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At least 919 records · Page 51

Regional Impacts of Ice Sheet Surface Representation Improvements in an Earth System Model

Ice sheet surface conditions and their subsequent impact on surface mass balance play an important role in ice sheet dynamics and ice sheet interaction with the overlying atmosphere and surrounding ocean. The NASA Global Modeling and Assimilation Office’s (GMAO) Goddard Earth Observing System (GEOS) ecosystem of models and reanalyses model ice sheet and glacier surface mass balance with a moderately complex snow and ice module, including prognostic surface albedo evolution, fractional snow cover, and snowpack hydrology and meltwater retention. With this configuration, Greenland near surface air temperatures and ice sheet melt are well represented in MERRA-2, GMAO’s current atmospheric reanalysis; however, the similarity to observations in some regions is due, in part, to compensating biases in surface energy budget. Recent improvements to GEOS’ cloud microphysics and longwave radiation parameterizations reduced biases in surface net longwave radiation and exacerbated surface net shortwave radiation biases, effectively increasing near surface temperatures and melting, particularly during the summer months. Here, we demonstrate the Earth system response to an improved representation of the ice sheet surface focused on minimizing the surface energy biases and increasing spatial and temporal representativeness. New changes to the surface albedo parameterization, including the introduction of a prognostic aerosol darkening scheme, help mitigate shortwave biases, while modifications to surface roughness characteristics improve near surface sensible heat fluxes. Focusing on the Arctic and Greenland, we examine the combined impact on these changes on regional weather conditions and ice sheet surface mass balance using a high resolution atmospheric only experiment, and we use a coupled model configuration to assess the impact on oceanic conditions and subseasonal-to-seasonal prediction. Overall, these improvements increase modeled ice sheet surface realism and provide a strong basis for more accurate ice sheet mass balance in GMAO’s future reanalyses and forecasting systems.

Lauren C Andrews↗

Regional Impacts of Ice Sheet Surface Representation Improvements in an Earth System Model

Ice sheet surface conditions and their subsequent impact on surface mass balance play an important role in ice sheet dynamics and ice sheet interaction with the overlying atmosphere and surrounding ocean. The NASA Global Modeling and Assimilation Office’s (GMAO) Goddard Earth Observing System (GEOS) ecosystem of models and reanalyses model ice sheet and glacier surface mass balance with a moderately complex snow and ice module, including prognostic surface albedo evolution, fractional snow cover, and snowpack hydrology and meltwater retention. With this configuration, Greenland near surface air temperatures and ice sheet melt are well represented in MERRA-2, GMAO’s current atmospheric reanalysis; however, the similarity to observations in some regions is due, in part, to compensating biases in surface energy budget. Recent improvements to GEOS’ cloud microphysics and longwave radiation parameterizations reduced biases in surface net longwave radiation and exacerbated surface net shortwave radiation biases, effectively increasing near surface temperatures and melting, particularly during the summer months. Here, we demonstrate the Earth system response to an improved representation of the ice sheet surface focused on minimizing the surface energy biases and increasing spatial and temporal representativeness. New changes to the surface albedo parameterization, including the introduction of a prognostic aerosol darkening scheme, help mitigate shortwave biases, while modifications to surface roughness characteristics improve near surface sensible heat fluxes. Focusing on the Arctic and Greenland, we examine the combined impact on these changes on regional weather conditions and ice sheet surface mass balance using a high resolution atmospheric only experiment, and we use a coupled model configuration to assess the impact on oceanic conditions and subseasonal-to-seasonal prediction. Overall, these improvements increase modeled ice sheet surface realism and provide a strong basis for more accurate ice sheet mass balance in GMAO’s future reanalyses and forecasting systems.

Lauren C. Andrews↗

Dielectric Permittivity Measurements of Geologic Samples at Venus Surface Temperatures

Synthetic-aperture radar (SAR) and radar sounding are two powerful remote sensing techniques used to examine the surface and subsurface of planets. Their value is critical in the case of Venus due to this planet’s global and visually opaque cloud layer. The recently selected VERITAS and EnVision orbital missions, slated to study the planet in the early 2030’s, employ radar instruments to image the surface (VERITAS and EnVision) and probe the subsurface (EnVision). For both techniques, the complex dielectric permittivity of the surface and subsurface materials control radar backscatter intensity and penetration depth. Since the 1970’s, many studies have characterized the dielectric permittivity of geologic materials collected both on Earth and on the Moon to constrain the radar reflectivity and transparency at a variety of radar frequencies [e.g., 1]. Two consistent findings from those studies are that complex permittivity depends on both the density (or porosity) and the composition of the material. Denser materials and more metal-rich compositions tend to have higher permittivity values and to incur greater propagation path loss. Water content also elevates permittivity of otherwise dry rocks/soils/regolith [e.g., 2]. However, permittivity is independent of frequency for the 0.5-18 GHz range, within which SAR imaging commonly lies. The one aspect poorly explored thus far is the effect of elevated temperatures on dielectric permittivity. Previous work suggests that increased lattice vibrations and flow of free electrons associated with an increase in temperature elevate both the real (reflectivity) and imaginary (path loss) parts of the complex permittivity. We are currently conducting a 3-year campaign to measure the complex dielectric permittivity of Venusrelevant geologic materials at Venus surface temperatures (380°C - 460°C) and with frequencies relevant to VERITAS, EnVision, and Magellan imaging synthetic aperture radars.

M Barmatz↗

High‐Pressure‐Induced Pseudo‐oxidation of Copper Surfaces by Carbon Monoxide

Abstract Instantaneous electronic and structural modifications of Cu surfaces by high‐pressure CO were explored. At pressures over a millibar range the coverage of CO on the Cu(1 1 1) surface reached approximately one monolayer, and we observed several shake‐up peaks in the Cu 2p photoemission spectra for the first time by using ambient pressure X‐ray photoelectron spectroscopy. These shake‐up peaks resembled those obtained for oxidized surface Cu atoms. We propose that these changes are related to the generation of a copper–carbonyl complex and subsequent Cu surface restructuring owing to lateral CO–CO repulsions. The generality of this finding was investigated in two model reactions, the water‐gas shift and CO oxidation, on a Cu(1 1 1) surface, and we clearly identified the pseudo‐oxidation of Cu. These reversible changes were found to be independent of the orientation of the Cu surface and are of general importance for Cu‐based heterogeneous catalysis.

Zhang, Xueqiang↗

Rare Earth Element-Induced Condensation of the Block V of the Repeats-in-Toxin Domain from CyaA from Bordetella pertussis for Separations

Rare earth elements (REEs) are critical for the development of a range of new technologies. However, the current industrial separation processes of these metals from natural sources, recycled materials, and industrial effluents involve the large consumption of organic solvents, resulting in a sizable environmental footprint. We aim to exploit the high affinity of the block V peptide of the repeats-in-toxin (RTX) domain of the adenylate cyclase protein from Bordetella pertussis for the separation of REEs. This peptide selectively binds with lanthanide (Ln) cations and can undergo Ln-induced phase separation, which can be used in bioseparation processes. Here, we evaluated the self-assembling structures of complexes of the RTX domain peptide folded in the presence of Ln 3+ cations. Size distribution and surface potential measurements of complexes were taken to understand the Ln-induced changes in the complexed peptide. Transmission electron microscopy imaging was used to explore the structures of complexes, while anomalous small-angle X-ray scattering measurements were used to determine the distribution of Ln 3+ ions within the protein-based macrostructures. In the presence of excess Ln 3+ , we observed the formation of coral-like cylindrical structures comprised of Ln 3+ -RTX complexes, with approximately eight trivalent metals per peptide within the nanosized assemblies. These findings provide new insights into the structural organization of assembled RTX domains and their ability to coordinate with REEs, forming nanosized, metal-rich structures that naturally condense, providing a proof-of-concept for protein-based separation processes of these critical materials.

chemical structure↗

Fourier-spectral element approximation of the ion–electron Braginskii system with application to tokamak edge plasma in divertor configuration

Due to the extreme conditions required to produce energy by nuclear fusion in tokamaks, simulating the plasma behavior is an important but challenging task. We focus on the edge part of the plasma, where fluid approaches are probably the best suited, and our approach relies on the Braginskii ion–electron model. Assuming that the electric field is electrostatic, this yields a set of 10 strongly coupled and non-linear conservation equations that exhibit multiscale and anisotropy features. The computational domain is a torus of complex geometrical section, that corresponds to the divertor configuration, i.e. with an “X-point” in the magnetic surfaces. To capture the complex physics that is involved, high order methods are used: The time-discretization is based on a Strang splitting, that combines implicit and explicit high order Runge–Kutta schemes, and the space discretization makes use of the spectral element method in the poloidal plane together with Fourier expansions in the toroidal direction. The paper thoroughly describes the algorithms that have been developed, provides some numerical validations of the key algorithms and exhibits the results of preliminary numerical experiments. In particular, we point out that the highest frequency of the system is intermediate between the ion and electron cyclotron frequencies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Benchmarking an Embedded Adaptive Sampling Configuration Interaction Method for Surface Reactions: H 2 Desorption from and CH 4 Dissociation on Cu(111)

Embedded (emb-) correlated wavefunction (CW) theory enables accurate assessments of both ground- and excited-state reaction mechanisms involved in heterogeneous catalysis. Embedded multireference second-order perturbation theory (emb-MRPT2) based on reference wavefunctions generated via embedded complete active space self-consistent field (emb-CASSCF) theory is currently state-of-the-art. However, the factorial scaling of CASSCF limits the size of active space and the complexity of systems that can be studied. In this work, we assess the efficacy of an alternative CW method, adaptive sampling configuration interaction (ASCI)–which enables large active spaces to be used–for studying surface reactions. We couple ASCI with density functional embedding theory (DFET) and benchmark its performance for two reactions: H 2 desorption from and CH 4 dissociation on the Cu(111) surface. Unlike embedded complete active space second-order perturbation theory (emb-CASPT2) that accurately reproduces a measured H 2 desorption barrier, embedded ASCI, using a very large active space (though one that still comprises a small portion of the full set of orbitals) fails to do so. Adding an extra correlation term from embedded Møller–Plesset second-order perturbation theory (emb-MP2) improves the desorption barrier and endothermicity predictions. Thus, the inaccuracy of embedded ASCI comes from the missing dynamic correlation from the many other electrons and orbitals not included in the active space. For CH 4 dissociation, again embedded ASCI overestimates the dissociation barrier compared to emb-CASPT2 predictions. Adding dynamic correlation from emb-MP2 helps correct the barrier. However, this composite approach suffers from double counting of correlation within embedded ASCI followed by emb-MP2 calculations. We therefore conclude that the state-of-the-art emb-MRPT2 based on reference wavefunctions generated via emb-CASSCF remains the method of choice for studying surface reactions. emb-ASCI is useful when large active spaces beyond the limit of emb-CASSCF are essential, such as to study complex surface reactions with significant multiconfigurational character (static correlation) but weak dynamic correlation.

08 HYDROGEN↗

Plutonium environmental chemistry: mechanisms for the surface-mediated reduction of Pu(v/vi)

In recent decades, interest in plutonium mobility has increased significantly due to the need of the United States, as well as other nations, to deal with commercial spent nuclear fuel, nuclear weapons disarmament, and the remediation of locations contaminated by nuclear weapons testing and production. Although there is a global consensus that geologic disposal is the safest existing approach to dealing with spent nuclear fuel and high-level nuclear waste, only a few nations are moving towards implementing a geologic repository due to technical and political barriers. Understanding the factors that affect the mobility of plutonium in the subsurface environment is critical to support the development of such repositories. The importance of redox chemistry in determining plutonium mobility cannot be understated. While Pu(IV) is generally assumed to be immobile in the subsurface environment due to sorption or precipitation, Pu(V) tends to be mobile due to its relatively low effective charge and weak complex formation. This review highlights one particularly important aspect of plutonium behaviour at the mineral–water interface—the concept of surface-mediated reduction, which describes the reduction of plutonium on a mineral surface. It provides a conceptual model for and evidence supporting or refuting each proposed mechanism for surface-mediated reduction including (i) radiolysis at the mineral surface, (ii) electron transfer via ferrous iron or manganese in the mineral structure, (iii) electron shuttling due to the semiconducting properties of the mineral, (iv) disproportionation of Pu(V), (v) facilitation by proton exchange sites, (vi) stabilisation of Pu(IV) due to the increased concentration gradient within the electrical double layer, and (vii) a Nernstian favourability of Pu(IV) surface complexes and colloids. It also provides new perspectives on future research directions.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Effect of Space Radiation Processing on Lunar Soil Surface Chemistry: X-Ray Photoelectron Spectroscopy Studies

Current understanding of the chemistry and microstructure of the surfaces of lunar soil grains is dominated by a reference frame derived mainly from electron microscopy observations [e.g. 1,2]. These studies have shown that the outermost 10-100 nm of grain surfaces in mature lunar soil finest fractions have been modified by the combined effects of solar wind exposure, surface deposition of vapors and accretion of impact melt products [1,2]. These processes produce surface-correlated nanophase Feo, host grain amorphization, formation of surface patinas and other complex changes [1,2]. What is less well understood is how these changes are reflected directly at the surface, defined as the outermost 1-5 atomic monolayers, a region not easily chemically characterized by TEM. We are currently employing X-ray Photoelectron Spectroscopy (XPS) to study the surface chemistry of lunar soil samples that have been previously studied by TEM. This work includes modification of the grain surfaces by in situ irradiation with ions at solar wind energies to better understand how irradiated surfaces in lunar grains change their chemistry once exposed to ambient conditions on earth.

Dukes, C.↗

Three-Dimensional Surface Downwelling Longwave Radiation Clear-Sky Effects in the Upper Colorado River Basin

In complex terrain, non-parallel surfaces receive emitted radiation from adjacent surfaces. Qualitatively, where surface skin temperatures and lower tropospheric temperature and humidity are not uniform, the downwelling longwave radiation (DLR) will be determined not just by radiation from the atmosphere above a given location, but also by adjacent surface temperatures. We quantify this three-dimensional longwave radiative effect over the Upper Colorado River Basin in clear-sky conditions by calculating surface DLR with observed land-surface temperatures from ECOSTRESS. We find that this effect is due to terrain-subtended sky-view and represents ~22% of the surface longwave flux, rising to ~28% and ~24% in the East and Southeast of the Basin, respectively, and can be >50% in extreme cases. The common omission of this effect in atmospheric radiation models leads to an underestimation of DLR in complex terrain, especially at higher elevations, which has significant implications for mountainous ecohydrology simulations.

3-dimensional effects↗

Direct Numerical Simulation of Transitional and Turbulent Flows Over Multi-Scale Surface Roughness—Part I: Methodology and Challenges

Abstract High-fidelity simulation of transitional and turbulent flows over multi-scale surface roughness presents several challenges. For instance, the complex and irregular geometrical nature of surface roughness makes it impractical to employ conforming structured grids, commonly adopted in large-scale numerical simulations due to their high computational efficiency. One possible solution to overcome this problem is offered by immersed boundary methods, which allow wall boundary conditions to be enforced on grids that do not conform to the geometry of the solid boundary. To this end, a three-dimensional, second-order accurate boundary data immersion method (BDIM) is adopted. A novel mapping algorithm that can be applied to general three-dimensional surfaces is presented, together with a newly developed data-capturing methodology to extract and analyze on-surface flow quantities of interest. A rigorous procedure to compute gradient quantities such as the wall shear stress and the heat flux on complex non-conforming geometries is also introduced. The new framework is validated by performing a direct numerical simulation (DNS) of fully developed turbulent channel flow over sinusoidal egg-carton roughness in a minimal-span domain. For this canonical case, the averaged streamwise velocity profiles are compared against results from the literature obtained with a body-fitted grid. General guidelines on the BDIM resolution requirements for multi-scale roughness simulation are given. Momentum and energy balance methods are used to validate the calculation of the overall skin friction and heat transfer at the wall. The BDIM is then employed to investigate the effect of irregular homogeneous surface roughness on the performance of an LS-89 high-pressure turbine blade at engine-relevant conditions using DNS. This is the first application of the BDIM to realize multi-scale roughness for transitional flow in transonic conditions in the context of high-pressure turbines. The methodology adopted to generate the desired roughness distribution and to apply it to the reference blade geometry is introduced. The results are compared to the case of an equivalent smooth blade.

Engineering↗

Intermittent Criticality Multi‐Scale Processes Leading to Large Slip Events on Rough Laboratory Faults

Abstract We discuss data of three laboratory stick‐slip experiments on Westerly Granite samples performed at elevated confining pressure and constant displacement rate on rough fracture surfaces. The experiments produced complex slip patterns including fast and slow ruptures with large and small fault slips, as well as failure events on the fault surface producing acoustic emission bursts without externally‐detectable stress drop. Preparatory processes leading to large slips were tracked with an ensemble of ten seismo‐mechanical and statistical parameters characterizing local and global damage and stress evolution, localization and clustering processes, as well as event interactions. We decompose complex spatio‐temporal trends in the lab‐quake characteristics and identify persistent effects of evolving fault roughness and damage at different length scales, and local stress evolution approaching large events. The observed trends highlight labquake localization processes on different spatial and temporal scales. The preparatory process of large slip events includes smaller events marked by confined bursts of acoustic emission activity that collectively prepare the fault surface for a system‐wide failure by conditioning the large‐scale stress field. Our results are consistent overall with an evolving process of intermittent criticality leading to large failure events, and may contribute to improved forecasting of large natural earthquakes.

Geochemistry & Geophysics↗

On the molecular complexity of the hot cores in Orion A - Grain surface chemistry as 'The last refuge of the scoundrel'

We have modeled the gas phase chemistry of warm molecular material around protostars that is seeded with evaporating grain mantles. We show that the release of simple molecules into the gas drives ion-molecule and neutral chemistries which can account for many of the complex O-bearing and N-bearing molecules observed in hot cores. Initial grain mantle components and secondary product molecules are identified, and the observational consequences are discussed.

Charnley, S. B.↗

Catalytic Oxidation of CO on a Curved Pt(111) Surface: Simultaneous Ignition at All Facets through a Transient CO-O Complex

The light-off of the CO oxidation is simultaneous on all Pt crystal surfaces vicinal to the (111) plane, regardless of the reaction conditions, and in contrast with the structural dependence of Pd. In this work, using ambient-pressure XPS we find that, immediately prior to ignition, atomic oxygen incorporates to the subsurface plane, leading to buckling of the topmost CO-Pt layer, and effectively equaling the CO desorption temperature at terraces and steps.

36 MATERIALS SCIENCE↗

A nanobody suite for yeast scaffold nucleoporins provides details of the nuclear pore complex structure

Nuclear pore complexes (NPCs) are the main conduits for molecular exchange across the nuclear envelope. The NPC is a modular assembly of ~500 individual proteins, called nucleoporins or nups. Most scaffolding nups are organized in two multimeric subcomplexes, the Nup84 or Y complex and the Nic96 or inner ring complex. Working in S. cerevisiae, and to study the assembly of these two essential subcomplexes, we here develop a set of twelve nanobodies that recognize seven constituent nucleoporins of the Y and Nic96 complexes. These nanobodies all bind specifically and with high affinity. We present structures of several nup-nanobody complexes, revealing their binding sites. Additionally, constitutive expression of the nanobody suite in S. cerevisiae detect accessible and obstructed surfaces of the Y complex and Nic96 within the NPC. Overall, this suite of nanobodies provides a unique and versatile toolkit for the study of the NPC.

59 BASIC BIOLOGICAL SCIENCES↗

Hyperspectral Radiative Transfer Modeling to Explore the Combined Retrieval of Biophysical Parameters and Canopy Fluorescence from FLEX - Sentinel-3 Tandem Mission Multi-Sensor Data

The FLuorescence EXplorer (FLEX) satellite mission, selected as ESA's 8th Earth Explorer, has been designed forthe measurement of sun-induced fluorescence (F) spectra emitted by plants. This will be accomplished through amulti-sensor approach by placing it in a common orbit in tandem with the Sentinel-3 (S3) mission, which willhave two optical sensors on board, OLCI (Ocean and Land Colour Instrument) and SLSTR (Sea and Land SurfaceTemperature Radiometer) to complement FLEX. These S3 instruments will be used in combination with theimaging spectrometers on board FLEX to provide data useful for atmospheric correction of FLEX data. However,a fully synergetic approach, i.e. by exploiting the spectral and directional information from all tandem missioninstruments together, is an attractive alternative which is explored in this paper. By employing all combined topof-atmosphere (TOA) spectral radiance data, one can (i) characterize the relevant optical properties of the atmosphere,(ii) retrieve biophysical canopy properties including the associated reflectance anisotropy, and (iii)retrieve a more accurate and consistent canopy F.Regarding retrieval methods, Fraunhofer Line Depth (FLD) and Spectral Fitting (SF) are well-known techniquesapplied to hyperspectral data. Both methods depend on a high spectral resolution and assume aLambertian (isotropic) canopy reflectance. However, most vegetation canopies are non-Lambertian. This impliesthat, in particular when ignoring the anisotropic surface reflection, substantial retrieval errors can occur due tothe interaction between atmospheric absorption bands and surface reflectance anisotropy. In this paper, a novelmethod based on spectral radiative transfer (RT) modeling is proposed, in which coupled RT models are used tosimulate TOA radiance spectra. These are then matched with ‘measured' spectra in order to retrieve surfacefluorescence, along with a suite of biophysical parameters, by model inversion through optimization. By applyingcoupled RT models of the soil-leaf-canopy and the surface-atmosphere systems, TOA radiance spectra canbe simulated for all optical sensors of this tandem mission. In this way, complex effects due to surface reflectanceanisotropy and the spectral sampling by the various instruments, which are difficult to compensate for in the endproducts, are properly taken into account by their incorporation in the forward modeling. Next, by model inversionof TOA radiance data via optimization, the most accurate F retrievals can be achieved in a consistentmanner, along with important canopy level biophysical parameters that may help interpret the F spectrum, suchas chlorophyll content and leaf area index (LAI). The potential of this approach has been explored in a numericalexperiment, and the results are presented in this paper. We find that, with the assumed well-characterized andplausible FLEX/S3 instrument performances, the simultaneous retrieval of biophysical canopy parameters and Fspectra would be possible with a remarkable accuracy, provided the correct atmospheric characterization isavailable.

Verhoef, Wouter↗

Depth‐ and Time‐Resolved Distributions of Snowmelt‐Driven Hillslope Subsurface Flow and Transport and Their Contributions to Surface Waters

Abstract Major components of hydrologic and elemental cycles reside underground, where their complex dynamics and linkages to surface waters are obscure. We delineated seasonal subsurface flow and transport dynamics along a hillslope in the Rocky Mountains (USA), where precipitation occurs primarily as winter snow and drainage discharges into the East River, a tributary of the Gunnison River. Hydraulic and geochemical measurements down to 10 m below ground surface supported application of transmissivity feedback of snowmelt to describe subsurface flow and transport through three zones: soil, weathering shale, and saturated fractured shale. Groundwater flow is predicted to depths of at least 176 m, although a shallower limit exists if hillslope‐scale hydraulic conductivities are higher than our local measurements. Snowmelt during the high snowpack water year 2017 sustained flow along the weathering zone and downslope within the soil, while negligible downslope flow occurred along the soil during the low snowpack water year 2018. We introduce subsurface concentration‐discharge ( C‐Q ) relations for explaining hillslope contributions to C‐Q observed in rivers and demonstrate their calculations based on transmissivity fluxes and measured pore water specific conductance and dissolved organic carbon. The specific conductance data show that major ions in the hillslope pore waters, primarily from the weathering and fractured shale, are about six times more concentrated than in the river, indicating hillslope solute loads are disproportionately high, while flow from this site and similar regions are relatively smaller. This methodology is applicable in different representative environments within snow‐dominated watersheds for linking their subsurface exports to surface waters.

54 ENVIRONMENTAL SCIENCES↗

Method and apparatus for detecting and quantifying bacterial spores on a surface

A method and an apparatus for detecting and quantifying bacterial spores on a surface. In accordance with the method: bacterial spores are transferred from a place of origin to a test surface, the test surface comprises lanthanide ions. Aromatic molecules are released from the bacterial spores; a complex of the lanthanide ions and aromatic molecules is formed on the test surface, the complex is excited to generate a characteristic luminescence on the test surface; the luminescence on the test surface is detected and quantified.

Ponce, Adrian↗