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All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Polymorphism influences singlet fission rates in tetracene thin films

Here, we report the effect of crystal structure and crystallite grain size on singlet fission (SF) in polycrystalline tetracene, one of the most widely studied SF and organic semiconductor materials. SF has been comprehensively studied in one polymoprh (Tc I), but not in the other, less stable polymorph (Tc II). Using carefully controlled thermal evaporation deposition conditions and high sensitivity ultrafast transient absorption spectroscopy, we found that for large crystallite size samples, SF in nearly pure Tc II films is significantly faster than SF in Tc I films. We also discovered that crystallite size has a minimal impact on the SF rate in Tc II films, but a significant influence in Tc I films. Large crystallites exhibit SF times of 125 ps and 22 ps in Tc I and Tc II, respectively, whereas small crystallites have SF times of 31 ps and 33 ps. Our results demonstrate first, that attention must be paid to polymorphism in obtaining a self-consistent rate picture for SF in tetracene and second, that control of polymorphism can play a significant role towards achieving a mechanistic understanding of SF in polycrystalline systems. In this latter context we show that conventional theory based on non-covalent tetracene couplings is insufficient, thus highlighting the need for models that capture the delocalized and highly mobile nature of excited states in elucidating the full photophysical picture.

14 SOLAR ENERGY↗
DOE OSTI2012

SELF-ORGANIZATION OF RECONNECTING PLASMAS TO MARGINAL COLLISIONALITY IN THE SOLAR CORONA

We explore the suggestions by Uzdensky and Cassak et al. that coronal loops heated by magnetic reconnection should self-organize to a state of marginal collisionality. We discuss their model of coronal loop dynamics with a one-dimensional hydrodynamic calculation. We assume that many current sheets are present, with a distribution of thicknesses, but that only current sheets thinner than the ion skin depth can rapidly reconnect. This assumption naturally causes a density-dependent heating rate which is actively regulated by the plasma. We report nine numerical simulation results of coronal loop hydrodynamics in which the absolute values of the heating rates are different but their density dependences are the same. We find two regimes of behavior, depending on the amplitude of the heating rate. In the case that the amplitude of heating is below a threshold value, the loop is in stable equilibrium. Typically, the upper and less dense part of a coronal loop is collisionlessly heated and conductively cooled. When the amplitude of heating is above the threshold, the conductive flux to the lower atmosphere required to balance collisionless heating drives an evaporative flow which quenches fast reconnection, ultimately cooling and draining the loop until the cycle begins again. The key elements of this cycle are gravity and the density dependence of the heating function. Some additional factors are present, including pressure-driven flows from the loop top, which carry a large enthalpy flux and play an important role in reducing the density. We find that on average the density of the system is close to the marginally collisionless value.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2013

SALTS AND RADIATION PRODUCTS ON THE SURFACE OF EUROPA

The surface of Europa could contain the compositional imprint of an underlying interior ocean, but competing hypotheses differ over whether spectral observations from the Galileo spacecraft show the signature of ocean evaporates or simply surface radiation products unrelated to the interior. Using adaptive optics at the W. M. Keck Observatory, we have obtained spatially resolved spectra of most of the disk of Europa at a spectral resolution {approx}40 times higher than seen by the Galileo spacecraft. These spectra show a previously undetected distinct signature of magnesium sulfate salts on Europa, but the magnesium sulfate is confined to the trailing hemisphere and spatially correlated with the presence of radiation products like sulfuric acid and SO{sub 2}. On the leading, less irradiated, hemisphere, our observations rule out the presence of many of the proposed sulfate salts, but do show the presence of distorted water ice bands. Based on the association of the potential MgSO{sub 4} detection on the trailing side with other radiation products, we conclude that MgSO{sub 4} is also a radiation product, rather than a constituent of a Europa ocean brine. Based on ocean chemistry models, we hypothesize that, prior to irradiation, magnesium is primarily in the form of MgCl{sub 2}, and we predict that NaCl and KCl are even more abundant, and, in fact, dominate the non-ice component of the leading hemisphere. We propose observational tests of this new hypothesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2010

Fe II EMISSION IN ACTIVE GALACTIC NUCLEI: THE ROLE OF TOTAL AND GAS-PHASE IRON ABUNDANCE

Active galactic nuclei (AGNs) have Fe II emission from the broad-line region (BLR) that differs greatly in strength from object to object. We examine the role of the total and gas-phase iron abundance in determining Fe II strength. Using AGN spectra from the Sloan Digital Sky Survey (SDSS) in the redshift range of 0.2 < z < 0.35, we measure the Fe/Ne abundance of the narrow-line region (NLR) using the [Fe VII]/[Ne V] line intensity ratio. We find no significant difference in the abundance of Fe relative to Ne in the NLR as a function of Fe II/H{beta}. However, the [N II]/[S II] ratio increases by a factor of 2 with increasing Fe II strength. This indicates a trend in N/S abundance ratio, and by implication in the overall metallicity of the NLR gas, with increasing Fe II strength. We propose that the wide range of Fe II strength in AGN largely results from the selective depletion of Fe into grains in the low ionization portion of the BLR. Photoionization models show that the strength of the optical Fe II lines varies almost linearly with gas-phase Fe abundance, while the ultraviolet Fe II strength varies more weakly. Interstellar depletions of Fe can be as large as 2 orders of magnitude, sufficient to explain the wide range of optical Fe II strength in AGNs. This picture is consistent with the similarity of the BLR radius to the dust sublimation radius and with indications of Fe II emitting gas flowing inward from the dusty torus.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2018

Processes of interaction of laser radiation with porous transparent materials during their ablation

The effect of ytterbium fibre laser radiation with λ = 1.07 μm on the pressed micropowders of transparent oxides and fluorides (CaF{sub 2}, Y{sub 2}O{sub 3}, Al{sub 2}O{sub 3}, YSZ, etc.) having low absorption coefficients is theoretically studied. Using the numerical modelling, it is established that the radiation scattering in the medium of particles 0.5 – 4.6 μm in diameter leads to the concentration of radiation in the local regions of the medium, with the intensity level exceeding the intensity of the incident radiation (0.46 MW cm{sup −2}) by many times. It is shown that with the growth of the refractive index n of the material from 1.38 (MgF{sub 2}) to 2.12 (YSZ) the intensity of radiation in the region of the strongest local maximum increases from 3.8 to 31 MW cm{sup −2}. In our opinion, this factor can be dominant in determining the possibility of achieving the ablation of such a medium by means of the radiation having an intensity of no greater than 1 MW cm{sup −2}. This hypothesis is experimentally checked by the example of preparing a nanopowder of CaF{sub 2} (n = 1.43) and 1 % Nd : Y{sub 2}O{sub 3} (n = 1.91) by evaporating the pressed target with the porosity 50 % by the continuous-wave radiation of the ytterbium fibre laser with the power 600 W and the intensity 0.4 MW cm{sup −2}. Inside the CaF{sub 2} target, the scattered radiation intensity is smaller than the optical breakdown threshold, and the target is not evaporated. Under the same conditions, the target made of higher-melting 1 % Nd : Y{sub 2}O{sub 3} evaporates well, and the efficiency of the nanopowder production amounts to 23 g h{sup −1}. (interaction of laser radiation with matter)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Understanding the distinct impacts of MCS and non-MCS rainfall on the surface water balance in the central US using a numerical water-tagging technique

Warm-season rainfall associated with mesoscale convective systems (MCSs) in the central US is characterized by higher intensity and nocturnal timing compared to rainfall from non-MCS systems, suggesting their potentially different footprints on the land surface. To differentiate the impacts of MCS and non-MCS rainfall on the surface water balance, a water tracer tool embedded in the Noah land surface model with multi-parameterization options (WT-Noah-MP) is used to numerically “tag” water from MCS and non-MCS rainfall separately during April to August (1997-2018) and track their transit in the terrestrial system. From the water-tagging results, over 50% of warm-season rainfall leaves the surface-subsurface system through evapotranspiration by the end of August, but non-MCS rainfall contributes a larger fraction. However, MCS rainfall plays a more important role in generating surface runoff. These differences are mostly attributed to the rainfall intensity differences. The higher intensity MCS rainfall tends to produce more surface runoff through infiltration excess flow and drives a deeper penetration of the rainwater into the soil. Over 70% of the top 10 percentile runoff is contributed by MCS rainfall, demonstrating its important contribution to local flooding. In contrast, lighter intensity non-MCS rainfall resides mostly in the top layer and contributes more to evapotranspiration through soil evaporation. Diurnal timing of rainfall has negligible effects on the flux partitioning for both MCS and non-MCS rainfall. Differences in soil moisture profiles for MCS and non-MCS rainfall and the resultant evapotranspiration suggest differences in their roles in soil moisture-precipitation feedbacks and ecohydrology.

Hu, Huancui↗
DOE OSTI2011

The impact of water flow configuration on crystallisation in LiBr/H2O absorption water heater

Lithium Bromide (LiBr) strong solution entering the absorber tends to crystallise when the absorber temperature is increased for a fixed evaporating pressure. This is considered the key technical barrier for the development of a LiBr absorption heat pump water heater. There are several approaches to avoid the crystallisation problem, such as chemical crystallisation inhibitors, heat and mass transfer enhancement and thermodynamic cycle modification. This paper investigates and compares two flow configurations of LiBr absorption heat pump water heater to evaluate the allowable operating conditions for each. The simulation results indicated that introducing the process water through the absorber first results in lower absorber temperature and hence less tendency for crystallisation.

42 ENGINEERING↗
DOE OSTI2013

Nevada National Security Site 2012 Waste Management Monitoring Report Area: 3 and Area 5 Radioactive Waste Management Sites

Environmental monitoring data are collected at and around the Area 3 and Area 5 Radioactive Waste Management Sites (RWMSs) at the Nevada National Security Site (NNSS). These data are associated with radiation exposure, air, groundwater, meteorology, and vadose zone. This report summarizes the 2012 environmental data to provide an overall evaluation of RWMS performance and to support environmental compliance and performance assessment (PA) activities. Some of these data (e.g., radiation exposure, air, and groundwater) are presented in other reports (National Security Technologies, LLC, 2012; 2013a; 2013b). Direct radiation monitoring data indicate exposure levels at the RWMSs are within the range of background levels measured at the NNSS. Slightly elevated exposure levels outside the Area 3 RWMS are attributed to nearby historical aboveground nuclear weapons tests. Air monitoring data show tritium concentrations in water vapor and americium and plutonium concentrations in air particles are only slightly above detection limits and background levels. The measured levels of radionuclides in air particulates and moisture are below Derived Concentration Standards for these radionuclides. Groundwater monitoring data indicate the groundwater in the uppermost aquifer beneath the Area 5 RWMS is not impacted by RWMS operations. Results of groundwater analysis from wells around the Area 5 RWMS were all below established investigation levels. Leachate samples collected from the leachate collection system at the mixed low-level waste cell were below established contaminant regulatory limits. The 133.9 millimeters (mm) (5.27 inches [in.]) of precipitation at the Area 3 RWMS during 2012 is 12% below the average of 153.0 mm (6.02 in.), and the 137.6 mm (5.42 in.) of precipitation at the Area 5 RWMS during 2012 is 11% below the average of 122.4 mm (4.82 in.). Water balance measurements indicate that evapotranspiration from the vegetated weighing lysimeter dries the soil and prevents downward percolation of precipitation more effectively than evaporation from the bare-soil weighing lysimeter. Automated vadose zone monitoring on Area 5 and Area 3 RWMS cell covers show no evidence of precipitation percolating through the cover to the waste. Moisture from precipitation did not percolate below 60 centimeters (cm) (2 feet [ft]) in the vegetated final cover on the U-3ax/bl disposal unit at the Area 3 RWMS, and moisture from precipitation and irrigation did not percolate below 45 cm (1.5 ft) on the 92-Acre Area final cover. Irrigation was applied to this cover for seed germination and plant growth. During 2012, there was no drainage through 2.4 meters (8 ft) of soil from the Area 3 drainage lysimeters that received only natural precipitation. Twenty percent of the applied precipitation and irrigation drained from the bare-soil drainage lysimeter that received 3 times natural precipitation. All 2012 monitoring data indicate that the Area 3 and Area 5 RWMSs are performing within expectations of the model and parameter assumptions for the facility PAs.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2014

Nevada National Security Site 2013 Waste Management Monitoring Report Area 3 and Area 5 Radioactive Waste Management Site

Environmental monitoring data are collected at and around the Area 3 and Area 5 Radioactive Waste Management Sites (RWMSs) within the Nevada National Security Site (NNSS). These data are associated with radiation exposure, air, groundwater, meteorology, and vadose zone. This report summarizes the 2013 environmental data to provide an overall evaluation of RWMS performance and to support environmental compliance and performance assessment (PA) activities. Some of these data (e.g., radiation exposure, air, and groundwater) are presented in other reports (National Security Technologies, LLC, 2013; 2014a; 2014b). Direct radiation monitoring data indicate exposure levels at the RWMSs are within the range of background levels measured at the NNSS. Slightly elevated exposure levels outside the Area 3 RWMS are attributed to nearby historical aboveground nuclear weapons tests. Air monitoring data show tritium concentrations in water vapor and americium and plutonium concentrations in air particles are close to detection limits and background levels. The measured levels of radionuclides in air particulates and moisture are below Derived Concentration Standards for these radionuclides. Groundwater monitoring data indicate the groundwater in the uppermost aquifer beneath the Area 5 RWMS is not impacted by RWMS operations. Results of groundwater analysis from wells around the Area 5 RWMS were all below established investigation levels. Leachate samples collected from the leachate collection system at the mixed low-level waste cell were below established contaminant regulatory limits. The 105.8 millimeters (mm) (4.17 inches [in.]) of precipitation at the Area 3 RWMS during 2013 is 30% below the average of 150.3 mm (5.92 in.), and the 117.5 mm (4.63 in.) of precipitation at the Area 5 RWMS during 2013 is 5% below the average of 123.6 mm (4.86 in.). Water balance measurements indicate that evapotranspiration from the vegetated weighing lysimeter dries the soil and prevents downward percolation of precipitation more effectively than evaporation from the bare-soil weighing lysimeter. Automated vadose zone monitoring on Area 5 and Area 3 RWMS cell covers show no evidence of precipitation percolating through the cover to the waste. Moisture from precipitation did not percolate below 60 centimeters (cm) (2 feet [ft]) in the vegetated final cover on the U-3ax/bl disposal unit at the Area 3 RWMS, and moisture from precipitation and irrigation did not percolate below 45 cm (1.5 ft) on the 92-Acre Area final cover. Irrigation was applied to this cover for seed germination and plant growth. During 2013, there was no drainage through 2.4 meters (8 ft) of soil from the Area 3 drainage lysimeters that received only natural precipitation. Twenty percent of the applied precipitation and irrigation drained from the bare-soil drainage lysimeter that received 3-times natural precipitation. All 2013 monitoring data indicate that the Area 3 and Area 5 RWMSs are performing within expectations of the model and parameter assumptions for the facility PAs.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

A novel approach to partitioning evapotranspiration into evaporation and transpiration in flooded ecosystems

Reliable partitioning of micrometeorologically measured evapotranspiration (ET) into evaporation (E) and transpiration (T) would greatly enhance our understanding of the water cycle and its response to climate change related shifts in local-to-regional climate conditions and rising global levels of vapor pressure deficit (VPD). While some methods on ET partitioning have been developed, their underlying assumptions make them difficult to apply more generally, especially in sites with large contributions of E. Here, we report a novel ET partitioning method using artificial neural networks (ANNs) in combination with a range of environmental input variables to predict daytime E from nighttime ET measurements. The study uses eddy covariance data from four restored wetlands in the Sacramento-San Joaquin Delta, California, USA, as well as leaf-level T data for validation. The four wetlands vary in their vegetation make-up and structure, representing a range of ET conditions. The ANNs were built with increasing complexity by adding the input variable that resulted in the next highest average value of model testing R 2 across all sites. The order of variable inclusion (and importance) was: VPD > gap-filled sensible heat flux (H_gf) > air temperature (T air ) > friction velocity (u * ) > other variables. The model using VPD, H_gf, T air , and u * showed the best performance during validation with independent data and had a mean testing R 2 value of 0.853 (averaged across all sites, range from 0.728 to 0.910). In comparison to other methods, our ANN method generated T/ET partitioning results which were more consistent with CO 2 exchange data especially for more heterogeneous sites with large E contributions. Further, our method improves the understanding of T/ET partitioning. While it may be particularly suited to flooded ecosystems, it can also improve T/ET partitioning in other systems, increasing our knowledge of the global water cycle and ecosystem functioning.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2016

Enhancement of the droplet nucleation in a dense supersaturated Lennard-Jones vapor

The vapor–liquid nucleation in a dense Lennard-Jones system is studied analytically and numerically. A solution of the nucleation kinetic equations, which includes the elementary processes of condensation/evaporation involving the lightest clusters, is obtained, and the nucleation rate is calculated. Based on the equation of state for the cluster vapor, the pre-exponential factor is obtained. The latter diverges as a spinodal is reached, which results in the nucleation enhancement. The work of critical cluster formation is calculated using the previously developed two-parameter model (TPM) of small clusters. A simple expression for the nucleation rate is deduced and it is shown that the work of cluster formation is reduced for a dense vapor. This results in the nucleation enhancement as well. To verify the TPM, a simulation is performed that mimics a steady-state nucleation experiments in the thermal diffusion cloud chamber. The nucleating vapor with and without a carrier gas is simulated using two different thermostats for the monomers and clusters. The TPM proves to match the simulation results of this work and of other studies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

NuSTAR OBSERVATIONS AND BROADBAND SPECTRAL ENERGY DISTRIBUTION MODELING OF THE MILLISECOND PULSAR BINARY PSR J1023+0038

We report the first hard X-ray (3-79 keV) observations of the millisecond pulsar (MSP) binary PSR J1023+0038 using NuSTAR. This system has been shown transiting between a low-mass X-ray binary (LMXB) state and a rotation-powered MSP state. The NuSTAR observations were taken in both LMXB state and rotation-powered state. The source is clearly seen in both states up to ∼79 keV. During the LMXB state, the 3-79 keV flux is about a factor of 10 higher than in the rotation-powered state. The hard X-rays show clear orbital modulation during the X-ray faint rotation-powered state but the X-ray orbital period is not detected in the X-ray bright LMXB state. In addition, the X-ray spectrum changes from a flat power-law spectrum during the rotation-powered state to a steeper power-law spectrum in the LMXB state. We suggest that the hard X-rays are due to the intrabinary shock from the interaction between the pulsar wind and the injected material from the low-mass companion star. During the rotation-powered MSP state, the X-ray orbital modulation is due to Doppler boosting of the shocked pulsar wind. At the LMXB state, the evaporating matter of the accretion disk due to the gamma-ray irradiation from the pulsar stops almost all the pulsar wind, resulting in the disappearance of the X-ray orbital modulation.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Thermal Energy Grid Storage (TEGS) Using Multi-Junction Photovoltaics (MPV) (Final Technical Report)

The project aimed to develop a thermal energy storage battery that converts electricity to heat and stores heat at ultra-high temperatures (>2000°C) in graphite blocks. The thermal battery discharge uses TPV cells that directly convert thermal energy to electrical energy without any moving parts. All components of this technology were successfully demonstrated at the laboratory scale in this project. Development of extremely low cost (< $20/kWh) grid level energy storage is a crucial necessity to reach high penetrations of renewables. The thermal battery technology developed in this project is expected to meet the cost targets that would enable full renewable penetration. The project focused on four key aspects of this technology: Converting electricity to ultra-high temperature heat: This was done through development of graphite Joule heaters. Major issues related to arcing, heater evaporation and deterioration due to long term oxidation were addressed to ensure lifetime exceeding the service lifetime of the battery. Converting ultra-high temperature heat back to electricity: This was done through development of beyond state-of-the-art TPV cells. We demonstrated energy conversion efficiency of >40% that is a world record and exceeds the average energy conversion efficiency of turbines in the USA. The findings are peer-reviewed and published in Nature, and received a wide media attention globally. Protecting the TPV cells to ensure lifetime: Deposition of volatilized material, such as sublimated material or particles, on the TPV cell could greatly reduce the efficiency and lifetime of the TPV cells by blocking their view to the heat source and causing cell overheating. In this project we developed and demonstrated an approach that reduces the deposition rate, ensuring long > 30 year life. Technoeconomic feasibility and commercialization: In collaboration with the project’s technical advisory board, we developed a technoeconomic model. The model shows that, at large scales (> 1GWh) the thermal battery technology is projected to reach a cost of energy stored below $10/kWh-e, with a cost per unit power < $0.5/W-e and a roundtrip efficiency of 50%. These results, along with the technical achievements in the project led to the creation of a startup company (i.e., Fourth Power) that is pursuing commercialization of the technology.

25 ENERGY STORAGE↗
DOE OSTI2016

Parameterizing microphysical effects on variances and covariances of moisture and heat content using a multivariate probability density function: a study with CLUBB (tag MVCS)

Abstract. Microphysical processes, such as the formation, growth, and evaporation of precipitation, interact with variability and covariances (e.g., fluxes) in moisture and heat content. For instance, evaporation of rain may produce cold pools, which in turn may trigger fresh convection and precipitation. These effects are usually omitted or else crudely parameterized at subgrid scales in weather and climate models.A more formal approach is pursued here, based on predictive, horizontally averaged equations for the variances, covariances, and fluxes of moisture and heat content. These higher-order moment equations contain microphysical source terms. The microphysics terms can be integrated analytically, given a suitably simple warm-rain microphysics scheme and an approximate assumption about the multivariate distribution of cloud-related and precipitation-related variables. Performing the integrations provides exact expressions within an idealized context.A large-eddy simulation (LES) of a shallow precipitating cumulus case is performed here, and it indicates that the microphysical effects on (co)variances and fluxes can be large. In some budgets and altitude ranges, they are dominant terms. The analytic expressions for the integrals are implemented in a single-column, higher-order closure model. Interactive single-column simulations agree qualitatively with the LES. The analytic integrations form a parameterization of microphysical effects in their own right, and they also serve as benchmark solutions that can be compared to non-analytic integration methods.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Sr-Nd-Pb isotope systematics of Australasian tektites: Implications for the nature and composition of target materials and possible volatile loss of Pb

The Australasian tektite (AAT) strewn field is the largest strewn field on the Earth with about ~10–30% coverage, both land and ocean, but a clearly identified source impact crater is absent despite the young age of AAT of ca. 790 ka. A genetic link between the Australasian tektites and their unequivocal parental materials is therefore largely impossible to establish. Nevertheless, the nature of the parental materials and the extent of volatilization can be constrained using the splash form tektites, carrying the chemical signatures of high-temperature processes, and the layered (so-called Muong Nong-type) tektites, which are less chemically homogenized and exceptionally abundant in the AAT field. New high-precision Sr, Nd and Pb isotopic measurements were obtained for a chemically and petrographically well-characterized suite of AAT, which included the Muong Nong-type (MN-AAT) with precisely known field locations in Laos and splash forms (SF-AAT) from different parts of the strewn field. Additionally, optically dark and light zones of the MN-AAT were also separately analyzed. Homogeneous ε Nd values from -11.8 to -11.2, combined with a narrow range of two-stage Nd model ages from 1.67 to 1.72 Ga for the entire AAT suite, point to a well-mixed source, in terms of REE, of the crustal segment from which the sedimentary material for tektites was ultimately derived. The Sr isotopic data largely overlap for SF-AAT and MN-AAT ( 87 Sr/ 86 Sr = 0.71636–0.72021) and indicate Paleozoic to Mesozoic sedimentary parentage. However, late Neogene to early Quaternary re-deposition and formation of a thick silt-sized sedimentary section with vertical stratification is required to comply with 10Be data. Lead isotope systematics documents at least three different components which can perhaps be represented by different mineral phases, such as feldspar, zircon, organic matter adsorbed on young sediments etc., sorted during fluvial transport and final deposition. In addition, the SF-AAT have systematically lower Pb contents than the MN-AAT, and generally show isotopically heavier Pb isotopic ratios. This is theoretically consistent with a preferential volatilization of lighter Pb isotopes during evaporation and considerably larger Pb loss from SF-AAT when compared to MN-AAT. Nevertheless, further experimental work would be necessary to unambiguously distinguish kinetic fractionation from source mixing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Large Ensemble Diagnostic Evaluation of Hydrologic Parameter Uncertainty in the Community Land Model Version 5 (CLM5)

Abstract Land surface models such as the Community Land Model version 5 (CLM5) seek to enhance understanding of terrestrial hydrology and aid in the evaluation of anthropogenic and climate change impacts. However, the effects of parametric uncertainty on CLM5 hydrologic predictions across regions, timescales, and flow regimes have yet to be explored in detail. The common use of the default hydrologic model parameters in CLM5 risks generating streamflow predictions that may lead to incorrect inferences for important dynamics and/or extremes. In this study, we benchmark CLM5 streamflow predictions relative to the commonly employed default hydrologic parameters for 464 headwater basins over the conterminous United States (CONUS). We evaluate baseline CLM5 default parameter performance relative to a large (1,307) Latin Hypercube Sampling‐based diagnostic comparison of streamflow prediction skill using over 20 error measures. We provide a global sensitivity analysis that clarifies the significant spatial variations in parametric controls for CLM5 streamflow predictions across regions, temporal scales, and error metrics of interest. The baseline CLM5 shows relatively moderate to poor streamflow prediction skill in several CONUS regions, especially the arid Southwest and Central U.S. Hydrologic parameter uncertainty strongly affects CLM5 streamflow predictions, but its impacts vary in complex ways across U.S. regions, timescales, and flow regimes. Overall, CLM5's surface runoff and soil water parameters have the largest effects on simulated high flows, while canopy water and evaporation parameters have the most significant effects on the water balance.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2013

RETENTION OF STELLAR-MASS BLACK HOLES IN GLOBULAR CLUSTERS

Globular clusters should be born with significant numbers of stellar-mass black holes (BHs). It has been thought for two decades that very few of these BHs could be retained through the cluster lifetime. With masses {approx}10 M{sub Sun }, BHs are {approx}20 times more massive than an average cluster star. They segregate into the cluster core, where they may eventually decouple from the remainder of the cluster. The small-N core then evaporates on a short timescale. This is the so-called Spitzer instability. Here we present the results of a full dynamical simulation of a globular cluster containing many stellar-mass BHs with a realistic mass spectrum. Our Monte Carlo simulation code includes detailed treatments of all relevant stellar evolution and dynamical processes. Our main finding is that old globular clusters could still contain many BHs at present. In our simulation, we find no evidence for the Spitzer instability. Instead, most of the BHs remain well mixed with the rest of the cluster, with only the innermost few tens of BHs segregating significantly. Over the 12 Gyr evolution, fewer than half of the BHs are dynamically ejected through strong binary interactions in the cluster core. The presence of BHs leads to long-term heating of the cluster, ultimately producing a core radius on the high end of the distribution for Milky Way globular clusters (and those of other galaxies). A crude extrapolation from our model suggests that the BH-BH merger rate from globular clusters could be comparable to the rate in the field.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2013

Preparation and Testing of Corrosion-and Spallation-Resistant Coatings

This Energy & Environmental Research Center (EERC) project is designed to determine if plating APMT®, a specific highly oxidation-resistant oxide dispersion-strengthened FeCrAl alloy made by Kanthal, onto nickel-based superalloy turbine parts is a viable method for substantially improving the lifetimes and maximum use temperatures of the parts. The method for joining the APMT plate to the superalloys is called evaporative metal bonding and involves placing a thin foil of zinc (Zn) between the plate and the superalloy, clamping them together, and heating in an atmosphere-controlled furnace. Upon heating, the Zn melts and dissolves the oxide skins of the alloys at the bond line, allowing the two alloys to diffuse into each other. The Zn then diffuses through the alloys and evaporates from their surfaces. Laboratory testing to determine the diffusion rate of Zn through the alloys has been completed. We have found that we were not able to create joints when temperatures much lower than the original temperature of 1214°C are used. Therefore, we limited our diffusion rate measurements to the two hold temperatures used in the procedure: 700° and 1214°C. The diffusivity of zinc in both APMT and CM247LC is quite similar at 700°C. Diffusivity in the APMT appears to be slightly higher, but the midline composition after 30 minutes at this temperature is quite similar. At 1214°C, the situation is very different. The calculated diffusivity of zinc in APMT is approximately 15 times higher than in CM247LC or Rene® 80 (~120 vs. ~8 μm²/min) at that temperature. In addition to the diffusion work, the coefficients of thermal expansions were determined for each of the alloys as a function of temperature. This information has been entered into a finite element model using ANSYS so that appropriate force-applying structures can be designed for use in joining structures composed of APMT and the nickel alloys. Gasifier sampling activities continue to determine what types of trace contaminants may occur in cleaned syngas that could lead to corrosion or deposition in turbines firing coal syngas. The EERC has several pilot-scale gasifiers that are continually used in a variety of test configurations as determined by the needs of the projects that are funding the tests. We are sampling both noncombusted and combusted syngas produced during some of the pilot-scale gasifier tests. After modifying our sampling procedures to minimize contamination from the oxidizer, we obtained very good filter samples from both syngas and from the combustion products of the syngas blended with natural gas. Scanning electron microscopy analyses showed that the particles captured on the filter from the syngas were typically 0.2 to 0.5 μm in diameter, whereas those captured from the combusted syngas were slightly larger and more spherical. However, the particles were so small that we could not obtain good spectra from them either at the EERC or JEOL America, the maker of the EERC electron microscope systems. Therefore, the EERC applied for and received time on electron microscopes using different signal analyzers at the Oak Ridge National Laboratory (ORNL) ShaRE User Facility, which is sponsored by the U.S. Department of Energy Scientific User Facilities Division of the Office of Basic Energy Sciences. At ORNL, both x-ray photoelectron spectroscopy (XPS) and Auger electron spectroscopy were performed on the samples because these are surface analyses that analyze electrons emitted from within a few nanometers of the surfaces of the particles and filters. The XPS data show that the particles do not contain any metals and, in fact, have an atomic composition almost identical to that of the polycarbonate filter. We currently believe that this indicates that the particles are primarily soot-based and not formed from volatilization of metals in the fluid-bed gasifier. The data indicate that the soot-based particles are not well burned in the thermal oxidizer, although they are significantly oxidized, nitrided, and sulfidized in the combustor. Ion etching to remove the surfaces of the particles indicates that the oxidation, nitridation, and sulfidation of the particles are primarily surface phenomena.

Electric↗