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At least 145 records · Page 8

Ground-based SMART-COMMIT Measurements for Studying Aerosol and Cloud Properties

From radiometric principles, it is expected that the retrieved properties of extensive aerosols and clouds from reflected/emitted measurements by satellite (and/or aircraft) should be consistent with those retrieved from transmitted/emitted radiance observed at the surface. Although space-borne remote sensing observations cover large spatial domain, they are often plagued by contamination of surface signatures. Thus, ground-based in-situ and remote-sensing measurements, where signals come directly from atmospheric constituents, the sun, and/or the Earth-atmosphere interactions, provide additional information content for comparisons that confirm quantitatively the usefulness of the integrated surface, aircraft, and satellite data sets. The development and deployment of SMARTCOMMIT (Surface-sensing Measurements for Atmospheric Radiative Transfer - Chemical, Optical & Microphysical Measurements of In-situ Troposphere) mobile facilities are aimed for the optimal utilization of collocated ground-based observations as constraints to yield higher fidelity satellite retrievals and to determine any sampling bias due to target conditions. To quantify the energetics of the surface-atmosphere system and the atmospheric processes, SMART-COMMIT instruments fall into three categories: flux radiometer, radiance sensor and in-situ probe. In this paper, we will demonstrate the capability of SMART-COMMIT in recent field campaigns (e.g., CRYSTAL-FACE, UAE 2, BASEASIA, NAMMA) that were designed and executed to study the compelling variability in temporal scale of both anthropogenic and natural aerosols (e.g., biomass-burning smoke, airborne dust) and cirrus clouds. We envision robust approaches in which well-collocated ground-based measurements and space-borne observations will greatly advance our knowledge of extensive aerosols and clouds.

Tsay, Si-Chee↗

Surface Temperature and the Compositional Effects of Electron Bombardment on Dione

Saturn’s icy moons are composed of mostly water ice with minor “contaminants,” such as CO2 ice, and a dark component thought to be organics, hematite and/or metallic Fe [1]. The space weathering process of electron bombardment is expected to be particularly important on the surfaces of Saturn’s inner moons (Mimas, Tethys, Dione, and Rhea), as they orbit within the extended plasma sheet of Saturn’s magnetosphere. Terrains exhibiting thermal anomalies (i.e., colder temperatures in the day and warmer temperatures at night than surrounding areas) correspond to regions of high energy electron bombardment [2; 3]. Energetic electrons impact the surfaces, fracturing ice particles into sub-micron sized grains, and this process becomes more effective for increasing particle energies [4]. In addition to alteration of ices, the dark material may also be modified or generated within icy surfaces by interaction with solar UV radiation, cosmic rays, or by particles trapped in Saturn’s magnetic field [5]. CO2 could be sourced from irradiation of dark organic material [7]. Many of these alterations should be observable in Visible and Infrared Mapping Spectrometer (VIMS) spectra [8]. We used surface temperatures derived from Cassini’s Composite Infrared Spectrometer (CIRS) to help isolate areas where space weathering due to electron bombardment is more predominant and investigated the subtle changes in VIMS spectra using machine learning techniques. We present our results here for Dione. On ocean worlds, space weathering products would be present along with any potential indications of life. We will need to understand the manifestation of space weathering in the data to separate the two processes.

Cindy Lee Young↗

A molecular model for ice nucleation and growth, attachment 1

The quantum mechanical technique is used to study ionic, configurational, and impurity defects in the ice surface. In addition to static calculations of the energetics of the water monomer-ice surface interactions, molecular dynamics studies were initiated. The calculations of the monomer-ice surface interaction, molecular dynamics studies were initiated. The calculations of monomer-ice surface interactions indicate that many adsorption sites exist on the ice surfaces and that the barriers between bonding sites are relatively low. Bonding on the prism face of ice is preferentially above lattice sites.

Plummer, P. L. M.↗

Simulating the Diffusion of Hydrogen in Amorphous Silicates: A ‘Jumping’ Migration Process and its Implications for Solar Wind Implanted Lunar Volatiles

We use molecular dynamics (MD) simulations to better explain the movement of atomic hydrogen in amorphous silica and quantify the planetary science implications of these findings. Previous MD simulations had a large range of predicted values and did not agree well with experiment. Our simulations sample atomic motion for a longer duration and consider a wider range of temperatures than previous simulations. In contrast to constant atomic motion, the hydrogen atoms were shown to undergo random intermittent jumps from one oxygen atom to another, the number of which increase with temperature. Predicted diffusion coefficients had a better agreement to experimental values than previous MD simulations, suggesting the importance of longer simulation durations for better statistics. The low activation energy and jumps observed at lunar temperatures do not support the theory of diurnal variations in OH content for an undamaged amorphous silica surface. Instead, we conclude that energetic solar wind impacts can induce two competing atomic hydrogen motion processes in the exposed surface: A prompt effect that induces jumps in the temperature spike volume, but also a long term effect of damage in the structure that traps atomic hydrogen. We then use SDTrimSP to quantify the damage created during exposure and MD to demonstrate the H retention and trapping near these defects. Damage was shown to be dependent on impact energy, with defects easily retaining implanted hydrogen. MD results like those presented herein on unweathered surfaces are therefore most relevant to magnetic anomalies. As a result, we demonstrate the importance of lunar volatile models to account for the damage state of the substrate when modelling hydrogen diffusion, retention, and subsequent OH/water production.

Liam S. Morrissey↗

Mars' Surface Radiation Environment Measured with the Mars Science Laboratory's Curiosity Rover

The Radiation Assessment Detector (RAD) on the Mars Science Laboratorys Curiosity rover beganmaking detailed measurements of the cosmic ray and energetic particle radiation environmenton the surface of Mars on 7 August 2012. We report and discuss measurements of the absorbeddose and dose equivalent from galactic cosmic rays and solar energetic particles on the martiansurface for 300 days of observations during the current solar maximum. These measurementsprovide insight into the radiation hazards associated with a human mission to the surface of Marsand provide an anchor point with which to model the subsurface radiation environment, withimplications for microbial survival times of any possible extant or past life, as well as for thepreservation of potential organic biosignatures of the ancient martian environment.

radiation environment↗

Advanced Pt-Based Core–Shell Electrocatalysts for Fuel Cell Cathodes

Proton-exchange membrane fuel cells (PEMFCs) are highly efficient energy storage and conversion devices. Thus, the platinum group metal (PGM)-based catalysts which are the dominant choice for the PEMFCs have received extensive interest during the past couple of decades. However, the drawbacks in the existing PGM-based catalysts (i.e., high cost, slow kinetics, poor stability, etc.) still limit their applications in fuel cells. The Pt-based core–shell catalysts potentially alleviate these issues through the low Pt loading with the associated low cost and the high corrosion resistance and further improve the oxygen reduction reaction’s (ORR’s) activity and stability. This Account focuses on the synthetic strategies, catalytic mechanisms, factors influencing enhanced ORR performance, and applications in PEMFCs for the Pt-based core–shell catalysts. We first highlight the synthetic strategies for Pt-based core–shell catalysts including the galvanic displacement of an underpotentially deposited non-noble metal monolayer, thermal annealing, and dealloying methods, which can be scaled-up to meet the requirements of fuel cell operations. Subsequently, catalytic mechanisms such as the self-healing mechanism in the Pt monolayer on Pd core catalysts, the pinning effect of nitrogen (N) dopants in N-doped PtNi core–shell catalysts, and the ligand effect of the ordered intermetallic structure in L10-Pt/CoPt core–shell catalysts and their synergistic effects in N-doped L10-PtNi catalysts are described in detail. Additionally, the core–shell structure in the Pt-based catalysts have two main effects for enhanced ORR performance: (i) the interaction between Pt shells and core substrates can tune the electronic state of the surface Pt, thus boosting the ORR activity and stability, and (ii) the outer Pt shell with modest thickness can enhance the oxidation and dissolution resistance of the core, resulting in improved durability. We then review the recent attempts to optimize the ORR performance of the Pt-based core–shell catalysts by considering the shape, composition, surface orientation, and shell thickness. The factors influencing the ORR performance can be grouped into two categories: the effect of the core and the effect of the shell. In the former, PtM core–shell catalysts which use different non-PGM element cores (M) are summarized, and in the latter, Pt-based core–shell catalysts with different shell structures and compositions are described. The modifications of the core and/or shell structure can not only optimize the intermediate-binding energetics on the Pt surface through tuning the strain of the surface Pt, which increases the intrinsic activity and stability, but also offer a significantly decreased catalyst cost. Finally, we discuss the membrane electrode assembly performance of Pt-based core–shell catalysts in fuel cell cathodes and evaluate their potential in real PEMFCs for light-duty and heavy-duty vehicle applications. Even though some challenges to the activity and lifetime in the fuel cells remain, the Pt-based core–shell catalysts are expected to be promising for many practical PEMFC applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ground-based Network and Supersite Measurements for Studying Aerosol Properties and Aerosol-Cloud Interactions

From radiometric principles, it is expected that the retrieved properties of extensive aerosols and clouds from reflected/emitted measurements by satellite (and/or aircraft) should be consistent with those retrieved from transmitted/emitted radiance observed at the surface. Although space-borne remote sensing observations contain large spatial domain, they are often plagued by contamination of surface signatures. Thus, ground-based in-situ and remote-sensing measurements, where signals come directly from atmospheric constituents, the sun, and the Earth-atmosphere interactions, provide additional information content for comparisons that confirm quantitatively the usefulness of the integrated surface, aircraft, and satellite datasets. The development and deployment of AERONET (AErosol RObotic NETwork) sunphotometer network and SMART-COMMIT (Surface-sensing Measurements for Atmospheric Radiative Transfer - Chemical, Optical & Microphysical Measurements of In-situ Troposphere) mobile supersite are aimed for the optimal utilization of collocated ground-based observations as constraints to yield higher fidelity satellite retrievals and to determine any sampling bias due to target conditions. To characterize the regional natural and anthropogenic aerosols, AERONET is an internationally federated network of unique sunphotometry that contains more than 250 permanent sites worldwide. Since 1993, there are more than 480 million aerosol optical depth observations and about 15 sites have continuous records longer than 10 years for annual/seasonal trend analyses. To quantify the energetics of the surface-atmosphere system and the atmospheric processes, SMART-COMMIT instrument into three categories: flux radiometer, radiance sensor and in-situ probe. Through participation in many satellite remote-sensing/retrieval and validation projects over eight years, SMART-COMMIT have gradually refine( and been proven vital for field deployment. In this paper, we will demonstrate the capability of AERONET SMART-COMMIT in current Asian Monsoon Year-2008 campaigns that are designed and being executed to study the compelling variability in temporal scale of both anthropogenic and natural aerosols (e.g., airborne dust, smoke, mega-city pollutant). Feedback mechanisms between aerosol radiative effects and monsoon dynamics have been recently proposed, however there is a lack of consensus on whether aerosol forcing would be more likely to enhance or reduce the strength of the monsoon circulation. We envision robust approaches which well-collocated ground-based measurements and space-borne observations will greatly advance our understanding of absorbing aerosols (e.g., "Global Dimming" vs. "Elevated Heat-Pump" effects) on aerosol cloud water cycle interactions.

Tsay, Si-Chee↗

A spectroscopic experimental and computer-assisted empirical model for the production and energetics of excited oxygen molecules formed by atom recombination on shuttle tile surfaces

A visible emission spectroscopic method was developed. The amounts of excited singlet and triplet oxygen molecules produced by recombination on the Space Shuttle Orbiter thermal protective tiles at elevated temperatures are determined. Rate constants and energetics of the extremely exothermic reaction are evaluated in terms of a chemical and mathematical model. Implications for potential contribution to Shuttle surface reentry heating fluxes are outlined.

Owan, D. A.↗

The Chemistry of Pluto and its Satellites

Pluto's bulk composition and the composition of the surface layers hold clues to the origin and evolution of a number of other Solar System bodies of comparable size in the region beyond Neptune. The July 14, 2015 flyby of the Pluto system with the New Horizons spacecraft afforded the opportunity to corroborate and greatly improve discoveries about the planet and its satellites derived Earth-based studies. It also revealed extraordinary details of the surface and atmosphere of Pluto, as well as the geology and composition of Charon and two smaller satellites. With a mean density of 1.86 g/sq cm, the bulk composition of Pluto is about two-thirds anhydrous solar composition rocky material and one-third volatiles (primarily H2O in liquid and solid states) by mass, the surface is a veneer of ices dominated by N2, with smaller amounts of CH4 and CO, as well as limited exposures of H2O ice (considered to be "bedrock"). N2, CH4, and CO occur as solid solutions at temperature-dependent mutual concentrations, each component being soluble in the others. Frozen C2H6 as a minor component has also been identified. Sublimation and recondensation of N2, CH4, and CO over seasonal (248 y) and Milankovich-type megaseasons (approx. 3 My) result in the redistribution of these ices over time and with latitude control. Solid N2 is found in glaciers originating in higher elevations and flowing at the present time into a basin structure larger than the State of Texas, forming a convecting lens of N2 that overturns on a timescale of order 10 My. The varied colors of Pluto's landscape arise from the energetic processing of the surface ices in processes that break the simple molecules and reassemble complex organic structures consisting of groups of aromatic rings connected by aliphatic chains. When synthesized in the laboratory by UV or electron irradiation of a Pluto mix of ice, this material, called tholin, has colors closely similar to Pluto. The Pluto ice tholin analog contains carboxylic acids, urea, ketones, aldehydes, amines, and some nitriles. The largest satellite, Charon has density 1.70 g/sq cm and it is about 3/5 anhydrous solar composition rock, with the remainder in H2O ice. The surface H2O ice is infused in some way with NH3, probably as a hydrate, distributed nonuniformly, but to some degree related to geological structures. Pluto's atmosphere is N2, CH4, with CO, C2-hydrocarbons, HCN, and other molecules in trace but detectable amounts. The atmosphere supports a complex haze structure with about 20 discrete layers, and suspected clouds. The haze is presumed to be made of aggregates of complex hydrocarbons (tholins) produced by photolysis of the atmospheric gases, and with similar composition to the ice tholins made on the planet's surface. Urea and a suite of carboxylic acids are of interest for prebiotic and biological chemistries.

SOLAR SYSTEMS↗

A molecular view of peptoid-induced acceleration of calcite growth

The extensive deposits of calcium carbonate (CaCO 3 ) generated by marine organisms constitute the largest and oldest carbon dioxide (CO 2 ) reservoir. These organisms utilize macromolecules like peptides and proteins to facilitate the nucleation and growth of carbonate minerals, serving as an effective method for CO 2 sequestration. However, the precise mechanisms behind this process remain elusive. In this study, we report the use of sequence-defined peptoids, a class of peptidomimetics, to achieve the accelerated calcite step growth kinetics with the molecular level mechanistic understanding. By designing peptoids with hydrophilic and hydrophobic blocks, we systematically investigated the acceleration in step growth rate of calcite crystals using in situ atomic force microscopy (AFM), varying peptoid sequences and concentrations, CaCO 3 supersaturations, and the ratio of Ca 2+ / HCO 3 − . Mechanistic studies using NMR, three-dimensional fast force mapping (3D FFM), and isothermal titration calorimetry (ITC) were conducted to reveal the interactions of peptoids with Ca 2+ and HCO 3 − ions in solution, as well as the effect of peptoids on solvation and energetics of calcite crystal surface. Our results indicate the multiple roles of peptoid in facilitating HCO 3 − deprotonation, Ca 2+ desolvation, and the disruption of interfacial hydration layers of the calcite surface, which collectively contribute to a peptoid-induced acceleration of calcite growth. These findings provide guidelines for future design of sequence-specific biomimetic polymers as crystallization promoters, offering potential applications in environmental remediation (such as CO 2 sequestration), biomedical engineering, and energy storage where fast crystallization is preferred.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Growth of topological insulator Bi 2 Se 3 particles on GaAs via droplet epitaxy

The discovery of topological insulators (TIs) and their unique electronic properties has motivated research into a variety of applications, including quantum computing. It has been proposed that TI surface states will be energetically discretized in a quantum dot nanoparticle. These discretized states could then be used as basis states for a qubit that is more resistant to decoherence. In this work, prototypical TI Bi2Se3 nanoparticles are grown on GaAs (001) using the droplet epitaxy technique, and we demonstrate the control of nanoparticle height, area, and density by changing the duration of bismuth deposition and substrate temperature. Within the growth window studied, nanoparticles ranged from 5 to 15 nm in height with an 8–18 nm equivalent circular radius, and the density could be relatively well controlled by changing the substrate temperature and bismuth deposition time.

Materials Science↗

A model for Io's atmosphere and sodium cloud

Observations of the sodium D-line emissions associated with the Galilean satellite Io suggest that the emitting region has two components. The first is an atmosphere which extends 1000 km above Io's surface. This is a relatively dense region which is optically thick in the sodium D lines. The second component is a surrounding optically thin cloud spread out along Io's orbit to form part of a torus. No emission was detected during any of three eclipses observed, although Io's sodium emission was consistently present when Io was near orbital elongation. This indicates that resonant scattering is the principal emission mechanism in both components. For the atmosphere, measurements of the D-line intensity, D-2/D-1 ratio, and line width indicate a temperature of 500 to 1000 K and a sodium column abundance of 3 by 10 to the 13th power per sq cm. Upper limits to the abundance of Mg, K, Ca, and Li indicate a high sodium abundance ratio in the atmosphere. This may also be true for Io's surface if sputtering by energetic particles is the source of the atmosphere. The sodium cloud has been detected as far as 60 arcsec from Io in the orbital plane and at least 6 arcsec above and below this plane. The cloud can be sustained by atoms escaping from the critical level at the top of the atmosphere.

Macy, W., Jr.↗

Negative ions in the ionospheres of planetary bodies without atmospheres

It is noted that negative ions may be formed in the ionospheres of Mercury, the moon, and Jupiter's satellites with densities of a few percent of the ionospheric electron density. Negative ions result from three mechanisms at the planetary surface: charge inversion during energetic proton scattering, with simultaneous secondary negative ion emission, and micrometeorite impacts. The density and distribution of negative ions around planetary bodies depends primarily on the negative ion lifetimes determined through photodetachment by solar radiation.

Wekhof, A.↗

A four-dimensional primitive equation model for coupled coastal-deep ocean studies

A prototype four dimensional continental shelf/deep ocean model is described. In its present form, the model incorporates the effects of finite amplitude topography, advective nonlinearities, and variable stratification and rotation. The model can be forced either directly by imposed atmospheric windstress and surface pressure distributions, and energetic mean currents imposed by the exterior oceanic circulation; or indirectly by initial distributions of shoreward propagation mesoscale waves and eddies. To avoid concerns over the appropriate specification of 'open' boundary conditions on the cross-shelf and seaward model boundaries, a periodic channel geometry (oriented along-coast) is used. The model employs a traditional finite difference expansion in the cross-shelf direction, and a Fourier (periodic) representation in the long-shelf coordinate.

Haidvogel, D. B.↗

Simulation studies for surfaces and materials strength

Three different investigations based on computer simulations were carried out. Simulation calculations were performed using model potentials with two- and three-body interactions which were represented by the Mie and the Axilrod-Teller potentials, respectively. In the first part, to analyze stability criteria for simple crystals, a parametrical investigation was performed and stability regions for five different crystalline structures were determined with respect to potential energy parameters. To simulate some of the basic surface processes such as diffusion and nucleation, in the second and third parts, silicon surfaces were considered as a specific example. In these studies diffusion of adatoms on stepped surfaces were simulated and energetics associated with the formation of kink sites were calculated.

Halicioglu, Timur↗

Integration of space and in situ observations to study global climate change

The use of model-based global data sets of atmospheric circulation for studying fundamental dynamical and physical processes is discussed, focusing on limitations of the available model-based data sets. Data from the Global Weather Experiment in 1979 were analyzed by two authorized level IIIb data centers in 1980 and in 1981. The analyses led to difference in data-sparse regions such as the tropics. Study areas which can be addressed by an internally-consistent long-term multivariate data set for the atmospheric circulation are considered, including mean climate, forcing for the ocean models, global hydrological cycle, atmospheric energetics, intraseasonal variability, land surface processes, and structure and variability of vertical velocity, divergence, and diabatic heating. It is concluded that the most comprehensive technique for integrating space and in situ observations to produce this type of data set would be a four-dimensional data assimilation system with a realistic physical model of the type employed in operational numerical weather prediction.

Bengtsson, L.↗

Solar proton produced neon in shergottite meteorites

Cosmogenic radionuclides produced by near-surface, nuclear interactions of energetic solar protons (approx. 10-100 MeV) were reported in several lunar rocks and a very small meteorites. We recently documented the existence and isotopic compositions of solar-produced (SCR) Ne in two lunar rocks. Here we present the first documented evidence for SCR Ne in a meteorite, ALH77005, which was reported to contain SCR radionuclides. Examination of literature data for other shergottites suggests that they may also contain a SCR Ne component. The existence of SCR Ne in shergottites may be related to a Martian origin.

Garrison, D. H.↗

Following the Oxidants to Enceladus

Potentially habitable bodies beyond the Earth are expected at minimum to have organics, liquid water, and oxidants. Simple hydrocarbon organics, potentially from breakdown of more complex molecules, have been measured in the plume gas of Enceladus, and a subsurface liquid reservoir may account in some models for the plume activity. Spectroscopic surface remote sensing measurements from other icy moons, and laboratory investigations of oxidant production in irradiated ices, all suggest that radiolytic oxidants should be abundantly produced in the upper ice crust of Enceladus from surface irradiation by magnetospheric energetic particles of Saturn. Potential oxidant inputs to astrobiology on Enceladus are compared to those at Europa, for which there is more definitive evidence for subsurface water but the presence of organics at significant abundances has yet to be established.

Cooper, John F.↗