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All sources NASA NTRS DOE OSTI

DOE OSTI2020

Longitudinal, Lateral, Vertical, and Temporal Thermal Heterogeneity in a Large Impounded River: Implications for Cold-Water Refuges

Dam operations can affect mixing of the water column, thereby influencing thermal heterogeneity spatially and temporally. This occurs by restricting or eliminating connectivity in longitudinal, lateral, vertical, and temporal dimensions. We examined thermal heterogeneity across space and time and identified potential cold-water refuges for salmonids in a large impounded river in inland northwestern USA. To describe these patterns, we used thermal infrared (TIR) imagery, in situ thermographs, and high-resolution, 3-D hydraulic mapping. We explained the median water temperature and probability of occurrence of cool-water areas using generalized additive models (GAMs) at reach and subcatchment scales, and we evaluated potential cold-water refuge occurrence in relation to these patterns. We demonstrated that (1) lateral contributions from tributaries dominated thermal heterogeneity, (2) thermal variability at confluences was approximately an order of magnitude greater than of the main stem, (3) potential cold-water refuges were mostly found at confluences, and (4) the probability of occurrence of cool areas and median water temperature were associated with channel geomorphology and distance from dam. These findings highlight the importance of using multiple approaches to describe thermal heterogeneity in large, impounded rivers and the need to incorporate these types of rivers in the understanding of thermal riverscapes because of their limited representation in the literature.

Mejia, Francine H.↗

DOE OSTI2021

Impact of solar geoengineering on temperatures over the Indonesian Maritime Continent

Climate change has been projected to increase the intensity and magnitude of extreme temperature in Indonesia. Solar radiation management (SRM) has been proposed as a strategy to temporarily combat global warming, buying time for negative emissions. Though the global impacts of SRM have been extensively studied in recent years, regional impacts, especially in the tropics, have received much less attention. This paper investigates the potential stratospheric sulfate aerosol geoengineering to modify mean and extreme temperature, as well as the relative humidity and wet bulb temperature (WBT) change over Indonesian Maritime Continent (IMC) based on simulations from three different earth system models. We applied statistical downscaling and corrected the bias of model output to reproduce historical temperatures and relative humidity over IMC. We compared SRM as specified by the Geoengineering Model Intercomparison Project (GeoMIP) G4 experiment – 5 Tg of SO 2 into the lower stratosphere between 2020 and 2069 – concurrent with the RCP4.5 emissions scenario. SRM is able to significantly reduce the temperature means and extremes, and although differences in magnitude of response and spatial pattern occur, there is a generally consistent response. Additionally, the spatial response of changes forced by RCP4.5 scenario and SRM impact is notably heterogeneous in the archipelago, highlighting uncertainties that would be critical in assessing socio-economic consequences of both doing, and not doing SRM. In general, SRM has bigger impacts in reducing temperatures over land than oceans, and the southern monsoon region shows more variability. SRM is also effective at reducing the likelihood of WBT > 27OC events compared to RCP4.5 after some years of SRM deployment as well as during the post-termination period of SRM. Regional downscaling may be an effective tool in obtaining policy-relevant information about local effects of different future scenarios involving SRM.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Sub-1K Cold-Electron Quantum Well Switching at Room Temperature

Quantum states can provide means to systematically manipulate the transport of electrons. Here, in this study, we present electron transport across quasi-bound states of two heterogeneous quantum wells (QWs), where the transport of thermally excited electrons is blocked or enabled depending on the relative positions of the two quasi-bound states, with an abrupt current onset occurring when the two QW states align. The QW switch comprises a source (Cr), QW1 (Cr 2 O 3 ), QW2 (SnO x , x < 2), a tunneling barrier (SiO 2 ), and a drain (Si), where the effective electron mass of QW1 (m* QW1 ) is selected to be larger than QW2 (m* QW2 ). The current-voltage (I-V) measurements of the fabricated devices show abrupt current onsets, with the current transition occurring within 0.25 mV, corresponding to an effective electron temperature of 0.8 K at room temperature. Since transistor power consumption is fundamentally tied to effective electron temperature, this sub-1K cold-electron QW switching holds promise for highly energy-efficient computing.

Fermi−Dirac thermal smearing↗

NASA NTRS2003

Influence of Idealized Heterogeneity on Wet and Dry Planetary Boundary Layers Coupled to the Land Surface

We examine the influence of surface heterogeneity on boundary layers using a large-eddy simulation coupled to a land-surface model. Heterogeneity, imposed in strips varying from 2-30 km (1 less than lambda/z(sub i) less than 18), is found to dramatically alter the structure of the free convective boundary layer by inducing significant organized circulations. A conditional sampling technique, based on the scale of the surface heterogeneity (phase averaging), is used to identify and quantify the organized surface fluxes and motions in the atmospheric boundary layer. The impact of the organized motions on turbulent transport depends critically on the scale of the heterogeneity lambda, the boundary layer height zi and the initial moisture state of the boundary layer. Dynamical and scalar fields respond differently as the scale of the heterogeneity varies. Surface heterogeneity of scale 4 less than lamba/z(sub i) less than 9 induces the strongest organized flow fields (up, wp) while heterogeneity with smaller or larger lambda/z(sub i) induces little organized motion. However, the organized components of the scalar fields (virtual potential temperature and mixing ratio) grow continuously in magnitude and horizontal scale, as lambda/z(sub i) increases. For some cases, the organized motions can contribute nearly 100% of the total vertical moisture flux. Patch-induced fluxes are shown to dramatically impact point measurements that assume the time-average vertical velocity to be zero. The magnitude and sign of this impact depends on the location of the measurement within the region of heterogeneity.

Houser, Paul↗

DOE OSTI2024

Assessing the Atmospheric Response to Subgrid Surface Heterogeneity in the Single-Column Community Earth System Model, Version 2 (CESM2)

Land-atmosphere interactions are central to the evolution of the atmospheric boundary layer and the subsequent formation of clouds and precipitation. Existing global climate models represent these connections with bulk approximations on coarse spatial scales, but observations suggest that small-scale variations in surface characteristics and co-located turbulent and momentum fluxes can significantly impact the atmosphere. Recent model development efforts have attempted to capture this phenomenon by coupling existing representations of subgrid-scale (SGS) heterogeneity between land and atmosphere models. Such approaches are in their infancy and it is not yet clear if they can produce a realistic atmospheric response to surface heterogeneity. Here, we implement a parameterization to capture the effects of SGS heterogeneity in the Community Earth System Model (CESM2), and compare single-column simulations against high-resolution Weather Research and Forecasting (WRF) large-eddy simulations (LESs), which we use as a proxy for observations. The CESM2 experiments increase the temperature and humidity variances in the lowest atmospheric levels, but the response is weaker than in WRF-LES. In part, this is attributed to an underestimate of surface heterogeneity in the land model due to a lack of SGS meteorology, a separation between deep and shallow convection schemes in the atmosphere, and a lack of explicitly represented mesoscale secondary circulations. These results highlight the complex processes involved in capturing the effects of SGS heterogeneity and suggest the need for parameterizations that communicate their influence not only at the surface but also vertically.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Chemical structure and complex growth modes of magnesium silicate hydrate: Nanoparticle orientation, aggregation, and fusion

The extent of utilization of magnesium silicate hydrate (MSH) in construction is limited partly because of insufficient data ascertaining the kinetics of its precipitation. In this report MSH grown homogeneously or heterogeneously in the range of magnesium to silicon solution molar concentration ratios, [Mg]/[Si] = 0.5-1.5, and temperature = 25-80 °C was analyzed for its chemical structure and morphology. Infrared spectroscopy and geochemical modeling show that increasing the [Mg]/[Si] ratio results in less silicate polymerization in MSH. Atomic force microscopy reveals the presence of nanoparticles that aggregate and fuse to form films. Oriented attachment of nanoparticles and features indicative of enhanced crystallinity were observed at higher temperatures and longer reaction times. These data provide direct evidence for the persistence of hierarchical structures (i.e., nanoparticles forming 3D microparticles and 2D film layers) at the nanoscale to mesoscale. These findings offer insights into the precise chemical synthesis of MSH and its widespread use as a binder for construction purposes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Reactive force fields for aqueous and interfacial magnesium carbonate formation

Here we develop Mg/C/O/H ReaxFF parameter sets for two environments: an aqueous force field for magnesium ions in solution and an interfacial force field for minerals and mineral–water interfaces. Since magnesium is highly ionic, we choose to fix the magnesium charge and model its interaction with C/O/H through Coulomb, Lennard-Jones, and Buckingham potentials. We parameterize the forcefields against several crystal structures, including brucite, magnesite, magnesia, magnesium hydride, and magnesium carbide, as well as Mg 2+ water binding energies for the aqueous forcefield. Then, we test the forcefield for other magnesium-containing crystals, solvent separated and contact ion-pairs and single-molecule/multilayer water adsorption energies on mineral surfaces. We also apply the forcefield to the forsterite–water and brucite–water interface that contains a bicarbonate ion. We observe that a long-range proton transfer mechanism deprotonates the bicarbonate ion to carbonate at the interface. Free energy calculations show that carbonate can attach to the magnesium surface with an energy barrier of about 0.22 eV, consistent with the free energy required for aqueous Mg–CO 3 ion pairing. Also, the diffusion constant of the hydroxide ions in the water layers formed on the forsterite surface are shown to be anisotropic and heterogeneous. These findings can help explain the experimentally observed fast nucleation and growth of magnesite at low temperature at the mineral–water–CO 2 interface in water-poor conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Zooming in: SCREAM at 100 m using regional refinement over the San Francisco Bay Area

Pushing global climate models to large-eddy simulation (LES) scales over complex terrain has remained a major challenge. This study presents the first known implementation of a global model – SCREAM (Simple Cloud-Resolving E3SM Atmosphere Model) – at 100 m horizontal resolution using a regionally refined mesh (RRM) over the San Francisco Bay Area. Two hindcast simulations were conducted to test performance under both strong synoptic forcing and weak, boundary-layer-driven conditions. We demonstrate that SCREAM can stably run at LES scales while realistically capturing topography, surface heterogeneity, and coastal processes. The 100 m SCREAM-RRM substantially improves near-surface wind speed, temperature, humidity, and pressure biases compared to the baseline 3.25 km simulation, and better reproduces fine-scale wind oscillations and boundary-layer structures. These advances leverage SCREAM's scale-aware SHOC turbulence parameterization, which transitions smoothly across scales without tuning. Performance tests show that while CPU-only simulations remain costly, GPU acceleration with SCREAMv1 on NERSC's Perlmutter system enables two-day hindcasts to complete in under two wall-clock days. Our results open the door to LES-scale studies of orographic flows, boundary-layer turbulence, and coastal clouds within a fully comprehensive global modeling framework.

Geosciences↗

NASA NTRS1986

Process-induced defects in solar cell silicon

The microstructure of as-grown and processed, edge-defined film-fed grown, silicon ribbons was studied in order to identify the basic mechanisms responsible for the change of the as-grown defect structure during processing at elevated temperatures. The short heat treatment required to diffuse the p-n junction was sufficient to cause heterogeneous precipitation of impurity atoms, particularly transition metals. In addition, an elastic recovery of the ribbon occurred by dislocation glide, resulting in the formation of a polygonizationlike structure of subboundaries in the base. Mechanisms are suggested by which twin boundaries, acting as dislocation obstacles, can concentrate the relatively low average dislocation densities typical of edge-defined film-fed grown ribbons (10 to the 4th to 10 to the 8th/sq cm) to values which are sufficient to induce the formation of subgrainlike boundary structures.

Gleichmann, R.↗

NASA NTRS1987

Elucidation of the organometallic vapor phase epitaxial growth mechanism for InP

A new technique for tracing the organometallic vapor epitaxial growth is reported. The pyrolysis of PH3, alone and in the presence of trimethylindium (TMIn), and of TMIn alone was studied by conducting the epitaxial growth of InP in D2 as the carrier gas, tracing growth reactions by mass spectrometric analysis of the product molecules. The TMIn alone pyrolyzes mostly homogeneously in the gas phase, while the PH3 pyrolysis is completely heterogeneous at the InP surface. Adding TMIn to PH3 results in a dramatic decrease in the pyrolysis temperature. PH3 molecules which interact with TMIn in the gas phase pyrolyze at temperatures as low as 250, and those decomposing without TMIn interaction pyrolyze at temperatures approximately 200 C higher. Similarly, the presence of PH3 lowers the TMIn pyrolysis temperature by at least 50 C. TMIn alone in D2 produces mainly CH3D molecules. For high PH3:TMIn ratios, CH4 is the only carbon-containing reaction product.

Buchan, N. I.↗

NASA NTRS1988

Antarctic ozone decrease: Possible impact on the seasonal and latitudinal distribution of total ozone as simulated by a 2-D model

Satellite borne instruments, the Total Ozone Mapping Spectrometer (TOMS) and the Solar Backscatter Ultraviolet spectrometer (SBUV), show that total column ozone has decreased by more than 5 percent in the neighborhood of 60 S at all seasons since 1979. This is considerably larger than the decrease calculated by 2-D models which take into account solar flux variation and increases of trace gas concentrations over the same period. The meteorological conditions (warmer temperature and the apparent lack of polar stratospheric clouds) at these latitudes do not seem to favor heterogeneous chemistry as the direct cause for the observed ozone reduction. A mechanism involving the seasonal transport of ozone-poor air mass from within the polar vortex to lower latitudes (the so-called dilution effect) is proposed as a possible explanation for the observed year-round ozone reduction in regions away from the vortex.

Ko, Malcolm K. W.↗

NASA NTRS2002

Changes in the Molar Ellipticities of HEWL Observed by Circular Dichroism and Quantitated by Time Resolved Fluorescence Anisotropy Under Crystallizing Conditions

Fluid models for simple colloids predict that as the protein concentration is increased, crystallization should occur at some sufficiently high concentration regardless of the strength of attraction. However, empirical measurements do not fully support this assertion. Measurements of the second virial coefficient (B22) indicate that protein crystallization occurs only over a discrete range of solution parameters. Furthermore, observations of a strong correlation between protein solubility and B22, has led to an ongoing debate regarding the relationship between the two. Experimental work in our lab, using Hen Egg White Lysozyme (HEWL), previously revealed that the rotational anisotropy of the protein under crystallizing conditions changes systematically with pH, ionic strength and temperature. These observations are now supported by recent work revealing that small changes in the molar ellipticity also occur systematically with changes in ionic strength and temperature. This work demonstrates that under crystallization conditions, the protein native state is characterized by a conformational heterogeneity that may prove fundamental to the relationship between protein crystallization and protein solubility.

Sumida, John↗

DOE OSTI2024

Data Acquisition System Selection and Calibration of Resistive Moisture Content Measurements for Large-Scale Field Studies in Cold Climate Residential Building Envelope Performance

The residential building stock built before the energy codes were enforced has several significant inefficiency problems in terms of insulation and air leakage. To decrease these inefficiencies, building retrofits are necessary. However, if the envelope is not appropriately designed, excessive accumulation of moisture content and thus mold formation and decay inside the envelope layers can be a vital problem. This risk becomes higher, especially in extreme climate conditions such as cold winters and hot and humid summers as in some northern regions of the U.S. Field studies are essential to test the long-term hygrothermal performance of building envelopes. Although in-situ temperature, RH, and heat flux measurements are straightforward, moisture content measurements are cumbersome. Mainly, because of the heterogeneous nature of the wood materials, deviations and nonuniformities within the materials are unavoidable. Resistance measurements are one of the oldest methods used to measure the moisture content of wood and other building materials. In large-scale studies, it is commonly preferred to use multi-purpose data acquisition systems (DAQ) and custom-made or prefabricated moisture pins to measure the electrical resistance (and thus moisture content) of critical building materials. These multi-purpose DAQ systems generally provide lower costs and offer more flexibility. However, these systems require calibration and fine-tuning to achieve accurate moisture content measurements. A large-scale, two-year-long field study was conducted in northern Minnesota to monitor the hygrothermal performance of residential retrofit wall systems in cold climates. Two base case walls and sixteen different wall treatments were tested. Moisture contents were measured at various layers in each wall treatment using 85 sets of moisture pins. This paper focuses on the overall approach, fabrication, and calibration methodology for the combination of custom-made moisture pins and a multi-purpose DAQ. The aim is to directly use the low-excitation multi-purpose DAQ without any extra voltage regulator. A half-bridge circuit is used to measure wood resistance with 4V excitation voltage and 100 kΩ and 500 kΩ reference resistors. The system is calibrated for four different materials: Douglas fir, lodgepole pine, western red cedar, and oriented strand board (OSB). Calibration experiments were done under controlled conditions in 50% and 65% RH test chambers. Resistance-based moisture content calibration curves are obtained for each species. Results show that higher reference resistors provided better calibration curves for lower excitation voltages.

Desjarlais, Andre Omer↗

NASA NTRS1997

Internal and Surface Phenomena in Heterogenous Metal Combustion

The phenomenon of gas dissolution in burning metals was observed in recent metal combustion studies, but it could not be adequately explained by the traditional metal combustion models. The research reported here addresses heterogeneous metal combustion with emphasis on the processes of oxygen penetration inside burning metal and its influence on the metal combustion rate, temperature history, and disruptive burning. The unique feature of this work is the combination of the microgravity environment with a novel micro-arc generator of monodispersed metal droplets, ensuring repeatable formation and ignition of uniform metal droplets with a controllable initial temperature and velocity. Burning droplet temperature is measured in real time with a three wavelength pyrometer. In addition, particles are rapidly quenched at different combustion times, cross-sectioned, and examined using SEM-based techniques to retrieve the internal composition history of burning metal particles. When the initial velocity of a spherical particle is nearly zero, the microgravity environment makes it possible to study the flame structure, the development of flame nonsymmetry, and correlation of the flame shape with the heterogeneous combustion processes.

Dreizin, Edward L.↗

DOE OSTI2023

Effect of Surface Temperature on the Distribution and Reactivity of Rh Active Sites for CO Oxidation

Single–atom catalysts are a fast–emerging area in which late–transition metal atoms are supported on oxides, metals, and carbonaceous supports. They show great promise for selective chemical reactions due to their well–defined active sites, and significantly reduce precious metal loading. However, oxide–supported single–atom catalysts have drawbacks such as deactivation due to sintering, and there are on–going debates about the exact nature of the active sites. Herein we report a model system where the surface temperature during Rh deposition on a copper oxide support dictates the Rh size distribution. Here our temperature–programmed desorption experiments reveal that Rh clusters perform CO oxidation at lower temperature than single atoms, and isotopic labelling demonstrates differences in the mechanism in that the C–O bond is broken and reformed on clusters, as opposed to a pure Mars van Krevelen mechanism for CO oxidation at the single–atom Rh sites. We further examine the cluster size distributions with scanning tunneling microscopy and X–ray photoelectron spectroscopy which confirm the presence of both clusters and single atoms for the lower temperature deposition and only single atoms for the higher temperature deposition. Together, these results provide a fundamental understanding of the differences in the CO oxidation mechanism on Rh atoms and clusters.

36 MATERIALS SCIENCE↗

NASA NTRS2004

Comparison of Local Scale Measured and Modeled Brightness Temperatures and Snow Parameters from the CLPX 2003 by Means of a Dense Medium Radiative Transfer Theory Model

Microwave remote sensing offers distinct advantages for observing the cryosphere. Solar illumination is not required, and spatial and temporal coverage are excellent from polar-orbiting satellites. Passive microwave measurements are sensitive to the two most useful physical quantities for many hydrological applications: physical temperature and water content/state. Sensitivity to the latter is a direct result of the microwave sensitivity to the dielectric properties of natural media, including snow, ice, soil (frozen or thawed), and vegetation. These considerations are factors motivating the development of future cryospheric satellite remote sensing missions, continuing and improving on a 26-year microwave measurement legacy. Perhaps the biggest issues regarding the use of such satellite measurements involve how to relate parameter values at spatial scales as small as a hectare to observations with sensor footprints that may be up to 25 x 25 km. The NASA Cold-land Processes Field Experiment (CLPX) generated a dataset designed to enhance understanding of such scaling issues. CLPX observations were made in February (dry snow) and March (wet snow), 2003 in Colorado, USA, at scales ranging from plot scale to 25 x 25 km satellite footprints. Of interest here are passive microwave observations from ground-based, airborne, and satellite sensors, as well as meteorological and snowpack measurements that will enable studies of the effects of spatial heterogeneity of surface conditions on the observations. Prior to performing such scaling studies, an evaluation of snowpack forward modelling at the plot scale (least heterogeneous scale) is in order. This is the focus of this paper. Many forward models of snow signatures (brightness temperatures) have been developed over the years. It is now recognized that a dense medium radiative transfer (DMRT) treatment represents a high degree of physical fidelity for snow modeling, yet dense medium models are particularly sensitive to snowpack structural parameters such as grain size, density, and depth---parameters that may vary substantially within a snowpack. Microwave radiometric data and snow pit measurements collected at the Local-Scale Observation Site (LSOS) during the third Intensive Observation Period (IOP3) of the CLPX have been used to test the capabilities of a DMRT model using the Quasi Crystalline Approximation with Coherent Potential (QCA-CP). The radiometric measurements were made by the University of Tokyo s Ground Based Microwave Radiometer-7 (GBMR-7) system. We evaluate the degree to which a DMRT-based model can accurately reproduce the GBMR-7 brightness temperatures at different frequencies and incidence angles.

Tedescol, Marco↗

DOE OSTI2024

Mechanochemical in Situ Encapsulation of Palladium in Covalent Organic Frameworks

Palladium-encapsulated covalent organic frameworks (Pd/COFs) have garnered enormous attention in heterogeneous catalysis. However, the dominant ex situ encapsulation synthesis is tedious (multistep), time-consuming (typically 4 days or more), and involves the use of noxious solvents. Here we develop a mechanochemical in situ encapsulation strategy that enables the one-step, time-efficient, and environmentally benign synthesis of Pd/COFs. By ball milling COF precursors along with palladium acetate (Pd(OAc) 2 ) in one pot under air at room temperature, Pd/COF hybrids were readily synthesized within an hour, exhibiting high crystallinity, uniform Pd dispersion, and superb scalability up to gram scale. Moreover, this versatile strategy can be extended to the synthesis of three Pd/COFs. Remarkably, the resulting Pd/DMTP-TPB showcases extraordinary activity (96-99% yield in 1 h at room temperature) and broad substrate scope (>10 functionalized biaryls) for the Suzuki-Miyaura coupling reaction of aryl bromides and arylboronic acids. Furthermore, the heterogeneity of Pd/DMTP-TPB is verified by recycling and leaching tests. Finally, the mechanochemical in situ encapsulation strategy disclosed herein paves a facile, rapid, scalable, and environmentally benign avenue to access metal/COF catalysts for efficient heterogeneous catalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Mechanically strengthened heterogeneous Sm-Co sintered magnets

Samarium-cobalt sintered magnets offer excellent magnetic properties, thermal stability, and corrosion resistance. They are used in a variety of defense and civilian applications, especially when elevated operation temperatures (e.g., 200 ºC to 550 ºC) are required. However, the utilization of these materials is restricted by their brittleness. Improving their mechanical resilience would make them more cost-effective, efficient, and robust in decarbonization and other function-related applications while reducing the pressure on critical material supply chains. In this paper, we engineer a series of novel heterogeneous microstructures, such as laminated coarse grain (CG)/fine grain (FG) and core/shell CG/FG microstructures, to produce unprecedented combinations of superior mechanical and magnetic properties without altering the chemical compositions of the magnets or common heat treatment procedures. Further, a 60% flexural strength enhancement is obtained using heterogeneous Sm 2 (CoFeCuZr) 17 sintered magnets with little impact on their magnetic properties. The mechanically robust heterogeneous Sm-Co sintered magnets have a minor (e.g., less than 4.6%) reduction in the energy product (BH) max due to a slightly reduced squareness of the demagnetization curve, with no decrease in either the remanence (B r ) or the intrinsic coercivity (H ci ). The flexural strengths of these heterogeneous Sm-Co magnets depend on the volume ratios and mean grain sizes of the FG/CG regions, as well as their microstructural architectures. The fine-grained regions act as mechanical strengthening sites, which can be strategically used when designing the magnet for different applications. This technology is highly compatible with existing magnet manufacturing processes and thus can be adopted readily by the magnet industry.

36 MATERIALS SCIENCE↗