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At least 19 records

Non-Contact Mass Density and Thermal Conductivity Measurements of Organic Thin Films Using Frequency–Domain Thermoreflectance

Thin-film organic materials are broadly used to study amorphous stabilization of active pharmaceuticals, control explosive detonation phenomena, and introduce insulation in novel thermal barriers. Their synthesis, however, introduces defects and thickness variations that warrant careful characterization of local thermophysical properties such as thermal conductivity and mass density. In this study, wide bandwidth (200 Hz to 20 MHz) frequency–domain thermoreflectance (FDTR) is demonstrated to simultaneously extract the thermal conductivity and mass density of 1 μm physical vapor-deposited indomethacin films on Si and SiO 2 substrates, as well as 10 and 100 μm films on Si. By assuming a bulk specific heat capacity, mass densities are determined with FDTR measurements of volumetric heat capacity and are in good agreement with the literature, as well as models based upon a dependence on porosity and the kinetic theory for phonons. Lastly, it is found that for broad-band FDTR measurements, insulating substrates provide improved fidelity for the extraction of thermal conductivity and volumetric heat capacity in organic thin films. Overall, this work demonstrates the potential for FDTR as a non-contact method to determine microscale mass density variations across the surface and thickness of organic thin films.

36 MATERIALS SCIENCE↗

Seasonal Seismicity in the Lake Biwa Region of Central Japan Moderately Modulated by Lake Water Storage Changes

Seasonal seismicity in Japan has been observed and attributed to variations induced by hydrological loading, as well as atmospheric and pore-fluid pressure. We examine the seasonal variations of crustal (<15 km depth) and low magnitude (M < 4.5) earthquakes in central Japan near the Biwako-Seigan Fault Zone (BSFZ), and analyze their correlation with the annual hydrological cycle of nearby Lake Biwa, the largest freshwater lake in Japan. The 2002–2018 lake water storage is estimated using water-level gauge and satellite altimetry data. Regional surface mass loading from soil moisture and snow predicted by the Global Land Data Assimilation System is used to augment the lake mass variation. We compute the stress and stressing-rate changes induced by the surface mass loading from lake storage, snow, and soil moisture at seismogenic depth (10 km) along the BSFZ using a finite element model incorporating a 3D Earth structure. The results show that seasonal surface mass loading generates 1–5 kPa peak-to-peak Coulomb stress change and 2.5–15 kPa/year stressing-rate variations on the fault segments along the BSFZ. Two of the four fault segments present significant correlation between local seismicity rate and loading-derived stress and/or stressing rate changes. Among the hydrological load components, lake water, snow, and soil moisture exhibit different annual phases, and the lake water storage dominates the total annual stress changes. Our analysis indicates that seasonal surface hydrological loads, especially lake water variations, modulate the seismicity rate along the BSFZ in central Japan.

58 GEOSCIENCES↗

Design of a prototypical natural circulation water-based reactor cavity cooling system (RCCS) for a pebble-bed generic FHR

A prototypical natural circulation water-based reactor cavity cooling system (RCCS) for the UC Berkeley Mark-1 pebble-bed gFHR is designed based on one-dimensional thermal hydraulics modeling and optimization implemented in an in-house MATLAB code. The model employs a lumped core consisting of fuel pebble and graphite pebble regions, while the graphite reflector, vessel, and RCCS are represented as separate but energy-coupled regions. The model is derived based on steady state energy balance equations accounting for conductive heat transfer from the lumped core to the vessel and subsequent radiative heat transfer to the RCCS and convective heat transfer in the water. Further, mass flow rate is calculated based on momentum and thermal energy balance in the RCCS. Starting with ANL’s water NSTF as baseline, effects of RCCS design parameters such as size of the plate between pipes, pipe diameter, source-to-sink distance, surface emissivity, and pitch from the core are examined in an integral effects framework which accounts for subsequent variation of the mass flow rate, number of pipes, convection coefficient, mean region and surface temperatures, radiative view factors, and water outlet temperature. The importance of including a prototypical reactor design in RCCS design calculations is emphasized as the calculations show that temperature drops from the core to the RCCS fluid to transfer the heat tend to be the limitation not the heat removal capacity of the fluid. A closed-loop design is obtained with capability to safely remove up to 0.72% of the nominal reactor power at maximum estimated peak conditions and 0.40% at shutdown. The design is based on physics calculations and does not account for economic optimization.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Analysis of secondary organic aerosol simulation bias in the Community Earth System Model (CESM2.1)

Organic aerosol (OA) has been considered as one of the most important uncertainties in climate modeling due to the complexity in presenting its chemical production and depletion mechanisms. To better understand the capability of climate models and probe into the associated uncertainties in simulating OA, we evaluate the Community Earth System Model version 2.1 (CESM2.1) configured with the Community Atmosphere Model version 6 (CAM6) with comprehensive tropospheric and stratospheric chemistry representation (CAM6-Chem) through a long-term simulation (1988–2019) with observations collected from multiple datasets in the United States. We find that CESM generally reproduces the interannual variation and seasonal cycle of OA mass concentration at surface layer with a correlation of 0.40 compared to ground observations and systematically overestimates (69%) in summer and underestimates (-19%) in winter. Through a series of sensitivity simulations, we reveal that modeling bias is primarily related to the dominant fraction of monoterpene-formed secondary organic aerosol (SOA), and a strong positive correlation of 0.67 is found between monoterpene emission and modeling bias in the eastern US during summer. In terms of vertical profile, the model prominently underestimates OA and monoterpene concentrations by 37%–99% and 82%–99%, respectively, in the upper air (>500 m) as validated against aircraft observations. Our study suggests that the current volatility basis set (VBS) scheme applied in CESM might be parameterized with monoterpene SOA yields that are too high, which subsequently results in strong SOA production near the emission source area. We also find that the model has difficulty in reproducing the decreasing trend of surface OA in the southeastern US probably because of employing pure gas VBS to represent isoprene SOA which is in reality mainly formed through multiphase chemistry; thus, the influence of aerosol acidity and sulfate particle change on isoprene SOA formation has not been fully considered in the model. This study reveals the urgent need to improve the SOA modeling in climate models.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Elucidating the Impact of Flow on Material-Sensitive Critical Heat Flux and Boiling Heat Transfer Coefficients: An Experimental Study with Various Materials

In this work, steady-state internal flow boiling critical heat flux (CHF) experiments were carried out at 10°C inlet subcooling and atmospheric pressure (84 kPa at an altitude of about 5300 feet) with mass flux ranging from 200 to 2,000 kg/m 2 -s on seven tube materials, including the accident-tolerant fuel cladding candidate FeCrAl (C26M) alloy. At a relatively low flow rate, the sensitivity of CHF to different materials was appreciable (the average difference among the tested materials was 19% at 200 kg/m 2 -s). As the absolute CHF differences stayed constant for higher flow rates, the increased flow rate led to reduced relative CHF differences among the tested materials (average relative difference of 15% at 1,000 kg/m 2 -s). FeCrAl alloy claddings that were oxidized under simulated Light Water Reactor (LWR) conditions yielded CHF comparable to as-received FeCrAl alloy cladding, with less than 1.8% difference. Experimental CHF results imply marginal material sensitivity impacts on the departure from nucleate boiling ratio in steady-state nuclear reactor cores. Yet, for accident progression analysis, material sensitivity may hold importance, as boiling behavior variation at low mass flux is appreciable. Macroscopic material parameters (surface wettability, surface roughness, and thermal properties) do not provide a suitable explanation for observed material-sensitive CHFs. Yet, surface roughness and thermal effusivity revealed power and linear relations, respectively, to the nucleate boiling heat transfer coefficients at low mass flux. At high mass flux, material sensitivity on nucleate boiling heat transfer significantly decreased due to the increased shear stress on boiling surface overwhelming material-related boiling implications.

36 MATERIALS SCIENCE↗

Interface stability of ultrasonic additively manufactured Zircaloy-4 during hydrothermal corrosion

Simulated pressurized water reactor conditions (330 °C, 15.6 MPa, ~20 ppb oxygen) without irradiation were used to investigate the hydrothermal corrosion behavior of ultrasonic additively manufactured Zircaloy-4 up to 1000 h. X-ray computed tomography allowed for visualization of defects from processing and their progression after corrosion experiments. The specimens were found to have clear variability in the mass change data, compared to typical wrought Zircaloy-4 specimens. The variation in the mass change after exposure was attributed to weld defects connected to the specimen surface which allowed ingress of oxidant into the samples. Defects visualized by computed tomography were found via metallography and characterized. In conclusion, ultrasonic additively manufactured Zircaloy-4 was found to have comparable corrosion behavior as wrought Zircaloy-4 for specimens which did not have clear surface defects along weld interfaces.

36 MATERIALS SCIENCE↗

High and Ultra-High Temperature Reaction Kinetics by Single Nanoparticle Mass Spectrometry

Methodology is presented for non-destructive, optically-detected single nanoparticle (NP) mass spectrometry, with the goal of extracting surface reaction kinetics for single NPs at high temperatures. Methods for determining the NP charge, mass, and temperature as a function of time are discussed, and the data are used to extract both the absolute kinetics for mass change, as well as the efficiencies of the surface processes that cause them. Factors that contribute to the uncertainties in absolute and relative mass determination, and in the resulting kinetic parameters, are discussed. The method allows the NP-to-NP variations in initial reactivity to be measured directly, along with the time evolution of reactivity resulting from NP structural/compositional changes that occur under reaction conditions. The strengths and limitations of single nanoparticle mass spectrometry as a high temperature surface kinetics tool are discussed in the context of sublimation and O2 oxidation kinetics experiments for single hafnium (Hf) NPs at temperatures ranging above 2400 K. The Hf oxidation kinetics are compared to analogous oxidation experiments for silicon, graphite, and carbon black NPs. In all four cases, the oxidation chemistry was dominated by processes that result in net mass loss, and the distinct mechanisms responsible are discussed. All four NPs also eventually passivated, i.e., the efficiencies for oxidative etching decreased by at least two orders of magnitude, relative to the initial efficiencies. Furthermore, the passivation mechanisms, which are quite different for carbon, compared to silicon or hafnium, are discussed. Carbon NP passivation is attributed to structural isomerization leading to fully coordinated, fullerene-like NP surfaces, while for silicon and hafnium, passivation results from delayed formation of an oxide layer, triggered by accumulation of oxygen in the NP sub-surface region.

36 MATERIALS SCIENCE↗

Grand Challenges of Hydrologic Modeling for Food-Energy-Water Nexus Security in High Mountain Asia

Climate-influenced changes in hydrology affect water-food-energy security that may impact up to two billion people downstream of the High Mountain Asia (HMA) region. Changes in water supply affect energy, industry, transportation, and ecosystems (agriculture, fisheries) and as a result, also affect the region's social, environmental, and economic fabrics. Sustaining the highly interconnected food-energy-water nexus (FEWN) will be a fundamental and increasing challenge under a changing climate regime. High variability in topography and distribution of glaciated and snow-covered areas in the HMA region, and scarcity of high resolution (in-situ) data make it difficult to model and project climate change impacts on individual watersheds. We lack basic understanding of the spatial and temporal variations in climate, surface impurities in snow and ice such as black carbon and dust that alter surface albedo, and glacier mass balance and dynamics. These knowledge gaps create challenges in predicting where and when the impact of changes in river flow will be the most significant economically and ecologically. In response to these challenges, the United States National Aeronautics and Space Administration (NASA) established the High Mountain Asia Team (HiMAT) in 2016 to conduct research to address knowledge gaps. This paper summarizes some of the advances HiMAT made over the past 5 years, highlights the scientific challenges in improving our understanding of the hydrology of the HMA region, and introduces an integrated assessment framework to assess the impacts of climate changes on the FEWN for the HMA region. The framework, developed under a NASA HMA project, links climate models, hydrology, hydropower, fish biology, and economic analysis. The framework could be applied to develop scientific understanding of spatio-temporal variability in water availability and the resultant downstream impacts on the FEWN to support water resource management under a changing climate regime.

54 ENVIRONMENTAL SCIENCES↗

Annual sea level variations in the Red Sea observed using GNSS

SUMMARY Annual sea level variations in the Red Sea have amplitudes of 15–20 cm as observed using various techniques such as tide gauges, satellite altimetry and recently Gravity Recovery and Climate Experiment (GRACE) satellite data. In this study, we demonstrate that Global Navigation Satellite System (GNSS) observations can also be used to measure the effect of these sea level variations. The extra water mass presses on the seafloor, which causes horizontal and vertical deformations. Using time-series from 10 coastal GNSS stations, we observe annual horizontal and vertical loading displacements with amplitudes of 2–5 mm. When correcting for atmospheric, hydrological and surface water loading and a residual geocentre motion, significant annual signals of approximately 0.5 and 2 mm are still observed for the horizontal and vertical components, respectively. In the northern Red Sea, the observed annual signals and predicted annual sea level loading show good agreement. This confirms that the signal is mostly a result of the variations in water mass and thermal expansion. Furthermore, we conclude that the uncertainties in the hydrological model over Ethiopia and Eritrea influence the loading over the southern Red Sea, which was underestimated in previous studies using GRACE data.

Alothman, A. O.↗

A Scalable Compact Additively Manufactured Molten Salt to Supercritical Carbon Dioxide Heat Exchanger for Solar Thermal Application

Design of an additively manufactured molten salt (MS) to supercritical carbon dioxide (sCO 2 ) primary heat exchanger (PHE) for solar thermal power generation is presented. The PHE is designed to handle temperatures up to 720 °C on the MS side and an internal pressure of 200 bar on the sCO 2 side. In the core, MS flows through a three-dimensional periodic lattice network, while sCO 2 flows within pin arrays. The design includes integrated sCO 2 headers located within the MS flow, allowing for a counterflow design of the PHE. The sCO 2 headers are configured to enable uniform flow distribution into each sCO 2 plate while withstanding an internal pressure of 200 bar and minimizing obstruction to the flow of MS around it. The structural integrity of the design is verified on additively manufactured (AM) 316 stainless steel sub-scale specimens. An experimentally validated, correlation-based sectional PHE core thermofluidic model is developed to study the impact of flow and geometrical parameters on the PHE performance, with varied parameters including the mass flowrate, surface roughness, and PHE dimensions. A process-based cost model is used to determine the impact of parameter variation on build cost. The model results show that a heat exchanger with a power density of 18.6 MW/m 3 (including sCO 2 header volume) and effectiveness of 0.88 can be achieved at a heat capacity rate ratio of 0.8. As a result, the impact of design and AM machine parameters on the cost of the PHE are assessed.

14 SOLAR ENERGY↗

Radial velocity variability and the evolution of hot subdwarf stars

Hot subdwarf stars represent a late and peculiar stage in the evolution of low-mass stars, since they are likely formed by close binary interactions. In this work, we perform a radial velocity (RV) variability study of a sample of 646 hot subdwarfs with multi-epoch radial velocities based on spectra from Sloan Digital Sky Survey (SDSS) and Large Sky Area Multi-Object Fibre Spectroscopic Telescope (LAMOST). The atmospheric parameters and RVs were taken from the literature. For stars with archival spectra but without literature values, we determined the parameters by fitting model atmospheres. In addition, we redetermined the atmospheric parameters and RVs for all the He-enriched sdO/Bs. This broad sample allowed us to study RV-variability as a function of the location in theT eff - log g- and T eff - log n (He)/n (H) diagrams in a statistically significant way. We used the fraction of RV-variable stars and the distribution of the maximum RV variations ΔRV max as diagnostics. Both indicators turned out to be quite inhomogeneous across the studied parameter ranges. A striking feature is the completely dissimilar behaviour of He-poor and He-rich hot subdwarfs. While the former have a high fraction of close binaries, almost no significant RV variations could be detected for the latter. This has led us to the conclusion that there is likely no evolutionary connection between these subtypes. On the other hand, intermediate He-rich- and extreme He-rich sdOB/Os are more likely to be related. Furthermore, we conclude that the vast majority of this population is formed via one or several binary merger channels. Hot subdwarfs with temperatures cooler than ~24 000 K tend to show fewer and smaller RV-variations. These objects might constitute a new subpopulation of binaries with longer periods and late-type or compact companions. The RV-variability properties of the extreme horizontal branch (EHB) and corresponding post-EHB populations of the He-poor hot subdwarfs match and confirm the predicted evolutionary connection between them. Stars found below the canonical EHB at somewhat higher surface gravities show large RV variations and a high RV variability fraction. These properties are consistent with most of them being low-mass EHB stars or progenitors of low-mass helium white dwarfs in close binaries.

79 ASTRONOMY AND ASTROPHYSICS↗

Tailoring Cu-Zr gradient nanoglass structures: Influence of nanoparticle size and cooling rates on glass-glass interfaces

The study of gradient nanoglasses (GNGs) has gained attention due to their unique mechanical properties and potential applications in advanced materials. This study employs molecular dynamics simulations to synthesize a GNG using Cu-Zr metallic glass nanoparticles (NPs) sized from 3 to 15 nm. The NPs were produced by melting and quenching metallic clusters at a relatively slow quench rate of 10 9 K/s. The synthesis of GNG is elucidated along with the characterization of its heterogeneous metallic glass nanostructure. A seamless GNG structure is formed through cold compression of Cu 64 Zr 36 amorphous NPs of varying sizes. The influence of NP size on the GNG structure is investigated, utilizing deeply relaxed NPs, which exhibit a characteristic Cu segregation pattern on their surfaces. The results highlight an increase in structural heterogeneity due to heterogeneous mass transport and the development of local composition and density variations caused by Cu segregation at glass-glass interfaces (GGIs). A reduction in NP size is correlated with decreased Cu atomic displacements and local density at GGIs, suggesting that larger NPs may produce stronger GGIs. This research presents a novel methodology for synthesizing heterogeneous metallic glasses, demonstrating the capacity to control and customize nanostructure heterogeneity through the manipulation of NP sizes and cooling rates. Furthermore, these findings enhance our understanding of structural evolution during nanoglass synthesis and lay the foundation for further exploration in nanomaterial synthesis and characterization.

36 MATERIALS SCIENCE↗

Integration of the fundamental knowledge on solvent-packing interactions into the multiscale framework for column scale design and optimization

The interfacial area, also known as the effective mass transfer area, is a key factor for determining the mass transfer for carbon dioxide (CO 2 ) capture via the chemical absorption process in a packed column, and thus the overall capture efficiency of the packed column. Most of the widely used empirical and semi-empirical models for interfacial area were derived indirectly through absorption mass transfer with simplifications based on fast chemical kinetics. This report presents the comprehensive unique multiscale approach to develop a surrogate model for effective mass transfer area in structured packed columns that accounts local hydrodynamics as well as variation in physical properties, and changes in solid surface characteristics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Comparison of Conventional and Constrained Variational Methods for Computing Large-Scale Budgets and Forcing Fields

Analyses of atmospheric heat and moisture budgets serve as an effective tool to study convective characteristics over a region and to provide large-scale forcing fields for various modeling applications. This paper examines two popular methods for computing large-scale atmospheric budgets: the conventional budget method (CBM) using objectively gridded analyses based primarily on radiosonde data and the constrained variational analysis (CVA) approach which supplements vertical profiles of atmospheric fields with measurements at the top of the atmosphere and at the surface to conserve mass, water, energy, and momentum. Successful budget computations are dependent on accurate sampling and analyses of the thermodynamic state of the atmosphere and the divergence field associated with convection and the large-scale circulation that influences it. Utilizing analyses generated from data taken during Dynamics of the Madden-Julian Oscillation (DYNAMO) field campaign conducted over the central Indian Ocean from October to December 2011, we evaluate the merits of these budget approaches and examine their limitations. While many of the shortcomings of the CBM, in particular effects of sampling errors in sounding data, are effectively minimized with CVA, accurate large-scale diagnostics in CVA are dependent on reliable background fields and rainfall constraints. Finally, for the DYNAMO analyses examined, the operational model fields used as the CVA background state provided wind fields that accurately resolved the vertical structure of convection in the vicinity of Gan Island. However, biases in the model thermodynamic fields were somewhat amplified in CVA resulting in a convective environment much weaker than observed.

54 ENVIRONMENTAL SCIENCES↗

Formation of niobium hydride precipitates in superconducting qubits

We report evidence for the formation of niobium hydride phase within niobium films on silicon substrates in superconducting qubits fabricated at Rigetti Computing. For this study, we combined complementary techniques—including room-temperature and cryogenic atomic force microscopy (AFM), synchrotron x-ray diffraction, and time-of-flight secondary ion mass spectroscopy (ToF-SIMS)—to directly reveal the existence of niobium hydride precipitates on the surface of superconducting qubits. Upon cryogenic cooling, we observed variation in the size and morphology of the hydrides, ranging from small (∼5 nm) irregular shapes to large (∼10–100 nm) domains within the Nb grains, which were fully converted to niobium hydrides. Since niobium hydrides are nonsuperconducting and can easily change in size and location upon different cooldowns to cryogenic temperature, our finding highlights a previously unknown source of decoherence in superconducting qubits. This contributes to quasiparticle losses, offering a potential explanation for changes in qubit performance upon cooldowns. Finally, by leveraging the RF performance of a 3D bulk Nb resonator, we quantify RF dissipation in a superconducting qubit caused by hydrogen concentration variation, and propose a practical engineering pathway to mitigate the formation of Nb hydrides for superconducting qubit applications.

Sung, Zuhawn [Fermi National Accelerator Laborator↗

Broken into Pieces: ATLAS and Aliqa Uma as One Single Stream

We present the first spectroscopic measurements of the ATLAS and Aliqa Uma streams from the Southern Stellar Stream Spectroscopic Survey (S 5), in combination with the photometric data from the Dark Energy Survey and astrometric data from Gaia. From the coherence of spectroscopic members in radial velocity and proper motion, we find that these two systems are extremely likely to be one stream with discontinuity in morphology and density on the sky (the “kink” feature). We refer to this entire stream as the ATLAS-Aliqa Uma stream, or the AAU stream. We perform a comprehensive exploration of the effect of baryonic substructures and find that only an encounter with the Sagittarius dwarf ∼0.5 Gyr ago can create a feature similar to the observed “kink.” In addition, we also identify two gaps in the ATLAS component associated with the broadening in the stream width (the “broadening” feature). These gaps have likely been created by small mass perturbers, such as dark matter halos, as the AAU stream is the most distant cold stream known with severe variations in both the stream surface density and the stream track on the sky. With the stream track, stream distance, and kinematic information, we determine the orbit of the AAU stream and find that it has been affected by the Large Magellanic Cloud, resulting in a misalignment between the proper motion and stream track. Together with the Orphan-Chenab Stream, AAU is the second stream pair that has been found to be a single stream separated into two segments by external perturbation.

79 ASTRONOMY AND ASTROPHYSICS↗

Single-colony MALDI mass spectrometry imaging reveals spatial differences in metabolite abundance between natural and cultured Trichodesmium morphotypes

Trichodesmium, a globally significant N 2 -fixing marine cyanobacterium, forms extensive surface blooms in nutrient-poor ocean regions. These blooms consist of a dynamic assemblage of Trichodesmium species that form distinct colony morphotypes and are inhabited by diverse microorganisms. Trichodesmium colony morphotypes vary in ecological niche, nutrient uptake, and organic molecule release, differentially impacting ocean carbon and nitrogen biogeochemical cycles. Here, we assessed the poorly studied spatial abundance of metabolites within and between three morphologically distinct Trichodesmium colonies collected from the Red Sea. We also compared these results with two morphotypes of the cultivable Trichodesmium strain IMS101. Using matrix-assisted laser desorption/ionization (MALDI) mass spectrometry imaging (MSI) coupled with liquid extraction surface analysis (LESA) tandem mass spectrometry (MS2), we identified and localized a wide range of small metabolites associated with single-colony Trichodesmium morphotypes. Our untargeted MALDI-MSI approach revealed 80 unique features (metabolites) shared between Trichodesmium morphotypes. Discrimination analysis showed spatial variations in 57 shared metabolites, accounting for 62% of the observed variation between morphotypes. The greatest variations in metabolite abundance were observed between the cultured morphotypes compared to the natural colony morphotypes, suggesting substantial differences in metabolite production between the cultivable strain IMS101 and the naturally occurring colony morphotypes that the cultivable strain is meant to represent. This study highlights the variations in metabolite abundance between natural and cultured Trichodesmium morphotypes and provides valuable insights into metabolites common to morphologically distinct Trichodesmium colonies, offering a foundation for future targeted metabolomic investigations.

59 BASIC BIOLOGICAL SCIENCES↗