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At least 271 records · Page 15

Correlated Trajectory Uncertainty for Adaptive Sequential Decision Making

One of the great challenges with decision making tasks on real world systems is the fact that data is sparse and acquiring additional data is expensive. In these cases, it is often crucial to make a model of the environment to assist in making decisions. At the same time, limited data means that learned models are erroneous, making it just as important to equip the model with good predictive uncertainties. In the context of learning sequential decision making policies, these uncertainties can prove useful for informing which data to collect for the greatest improvement in policy performance \citep{mehta2021experimental, mehta2022exploration} or informing the policy about unsure regions of state and action space to avoid during test time \citep{yu2020mopo}. Additionally, assuming that realistic samples of the environment can be drawn, an adaptable policy can be trained that attempts to make optimal decisions for any given possible instance of the environment \citep{ghosh2022offline, chen2021offline}. In this work, we examine the so-called ``probabilistic neural network'' (PNN) model that is ubiquitous in model-based reinforcement learning (MBRL) works. We argue that while PNN models may have good marginal uncertainties, they form a distribution of non-smooth transition functions. Not only are these samples unrealistic and may hamper adaptability, but we also assert that this leads to poor uncertainty estimates when predicting multiple step trajectory estimates. To address this issue, we propose a simple sampling method that can be implemented on top of pre-existing models.We evaluate our sampling technique on a number of environments, including a realistic nuclear fusion task, and find that, not only do smooth transition function samples produce more calibrated uncertainties, but they also lead to better downstream performance for an adaptive policy.

Offline Reinforcement Learning↗

Ion irradiation study of lithium silicates for fusion blanket applications

Here, this study reports on the microstructural and compositional evolutions, deuterium release and lithium loss behavior in lithium silicates. Pellets of biphasic Li 4 SiO 4 and Li 2 SiO 3 were fabricated using hot pressing of powders. Sequential irradiation with Si + , He + and D + ions was performed up to 773 K to emulate one-year 6 Li burnup in 6 Li 4 SiO 4 inside the SlimCS DEMO. Crystalline Li 4 SiO 4 phase was not observed in the irradiated depth region of all the samples in this study. In spite of full amorphization in the near-surface region, Li 2 SiO 3 irradiated to a high dose at 773 K remained crystalline in the damage peak region, suggesting that Li 2 SiO 3 is more irradiation resistant to amorphization than Li 4 SiO 4 . Radiolysis may be primarily responsible for silicate decomposition and amorphization. Data from this study also show that D release from the pellet is very efficient during ion irradiation at 773 K, which is accompanied with a significant Li loss. Thermal annealing for 10 min at 773 K for the room-temperature irradiated pellet leads to a nearly complete D release without an observable Li loss. A concept of Ni coating on tritium breeder materials is discussed with supporting data to minimize Li loss without a significant impact on tritium diffusion and release.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Quantitative Extraction and Mass Spectrometry Analysis at a Single-Cell Level

Quantitative live cell mass spectrometry analysis at a subcellular level requires the precisely controlled extraction of subpicoliter volumes of material from the cell, sensitive analysis of the extracted analytes, and their accurate quantification without prior separation. In this study, we demonstrate that localized electroosmotic extraction provides a direct path to addressing this challenge. Specifically, we demonstrate quantitative mass spectrometry analysis of biomolecules in picoliter volumes extracted from live cells. Electroosmotic extraction was performed using two electrodes and a finely pulled nanopipette with tip diameter of <1 µm containing a hydrophobic electrolyte compatible with mass spectrometry analysis. The electroosmotic drag was used to drive analytes out of the cell into the nanopipette. Analyte molecules extracted both from solutions and cell samples were analyzed using nanoelectrospray ionization (nanoESI) directly from the nanopipette into a mass spectrometer. More than 50 metabolites including sugars and flavonoids were detected in positive mode in 2-5 pL volumes of the cytoplasmic material extracted from Allium cepa. Quantification of the extracted glucose was performed using sequential extraction of a known volume of the aqueous solution containing glucose-d2 standard of known concentration. We found that the ratio of the signal of glucose to glucose-d2 increased linearly with glucose concentration. This observation indicates that the approach developed in this study enables quantitative analysis of small volumes of metabolites extracted from cells. Furthermore, we observed efficient separation of hydrophilic and hydrophobic analytes through partitioning into the aqueous and hydrophobic electrolyte phase, respectively, which provides additional important information on the molecular properties of extracted metabolites.

Yin, Ruichuan↗

Atomic-Scale Characterization and Electronic Properties of Gold-Capped Niobium Films for Superconducting Qubits

Niobium thin films are central to superconducting qubits, but their complex native oxides contribute significantly to microwave losses. A promising mitigation strategy is to suppress oxide formation using engineered thin-film encapsulation layers. Recent experiments have shown that ∼10 nm metallic overlayers on Nb capacitor films can improve the energy relaxation time T1 of transmon qubits. Here, we present a comparative study of Au-capped Nb films fabricated in situ by molecular beam epitaxy and ex situ by sequential deposition benchmarked against bare Nb films. Using complementary structural, chemical, and spectroscopic techniques, we correlate the interface quality with superconducting electronic properties of the Au surface. Low-temperature scanning tunneling spectroscopy (STS) provides spatially resolved quasiparticle density-of-states maps. While both Au-capped Nb samples exhibit large areas with uniform, fully gapped density of states, clear differences emerge between the two interfaces. Compared to in situ Nb-Au, ex situ Nb-Au exhibits a reduced induced superconducting gap, broadened coherence peak, and localized in-gap states, consistent with a residual NbxOy layer at the interface. Supported by complementary structural and chemical analyses, these findings demonstrate that STS directly links nanoscale superconducting properties to interface preparation, highlighting the importance of controlled in situ encapsulation for minimizing dissipation and improving quantum coherence.

Makita, Junki [MIT; Temple U.] (ORCID:000000026889↗

Speciation of Mercury in Sludge Solids: Unwashed Sludge

The objective of this applied research task is to study the type and concentration of mercury compounds found within the contaminated Savannah River Site Liquid Waste System (SRS LWS). A method of selective sequential extraction (SSE), originally developed by (Eurofins) Frontier Global Sciences (FGS) and adapted by the Savannah River National Laboratory (SRNL), utilizes an extraction procedure divided into seven separate tests for different species of mercury. In the SRNL’s modified procedure four of these tests were applied to an unwashed sample of high-level radioactive waste sludge.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Recursive Gaussian Process over graphs for Integrating Multi-timescale Measurements in Low-Observable Distribution Systems

The transition to a smarter grid is empowered by enhanced sensor deployments and smart metering infrastructure in the distribution system. Measurements from these sensors and meters can be used for many applications, including distribution system state estimation (DSSE). However, these measurements are typically sampled at different rates and could be intermittent due to losses during the aggregation process. These multi timescale measurements should be reconciled in real-time to perform accurate grid monitoring. This paper tackles this problem by formulating a recursive multi-task Gaussian process (RGP-G) approach that sequentially aggregates sensor measurements. Specifically, we formulate a recursive multi-task GP with and without network connectivity information to reconcile the multi time-scale measurements in distribution systems. Here, the proposed framework is capable of aggregating the multi-time scale measurements batch-wise or in real-time. Following the aggregation of the multi time-scale measurements, the spatial states of the consistent time-series are estimated using matrix completion based DSSE approach. Simulation results on IEEE 37 and IEEE 123 bus test systems illustrate the efficiency of the proposed methods from the standpoint of both multi time-scale data aggregation and DSSE.

42 ENGINEERING↗

Spectral and Structural Characteristics of Molybdates (Lu{sub 1 –} {sub x}Eu{sub x}){sub 2}(MoO{sub 4}){sub 3}

The structure, the photoluminescence, and IR absorption spectra of solid solutions (Lu{sub 1 ‒} {sub x}Eu{sub x}){sub 2}(MoO{sub 4}){sub 3} have been studied over a wide range of europium concentrations (0 ≤ x ≤ 1). It has been found that there is a correlation between the structure and the spectral characteristics of these compounds. Three types of crystal phases are sequentially changed as the europium concentration increases. The photoluminescence and IR absorption spectra of the monoclinic phase with space group P2{sub 1}/a have been studied for the first time. The glow maximum at a resonant excitation of Eu{sup 3+} ions is shown to be observed in the samples with orthorhombic structure Pba2 at x ~ 0.8. The samples existing in monoclinic P2{sub 1}/a phase at x ~ 0.2 demonstrate the maximum luminescence intensity upon excitation in the band with the charge transfer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Modeling spatial patterns in soil arsenic to estimate natural baseline concentrations

ABSTRACT Arsenic in soil is an important public health concern. Toxicity guidelines and models based on laboratory studies (i.e., U.S. EPA’s Integrated Risk Information System) should consider natural soil As concentrations to avoid unnecessary remediation burdens on society. We used soil and stream sediment samples from the USGS National Geochemical Survey database to assess the spatial distribution of natural As in a 1.16E+5 km2 area. Samples were collected at 348 soil and 144 stream locations, providing approximately one sample for every 290 km2. Sample sites were selected to minimize the potential influence of anthropogenic inputs. Samples were processed using acid digestion of whole samples (concentrated HCl and ascorbic acid) and concentrations were measured using hydride-generation atomic absorption spectrometry. Soil As ranged from 2.0 to 45.6 mg kg-1. Geostatistical techniques were used to model and map the spatial variability of As. The mean and variance at unsampled locations were estimated using sequential Gaussian simulation. Five areas of elevated concentration (> the median of 10 mg kg-1) were identified and the relationships to geologic parent materials, glacial sedimentation patterns, and soil conditions interpreted. Our results showed As concentrations >10 mg kg-1 were common, and >20 mg kg-1 were not unusual for the central and west central portions of Ohio (USA). In contrast, concentrations <4 mg kg-1 were rare. Measured concentrations typically exceeded the soil As human generic screening levels of 0.39 mg/kg (1); the calculated value that corresponds to a cancer risk level of 1 in 1,000,000 for soil ingestion. Because the As content of Ohio soils is similar to many world soils, the USEPA generic soil screening level of 0.39 mg/kg is of little utility. A more useful and practical approach would be the uses of natural background levels. Regional soil As patterns based on geology and biogeochemistry and not political boundaries should be used for soil screening and other risk assessment determinations.

arsenic, background, mapping, geostatistics, toxic↗

Robotic Planning under Uncertainty in Spatiotemporal Environments in Expeditionary Science

In the expeditionary sciences, spatiotemporally varying environments -- hydrothermal plumes, algal blooms, lava flows, or animal migrations -- are ubiquitous. Mobile robots are uniquely well-suited to study these dynamic, mesoscale natural environments. We formalize expeditionary science as a sequential decision-making problem, modeled using the language of partially-observable Markov decision processes (POMDPs). Solving the expeditionary science POMDP under real-world constraints requires efficient probabilistic modeling and decision-making in problems with complex dynamics and observational models. Previous work in informative path planning, adaptive sampling, and experimental design have shown compelling results, largely in static environments, using data-driven models and information-based rewards. However, these methodologies do not trivially extend to expeditionary science in spatiotemporal environments: they generally do not make use of scientific knowledge such as equations of state dynamics, they focus on information gathering as opposed to scientific task execution, and they make use of decision-making approaches that scale poorly to large, continuous problems with long planning horizons and real-time operational constraints. In this work, we discuss these and other challenges related to probabilistic modeling and decision-making in expeditionary science, and present some of our preliminary work that addresses these gaps. We ground our results in a real expeditionary science deployment of an autonomous underwater vehicle (AUV) in the deep ocean for hydrothermal vent discovery and characterization. Our concluding thoughts highlight remaining work to be done, and the challenges that merit consideration by the reinforcement learning and decision-making community.

Preston, Victoria↗

Silver Nanowire-Indium Zinc Oxide Composite Flexible Transparent Conducting Electrodes Made by Spin- coating and Photonic Curing

Realizing high-throughput, low-cost perovskite solar cell (PSC) manufacturing is highly sought-after in photovoltaic (PV) research in recent years. To fully achieve roll-to-roll (R2R) manufacturing of PSCs, it is important to consider the flexible transparent electrode (TE). PET/ITO is a commonly used substrate for making flexible PSCs. When optimizing transparent conducting materials, there is a tradeoff between sheet resistance (Rsh) and optical transparency. Because commercial PET/ITO substrates are made with slow (~1 m/min) vacuum deposition processes, they tend to be expensive. Therefore, it would be advantageous to develop a high-throughput, R2R compatible, solution-deposition approach for fabricating the TE on PET substrates. While various solution-deposition processes, such as blade coating or slot-die coating, can achieve the desired web speed of > 10 m/min, there is still a need to improve the post-deposition annealing step. One promising post-deposition processing technique is intense-pulsed-light processing, also known as photonic curing. Photonic curing delivers short (0.01 – 100 ms) pulses of broadband (200 – 1500 nm) light from a xenon flash lamp to the samples. Any materials in the sample stack that absorb light will convert the impinging light pulse into heat within the sample, which drives changes in the sample (calcination, phase change, crystallization, etc.). Photonic curing has three main advantages over thermal annealing: 1. Faster processing speed (milliseconds or seconds). 2. Compatibility with plastic substrates. 3. Smaller physical footprint and less wasted energy. Since the light pulses are on for a short time, the intensity can be high while the total energy delivered to the sample is low, minimizing damages to the plastic substrates. In this work, a hybrid TE material is fabricated on PET substrates using photonic curing. The hybrid TE material contains a layer of silver nanowires (AgNWs) and a layer of metal-oxide (InOx, ITO, IZO, etc.). The AgNWs increase the light absorbed by the film during the photonic curing process, which leads to higher processing temperatures, possibly improving the conversion of the metal-oxide layer. The AgNWs also enhance the electrical conductivity of the final TE layer after photonic curing. A AgNW and metal-oxide bilayer is formed by spin coating each solution onto the PET substrate sequentially followed by a single photonic curing process. We use average optical transmittance (Tavg) from 400 to 700 nm and average Rsh to evaluate the TE performance. The following photonic curing parameters are varied to optimize Tavg (maximize) and Rsh (minimize): Pulse voltage, pulse envelope, number of micro-pulses, duty cycle, number of pulses, and pulse repetition rate. Preliminarily, we also observe a significant impact on the TE properties by the volume of AgNW deposited during the spin coating deposition step. Using dispense volumes of 80 µL and 20 µL, we achieve samples with Tavg = 73%, Rsh = 19 Ω/sq, and roughness = 9 nm, and Tavg = 83%, Rsh = 58 Ω/sq, and roughness = 5.6 nm, respectively, after photonic curing.

14 SOLAR ENERGY↗

Effect of Sequential Heat Impacts on the Formation of a Stable State of the xLPM–(1 – x)PT Multiferroic Composites

The effect of thermal cycling and sintering temperature on the chemical and thermodynamic stability of the bulk multiferroic xLa{sub 0.7}Pb{sub 0.3}MnO{sub 3}–(1 – x)PbTiO{sub 3} quasi-ceramic and ceramic composites has been experimentally investigated. It is shown that the limiting temperature of the long-term sample firing should not exceed 1070 K. It has been found that sintering at this temperature and/or short-term exposure of the samples at higher temperatures (up to 1220 K) significantly increase the sample compactness, stabilize the thermal expansion, and enhance the quality of the composites. It has been established that the component grain integrity is violated by shrinkage of the samples and a sharp change in their volume during the phase transition of a ferroelectric component.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Monitoring Aqueous Reprocessing Systems for Detection of Facility Misuse

Traditional approaches to material control and accounting at used nuclear fuel reprocessing facilities relies in large part on laboratory-based destructive assay of periodic samples taken from key stages. These techniques are highly accurate, but limited inspection frequency may limit the size and operation of a reprocessing facility. Online monitoring techniques using inline detectors can be applied to fuel reprocessing systems to improve the situational awareness as the facility is operating to provide additional indicators of the evolving state of the facility between normal inspection periods, potentially alerting regulators to the need for additional inspection. The Multi-Isotope Process (MIP) Monitor combines medium-resolution gamma detectors with statistical data analysis techniques to monitor reprocessing systems for anomalous conditions resulting from process control issues or malfeasance. Gamma spectra collected from the H-Canyon reprocessing facility were modeled using principal component analysis to demonstrate the efficacy of the MIP Monitor for detecting notional diversion scenarios.

safeguards, nuclear fuel reprocessing, gamma spect↗

Synthesis and High-Temperature Heat Capacity of Pb{sub 8}La{sub 2}(GeO{sub 4}){sub 4}(VO{sub 4}){sub 2} and Pb{sub 8}Nd{sub 2}(GeO{sub 4}){sub 4}(VO{sub 4}){sub 2} with the Apatite Structure

The Pb{sub 8}La{sub 2}(GeO{sub 4}){sub 4}(VO{sub 4}){sub 2} and Pb{sub 8}Nd{sub 2}(GeO{sub 4}){sub 4}(VO{sub 4}){sub 2} germanatovanadates with the apatite structure have been prepared by solid-state reactions, by sequentially firing stoichiometric mixtures of PbO, La{sub 2}O{sub 3} (Nd{sub 2}O{sub 3}), GeO{sub 2}, and V{sub 2}O{sub 5} in air at temperatures of 773, 873, 973, and 1073 K. The effect of temperature on the heat capacity of the resultant polycrystalline samples has been studied by differential scanning calorimetry at temperatures from 350 to 950 K using polycrystalline samples. The experimental C{sub p}(T) data have been used to evaluate the thermodynamic functions of the lead lanthanum and lead neodymium germanatovanadates.

36 MATERIALS SCIENCE↗

Synchrotron resolved microscale mineralogy and elemental composition of individual plinthic and manganiferous nodules from agricultural soils

Iron and manganese oxides are strong sorbents and elemental scavengers in the environment that can form macroscopic nodules in soils. Despite their importance in the geochemical cycling of nutrients and contaminants, nodules are rarely characterized. When analyzed, they are often combined into bulk samples, obscuring individual characteristics. This study investigates the composition and mineralogy of individual plinthic and manganiferous nodules in soil from cropping systems in the Farming Systems Project in Beltsville, Maryland. Elemental composition indicates the accumulation of contaminants and nutrients, including copper in all nodules and high levels of phosphorus in select nodules. Sequential extractions determine that highly crystalline minerals comprise the nodules, locking away these nutrients and contaminants. Bulk X-ray diffraction (XRD) demonstrated distinct mineralogies in the plinthic and manganiferous nodules, with the former comprised of quartz, goethite, and kaolinite, and the latter consisting of quartz, Mn 2 O 3 , and hematite. Synchrotron and laboratory-based X-ray fluorescence (XRF) mapping gives critical insight into the elemental distribution within the nodules and elucidates spatial elemental associations, including the coupling of manganese and iron in the manganiferous nodules. XRF maps paired with µXRD provide microscale spatial resolution in mineralogy, which resolved several phases not apparent in bulk XRD, manganese’s association with goethite, and minerals indicative of redox transformations, including magnetite and maghemite. These novel results provide critical insight into the microscale mineralogy and individual elemental composition of plinthic and manganiferous nodules, as well as how they alter bulk soil geochemistry in ways largely unaccounted for in research on soil systems.

36 MATERIALS SCIENCE↗

Optimal experimental design: Formulations and computations

Questions of ‘how best to acquire data’ are essential to modelling and prediction in the natural and social sciences, engineering applications, and beyond. Optimal experimental design (OED) formalizes these questions and creates computational methods to answer them. This article presents a systematic survey of modern OED, from its foundations in classical design theory to current research involving OED for complex models. We begin by reviewing criteria used to formulate an OED problem and thus to encode the goal of performing an experiment. We emphasize the flexibility of the Bayesian and decision-theoretic approach, which encompasses information-based criteria that are well-suited to nonlinear and non-Gaussian statistical models. We then discuss methods for estimating or bounding the values of these design criteria; this endeavour can be quite challenging due to strong nonlinearities, high parameter dimension, large per-sample costs, or settings where the model is implicit. A complementary set of computational issues involves optimization methods used to find a design; we discuss such methods in the discrete (combinatorial) setting of observation selection and in settings where an exact design can be continuously parametrized. Finally we present emerging methods for sequential OED that build non-myopic design policies, rather than explicit designs; these methods naturally adapt to the outcomes of past experiments in proposing new experiments, while seeking coordination among all experiments to be performed. Throughout, we highlight important open questions and challenges.

97 MATHEMATICS AND COMPUTING↗

Uncovering multiscale structure-property correlations via active learning in scanning tunneling microscopy

Atomic arrangements and local sub-structures fundamentally influence emergent material functionalities. These structures are conventionally probed using spatially resolved studies and the property correlations are deciphered by a researcher based on sequential explorations, thereby limiting the efficiency and scope. Here we demonstrate a multi-scale Bayesian deep-learning based framework that automatically correlates material structure with its electronic properties using scanning tunneling microscopy (STM) measurements in real-time. Its predictions are used to autonomously direct exploration toward regions of the sample that optimize a given material property. This method is deployed on a low-temperature ultra-high vacuum STM to understand the structure-property relationship in a europium-based semimetal, EuZn 2 As 2 , a promising candidate relevant to magnetism-driven topological phenomena. The framework employs a sparse-sampling approach to efficiently construct the scalar-property space using minimal measurements, about 1–10% of the data required in standard hyperspectral methods. Moreover, we formulate the problem hierarchically across length scales, implementing autonomous workflow to locate mesoscopic and atomic structures that correspond to a target material property. This framework offers the choice to design scalar-property from the spectroscopic data to steer sample exploration. Our findings reveal correlations of the electronic properties unique to surface terminations, local defect density, and point defects.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Why natural monazite never becomes amorphous: Experimental evidence for alpha self-healing

Monazite, a common accessory rare-earth orthophosphate mineral in the continental crust widely used in U-Pb geochronology, holds promise for (U-Th)/He thermochronology and for the immobilization of Pu and minor actinides (MA) coming from spent nuclear fuel reprocessing. Previous results obtained on natural and plutonium-doped monazite have demonstrated the ability of this structure to maintain a crystalline state despite high radiation damage levels. However, the low critical temperature (180 °C), above which amorphization cannot be achieved in natural monazite under ion irradiation, does not explain this old and unsolved paradox: why do natural monazites, independent of their geological history, remain crystalline even when they did not experience any thermal event that could heal the defects? This is what the present study aims to address. Synthetic polycrystals of LaPO 4 -monazite were irradiated sequentially and simultaneously with α particles (He) and gold (Au) ions. Here, our results demonstrate experimentally for the first time in monazite, the existence of the defect recovery mechanism, called α-healing, acting in this structure due to electronic energy loss of α particles, which explains the absence of amorphization in natural monazite samples. This mechanism is critically important for monazite geo- and thermochronology and to design and predictively model the long-term behavior of ceramic matrices for nuclear waste conditioning.

36 MATERIALS SCIENCE↗