments are presented. In addition, preliminary results toward the development of physics-based degradation models are presented focusing on the electrolyte evaporation failure mechanism. An empirical degradation model based on percentage capacitance loss under electrical overstress is presented and used in: (i) a Bayesian-based implementation of model-based prognostics using a discrete Kalman filter for health state estimation, and (ii) a dynamic system representation of the degradation model for forecasting and remaining useful life (RUL) estimation. A leave-one-out validation methodology is used to assess the validity of the methodology under the small sample size constrain. The results observed on the RUL estimation are consistent through the validation tests comparing relative accuracy and prediction error. It has been observed that the inaccuracy of the model to represent the change in degradation behavior observed at the end of the test data is consistent throughout the validation tests, indicating the need of a more detailed degradation model or the use of an algorithm that could estimate model parameters on-line. Based on the observed degradation process under different stress intensity with rest periods, the need for more sophisticated degradation models is further supported. The current degradation model does not represent the capacitance recovery over rest periods following an accelerated aging stress period.

Celaya, Jose R.↗

An uncertainty-focused database approach to extract spatiotemporal trends from qualitative and discontinuous lake-status histories

Changes in lake status are often interpreted as palaeoclimate indicators due to their dependence on precipitation and evaporation. The Global Lake Status Database (GLSDB) has since long provided a standardised synopsis of qualitative lake status over the last 30,000 14C years. Potential sources of uncertainty however are not recorded in the GLSDB. Here we present an updated and improved relational-database framework that incorporates uncertainty in both chronology and the interpretation of palaeoenvironmental data. The database uses peer-reviewed palaeolimnological studies to produce a consensus on qualitative lake-status histories, whose chronologies are revised and standardized through the recalibration of radiocarbon dates and the application of Bayesian age-depth modelling for stratigraphic archives. Quantitative information on absolute water-level elevation is preserved if available from geomorphological sources. We also propose a new probabilistic analytical framework that accounts for these uncertainties to reconstruct synoptic, integrated environmental signals. The process is based on a Monte Carlo algorithm that iteratively samples individual lake-status histories within the limits of their uncertainties to produce many possible scenarios. We then use Recursively-Subtracted Empirical Orthogonal Function analysis to extract dominant patterns of lake-status variability from these scenarios. As a proof of concept, we apply this framework to 67 sites in eastern and southern Africa whose lake-status histories cover part of the late Pleistocene and/or Holocene. We show that, despite the sometimes large temporal and interpretation uncertainties, and the inclusion of highly discontinuous lake-status time series, identifying the major known millennial-scale climatic phases during the last 20,000 years is possible. Our framework was also able to identify an antiphased response between the lake basins in eastern and interior southern Africa to these changes. Here, we propose that our new database and methodology framework serves as a template for efficient lake-status data synthesis, encourages the incorporation of lake-status data in palaeoclimate syntheses, and expands the possibilities for the use of such data in the evaluation of climate models.

58 GEOSCIENCES↗

The extended ‘stellar halo’ of the Ursa Minor dwarf galaxy

Stellar candidates in the Ursa Minor (UMi) dwarf galaxy have been found using a new Bayesian algorithm applied to Gaia EDR3 data. Five of these targets are located in the extreme outskirts of UMi, from ∼5 to 12 elliptical half-light radii (r h ), where r h (UMi) = 17.32 ± 0.11 arcmin, and have been observed with the high-resolution Gemini Remote Access to CFHT ESPaDOnS Spectrograph at the Gemini North telescope. Precise radial velocities (σ RV < 2 km s −1 ) and metallicities (σ [Fe/H] < 0.2 dex) confirm their memberships of UMi. Detailed analysis of the brightest and outermost star (Target 1, at ∼12r h ), yields precision chemical abundances for the α (Mg, Ca, and Ti), odd-Z (Na, K, and Sc), Fe-peak (Fe, Ni, and Cr), and neutron-capture (Ba) elements. With data from the literature and APOGEE data release 17, we find the chemical patterns in UMi are consistent with an outside-in star-formation history that includes yields from core-collapse supernovae, asymptotic giant branch stars, and Type Ia supernovae. Evidence for a knee in the [α/Fe] ratios near [Fe/H] ∼ −2.1 indicates a low star-formation efficiency similar to that in other dwarf galaxies. Detailed analysis of the surface number density profile shows evidence that UMi’s outskirts have been populated by tidal effects, likely as a result of completing multiple orbits around the Galaxy.

79 ASTRONOMY AND ASTROPHYSICS↗

Statistical Uncertainty in Paleoclimate Proxy Reconstructions

A quantitative analysis of any environment older than the instrumental record relies on proxies. Uncertainties associated with proxy reconstructions are often underestimated, which can lead to artificial conflict between different proxies, and between data and models. In this paper, using ordinary least squares linear regression as a common example, we describe a simple, robust and generalizable method for quantifying uncertainty in proxy reconstructions. We highlight the primary controls on the magnitude of uncertainty, and compare this simple estimate to equivalent estimates from Bayesian, nonparametric and fiducial statistical frameworks. We discuss when it may be possible to reduce uncertainties, and conclude that the unexplained variance in the calibration must always feature in the uncertainty in the reconstruction. This directs future research toward explaining as much of the variance in the calibration data as possible. We also advocate for a “data-forward” approach, that clearly decouples the presentation of proxy data from plausible environmental inferences.

58 GEOSCIENCES↗

Improved Characterization of PSC Processes Derived from a Third-Generation CALIOP and MLS Detection and Composition Classification Algorithm

The new 3-year CloudSat and CALIPSO Science Team project described in this poster will use a unique combination of data from the Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) instrument on CALIPSO and the Microwave Limb Sounder (MLS) on Aura, in conjunction with supporting meteorological information and detailed modeling studies, to advance our understanding of polar stratospheric cloud (PSC) processes and their role in ozone depletion. We will develop a third-generation (Gen3) PSC detection and composition algorithm that incorporates a new, more robust two-dimensional, multi-channel CALIOP feature detection scheme (2D-McDA). We will also devise and implement an improved two-dimensional PSC composition classification scheme that utilizes multiple parameters (e.g., CALIOP 532-nm parallel and perpendicular scattering ratios, CALIOP 1064-nm total scattering ratio, MLS HNO3 and H2O, ambient temperature, and temperature histories) in a Bayesian approach to determine the most likely PSC composition and help constrain solid PSC particle number density and size/shape. The combined CALIOP/MLS analyses will allow us to study in detail the full life cycle of PSCs and their resulting impact on gas-phase HNO3 and H2O, which should lead to improved parameterizations of PSC microphysics in global CCMs where detailed particle information is not available. The Gen3 CALIOP PSC algorithm will be a natural stepping-stone toward the analysis of data collected during future spaceborne lidar missions, such as NASA’s Atmosphere Observation System (AtmOS) mission currently scheduled for launch late in this decade. We will also investigate possible trends in PSC occurrence and composition over the entire CALIOP data record and through further comparisons with the Stratospheric Aerosol Measurement (SAM) II solar occultation PSC record from 1979-1989. Finally, we will validate the mountain-wave parameterization and PSC schemes used in the UM-UKCA (Unified Model coupled to the United Kingdom Chemistry and Aerosol module) chemistry-climate model through detailed comparisons with earlier CALIOP PSC data products and those developed under this proposal.

CALIPSO↗

Constraining neutrino oscillation and interaction parameters with the NOvA Near Detector and Far Detector data using Markov Chain Monte Carlo

This thesis reports a constraint of the neutrino oscillation parameters $\Delta m^{2}_{32}$, $\sin^2 \theta_{23}$, and $\delta_{CP}$ using the NuMI Off-Axis $\nu$ Appearance (NOvA) experiment's Near Detector (ND) data and Far Detector (FD) fake data set simultaneously. This thesis also reports a constraint on NOvA's systematic uncertainty model solely with its Near Detector data. The Hamiltonian Monte Carlo algorithm is used to estimate Bayesian Credible Intervals for the oscillation and interaction parameters. The $1\sigma$ Credible Intervals for $\sin^2 \theta_{23}$ are $(0.44, 0.512)$ $\cup$ $(0.536, 0.56)$, for $\Delta m^{2}_{32}$ $(2.41 \times 10^{-3}$ eV$^2,\ 2.52 \times 10^{-3}$ eV$^2)$, and for $\delta_{CP}$ $(0.74\pi,\ 1.1\pi)$ $\cup$ $(1.38\pi,\ 1.58\pi)$. The statistical power of the ND data constrains NOvA's interaction parameters, while the FD fake data constrains the oscillation parameters. This is the first analysis within NOvA to constrain the ND and FD prediction sim ultaneously, and to investigate the neutrino interaction modeling in the context of constraining the oscillation parameters. To constrain the ND data requires a sophisticated understanding of the neutrino interaction modeling and its uncertainties. The interested reader is advised to focus on Chapters 4 and 6, which discuss the ND selection, uncertainties, and ND-only fits to data. The reader interested in oscillation parameter constraints will find this in Chapter 7.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

High-resolution structure of viruses from random diffraction snapshots

The advent of the X-ray free-electron laser (XFEL) has made it possible to record diffraction snapshots of biological entities injected into the X-ray beam before the onset of radiation damage. Algorithmic means must then be used to determine the snapshot orientations and thence the threedimensional structure of the object. Existing Bayesian approaches are limited in reconstruction resolution typically to 1/10 of the object diameter, with the computational expense increasing as the eighth power of the ratio of diameter to resolution.We present an approach capable of exploiting object symmetries to recover three-dimensional structure to high resolution, and thus reconstruct the structure of the satellite tobacco necrosis virus to atomic level. Our approach offers the highest reconstruction resolution for XFEL snapshots to date and provides a potentially powerful alternative route for analysis of data from crystalline and nano-crystalline objects.

59 BASIC BIOLOGICAL SCIENCES↗

Investigating Kinetic Mechanisms of Soot Formation in Plasma Pyrolysis of Methane via Active Learning (Final Technical Report)

Plasma pyrolysis of methane is an effective route for zero-carbon hydrogen production. Yet, soot generated from pyrolysis of hydrocarbons is detrimental to the climate and human health. There is ample experimental and theoretical evidence that suggests polycyclic aromatic hydrocarbons (PAHs) are the molecular precursors to soot particles. The reaction pathways of PAH formation are intricately dependent on a multitude of process parameters, whose kinetic mechanisms are not well-understood in plasma pyrolysis. This project aims to leverage advances in the kinetic modeling of soot formation in combustion, as well as in surrogate modeling and active learning, to systematically investigate the effects of process parameter on the kinetics of PAH formation in plasma pyrolysis of methane. To this end, we propose to use the PAH formation kinetics model developed by the PPPL/PU group based on the well-established ABF and HACA mechanisms, coupled with low-temperature plasma models. We will develop an active learning (AL) framework based on Bayesian optimization to systematically and data-efficiently explore the complex and multivariable parameter space of plasma pyrolysis in order to quantify the effects of plasma and feed parameters on the ABF and HACA kinetic pathways. AL is the branch of machine learning concerned with systematically querying samples from a system (experimental or computational) to train a data-driven model that maps design parameters to a performance criterion. We will use the data generated via AL to perform global sensitivity analysis, combined with uncertainty quantification, to elucidate the impact of different reaction pathways on minimizing formation of soot precursors. This study will result in an improved understanding of kinetics of PAH formation in plasma pyrolysis and can pave the way for more advanced mechanistic studies (e.g., soot nucleation mechanisms). Additionally, the findings will be useful for establishing practical strategies for increasing the pyrolysis efficiency and producing high-grade carbon for synthesis of nanomaterials.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Bayes Analysis and Reliability Implications of Stress-Rupture Testing a Kevlar/Epoxy COPV Using Temperature and Pressure Acceleration

Composite Overwrapped Pressure Vessels (COPVs) that have survived a long service time under pressure generally must be recertified before service is extended. Flight certification is dependent on the reliability analysis to quantify the risk of stress rupture failure in existing flight vessels. Full certification of this reliability model would require a statistically significant number of lifetime tests to be performed and is impractical given the cost and limited flight hardware for certification testing purposes. One approach to confirm the reliability model is to perform a stress rupture test on a flight COPV. Currently, testing of such a Kevlar49 (Dupont)/epoxy COPV is nearing completion. The present paper focuses on a Bayesian statistical approach to analyze the possible failure time results of this test and to assess the implications in choosing between possible model parameter values that in the past have had significant uncertainty. The key uncertain parameters in this case are the actual fiber stress ratio at operating pressure, and the Weibull shape parameter for lifetime; the former has been uncertain due to ambiguities in interpreting the original and a duplicate burst test. The latter has been uncertain due to major differences between COPVs in the database and the actual COPVs in service. Any information obtained that clarifies and eliminates uncertainty in these parameters will have a major effect on the predicted reliability of the service COPVs going forward. The key result is that the longer the vessel survives, the more likely the more optimistic stress ratio model is correct. At the time of writing, the resulting effect on predicted future reliability is dramatic, increasing it by about one "nine," that is, reducing the predicted probability of failure by an order of magnitude. However, testing one vessel does not change the uncertainty on the Weibull shape parameter for lifetime since testing several vessels would be necessary.

Phoenix, S. Leigh↗

Uncertainty quantification given discontinuous climate model response and a limited number of model runs.

Uncertainty quantification in complex climate models is challenged by the sparsity of available climate model predictions due to the high computational cost of model runs. Another feature that prevents classical uncertainty analysis from being readily applicable is bifurcative behavior in climate model response with respect to certain input parameters. A typical example is the Atlantic Meridional Overturning Circulation. The predicted maximum overturning stream function exhibits discontinuity across a curve in the space of two uncertain parameters, namely climate sensitivity and CO2 forcing. We outline a methodology for uncertainty quantification given discontinuous model response and a limited number of model runs. Our approach is two-fold. First we detect the discontinuity with Bayesian inference, thus obtaining a probabilistic representation of the discontinuity curve shape and location for arbitrarily distributed input parameter values. Then, we construct spectral representations of uncertainty, using Polynomial Chaos (PC) expansions on either side of the discontinuity curve, leading to an averaged-PC representation of the forward model that allows efficient uncertainty quantification. The approach is enabled by a Rosenblatt transformation that maps each side of the discontinuity to regular domains where desirable orthogonality properties for the spectral bases hold. We obtain PC modes by either orthogonal projection or Bayesian inference, and argue for a hybrid approach that targets a balance between the accuracy provided by the orthogonal projection and the flexibility provided by the Bayesian inference - where the latter allows obtaining reasonable expansions without extra forward model runs. The model output, and its associated uncertainty at specific design points, are then computed by taking an ensemble average over PC expansions corresponding to possible realizations of the discontinuity curve. The methodology is tested on synthetic examples of discontinuous model data with adjustable sharpness and structure.

54 ENVIRONMENTAL SCIENCES↗

AUTOMATING SPENT FUEL DEFECT DETECTION WITH FUSED DCVD AND GET DATA

Within the safeguards regime, spent fuel monitoring has long been implemented to verify facility declarations. As the number and size of facilities under safeguards increase, so does time spent on highly repetitive spent fuel monitoring, making it an area ripe for automation. However, due to international proliferation concerns, automation must be robust and provide estimates of confidence in the results. Cerenkov Viewing Devices (CVDs) are widely implemented for spent fuel monitoring, but their single defect detection ability is limited. In this research, we augment CVD measurements with Gamma Emission Tomographer (GET) data in order to increase defect detection above the level of either detector method individually. Here we present the development and implementation of a Bayesian data fusion algorithm for classification of individual fuel rods as defects or nondefects across two burn-up and cooling time scenarios. Results show a nearly 75% single defect detection capability with a 10% false positive rate for 17x17 PWR fuel assemblies. The Bayesian framework also enables calculation of uncertainties associated with each classification. These results also show a moderate ability to generalize across both high burn-up and short cooling times as well as low burn-up and long cooling times.

Safeguards, image analysis, metric learning, Data ↗

Analysis of the Westland Data Set

The "Westland" set of empirical accelerometer helicopter data with seeded and labeled faults is analyzed with the aim of condition monitoring. The autoregressive (AR) coefficients from a simple linear model encapsulate a great deal of information in a relatively few measurements; and it has also been found that augmentation of these by harmonic and other parameters call improve classification significantly. Several techniques have been explored, among these restricted Coulomb energy (RCE) networks, learning vector quantization (LVQ), Gaussian mixture classifiers and decision trees. A problem with these approaches, and in common with many classification paradigms, is that augmentation of the feature dimension can degrade classification ability. Thus, we also introduce the Bayesian data reduction algorithm (BDRA), which imposes a Dirichlet prior oil training data and is thus able to quantify probability of error in all exact manner, such that features may be discarded or coarsened appropriately.

Wen, Fang↗

Use and Impact of Covariance Data in the Japanese Latest Adjusted Library ADJ2010 Based on JENDL-4.0

The current status of covariance applications to fast reactor analysis and design in Japan is summarized. In Japan, the covariance data are mainly used for three purposes: (1) to quantify the uncertainty of nuclear core parameters, (2) to identify important nuclides, reactions and energy ranges which are dominant to the uncertainty of core parameters, and (3) to improve the accuracy of core design values by adopting the integral data such as the critical experiments and the power reactor operation data. For the last purpose, the cross section adjustment based on the Bayesian theorem is used. After the release of JENDL-4.0, a development project of the new adjusted group-constant set ADJ2010 was started in 2010 and completed in 2013. In the present paper, the final results of ADJ2010 are briefly summarized. In addition, the adjustment results of ADJ2010 are discussed from the viewpoint of use and impact of nuclear data covariances, focusing on {sup 239}Pu capture cross section alterations. For this purpose three kind of indices, called “degree of mobility,” “adjustment motive force,” and “adjustment potential,” are proposed.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Quantifying the basic reproduction number and underestimated fraction of Mpox cases worldwide at the onset of the outbreak

In 2022, there was a global resurgence of mpox, with different clinical-epidemiological features compared with previous outbreaks. Sexual contact was hypothesized as the primary transmission route, and the community of men having sex with men (MSM) was disproportionately affected. Because of the stigma associated with sexually transmitted infections, the real burden of mpox could be masked. We quantified the basic reproduction number (R 0 ) and the underestimated fraction of mpox cases in 16 countries, from the onset of the outbreak until early September 2022, using Bayesian inference and a compartmentalized, risk-structured (high-/low-risk populations) and two-route (sexual/non-sexual transmission) mathematical model. Machine learning (ML) was harnessed to identify underestimation determinants. Estimated R 0 ranged between 1.37 (Canada) and 3.68 (Germany). The underestimation rates for the high- and low-risk populations varied between 25–93% and 65–85%, respectively. The estimated total number of mpox cases, relative to the reported cases, is highest in Colombia (3.60) and lowest in Canada (1.08). In the ML analysis, two clusters of countries could be identified, differing in terms of attitudes towards the 2SLGBTQIAP+ community and the importance of religion. Given the substantial mpox underestimation, surveillance should be enhanced, and country-specific campaigns against the stigmatization of MSM should be organized, leveraging community-based interventions.

60 APPLIED LIFE SCIENCES↗

On the Need to Align Intent and Implementation in Uncertainty Quantification for Machine Learning

Quantifying uncertainties for machine learning (ML) models is a foundational challenge in modern data analysis. This challenge is compounded by at least two key aspects of the field: (a) inconsistent terminology surrounding uncertainty and estimation across disciplines, and (b) the varying technical requirements for establishing trustworthy uncertainties in diverse problem contexts. In this position paper, we aim to clarify the depth of these challenges by identifying these inconsistencies and articulating how different contexts impose distinct epistemic demands. We examine the current landscape of estimation targets (e.g., prediction, inference, simulation-based inference), uncertainty constructs (e.g., frequentist, Bayesian, fiducial), and the approaches used to map between them. Drawing on the literature, we highlight and explain examples of problematic mappings. To help address these issues, we advocate for standards that promote alignment between the \textit{intent} and \textit{implementation} of uncertainty quantification (UQ) approaches. We discuss several axes of trustworthiness that are necessary (if not sufficient) for reliable UQ in ML models, and show how these axes can inform the design and evaluation of uncertainty-aware ML systems. Our practical recommendations focus on scientific ML, offering illustrative cases and use scenarios, particularly in the context of simulation-based inference (SBI).

Trivedi, Shubhendu [MIT] (ORCID:0000000312374301)↗

In-situ resource utilization for the human exploration of Mars : a Bayesian approach to valuation of precursor missions

The need for sufficient quantities of oxygen, water, and fuel resources to support a crew on the surface of Mars presents a critical logistical issue of whether to transport such resources from Earth or manufacture them on Mars. An approach based on the classical Wildcat Drilling Problem of Bayesian decision theory was applied to the problem of finding water in order to compute the expected value of precursor mission sample information. An implicit (required) probability of finding water on Mars was derived from the value of sample information using the expected mass savings of alternative precursor missions.

water↗

TOWARD A NEW KIND OF ASTEROSEISMIC GRID FITTING

Recent developments in instrumentation (e.g., in particular the Kepler and CoRoT satellites) provide a new opportunity to improve the models of stellar pulsations. Surface layers, rotation, and magnetic fields imprint erratic frequency shifts, trends, and other non-random behavior in the frequency spectra. As our observational uncertainties become smaller, these are increasingly important and difficult to deal with using standard fitting techniques. To improve the models, new ways to compare their predictions with observations need to be conceived. In this paper, we present a completely probabilistic (Bayesian) approach to asteroseismic model fitting. It allows for varying degrees of prior mode identification, corrections for the discrete nature of the grid, and most importantly implements a treatment of systematic errors, such as the 'surface effects'. It removes the need to apply semi-empirical corrections to the observations prior to fitting them to the models and results in a consistent set of probabilities with which the model physics can be probed and compared. As an example, we show a detailed asteroseismic analysis of the Sun. We find a most probable solar age, including a 35 {+-} 5 million year pre-main-sequence phase, of 4.591 billion years, and initial element mass fractions of X{sub 0} = 0.72, Y{sub 0} = 0.264, Z{sub 0} = 0.016, consistent with recent asteroseismic and non-asteroseismic studies.

79 ASTRONOMY AND ASTROPHYSICS↗