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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Developing Platinum-Group-Metal-Free Catalysts for Oxygen Reduction Reaction in Acid: Beyond the Single Metal Site

This project is to develop M (x) -N-C catalysts with dense multiple metal center (MMC) sites to meet the DOE 2025 activity target of 0.044 mA/cm 2 at 0.9 V IR-free ., as well as other goals such as durability. We have made important contributions to both catalyst development and fundamental understandings of the active sites in M-N-C catalysts in this project. We successfully made M (x) -N-C catalysts with some multiple metal center (MMC) sites by combining ionothermal carbonization with chemical vapor deposition (CVD). These catalysts, however, are not as active as the most active single-atom Fe-N-C catalysts made by the similar CVD process, owing likely to the low site density and the presence of inorganic Fe species such as iron carbides and nanoparticles. The most significant accomplishments we achieved in this project are: (1) we unraveled the formation pathway of Fe-N 4 sites during pyrolysis step-by-step and identified the trans-metalation mechanism, in collaboration with Deborah Myers and her colleagues at Argonne National Laboratory (ANL); (2) inspired by this finding, we pioneered the CVD synthesis of M-N-C catalysts (M = Mn, Fe, and Co), in which the Fe-N-C catalyst by CVD demonstrated an ORR activity of 33 mA/cm 2 at 0.9 V in H 2 -O 2 proton exchange membrane fuel cells (PEMFCs), very close to the ultimate goal of 35 mA/cm 2 of our project. This catalyst is the first Fe-N-C catalyst that contains only D1 sites without the D2 sites; whereas D1 and D2 sites have been always identified by Mossbauer in previous Fe-N-C catalysts. This finding helps to understand what the D1 and D2 sites are and their roles in catalyzing the ORR. (3) by improving the mass transport of the carbon matrix prior to the CVD process, the revised Fe-N-C catalyst made by CVD delivered a maximum power density of 0.53 W/cm 2 in H 2 -air PEMFCs. The improvement strategy was partly inspired by the computational modeling work by Adam Weber from LBNL, the Co-PI of this project, by developing, coding, and exercising a continuum level model of transport phenomena within a PGM-free catalyst layer. The model demonstrated that local resistances combined with limited site density of the PGM-free catalyst can result in limiting currents and poor polarization performance. The model also gave design guidance for impact of ECSA and overall catalyst-layer thickness. However, both Fe-N-C and Co-N-C catalysts developed by CVD showed poor durability in PEMFCS, in comparison with the traditional M-N-C catalysts synthesized via regular pyrolysis process. Consequently, we did not achieve the proposed durability targets. Despite so, we believe the FeNC-CVD catalysts with the poor durability and D1 sites only provides an excellent platform to understand the degradation mechanism of Fe-N-C in PEMFCs, the most important challenge in the development of M-N-C catalysts.

08 HYDROGEN↗
DOE OSTI2025

Light control of intramolecular nuclear dynamics by vortex electron localization

In strong-field ionization of molecules, intense light pulses are thought to have a negligible direct influence on atomic nuclei. Molecular dissociation is thus expected to be determined by the geometrical configuration of the molecular ion at the ionization instant. Contrary to this picture, we observe a counterintuitive electron-proton angular correlation and the formation of proton vortices following strong-field ionization of H 2 molecules by bicircularly polarized two-color laser fields. We explain this phenomenon by the pathway interference and localization of the residual H 2 ⁡+ electron in different angular-momentum states formed in the tail of the driving laser pulse. We validate this interpretation by combining a quantum-mechanical numerical simulation of the field-driven coupled electronic-nuclear dynamics and a semiclassical-trajectory model for the phase accumulation of the laser-driven electronic-nuclear wave packet. Our joint experimental and theoretical study reveals a general picture of vortex electron localization which can be used for controlling molecular-bond breaking with circularly polarized laser fields.

Atomic & molecular processes in external fields↗
NASA NTRS2019

Technology Development for the Modification of High Aspect Ratio Geometries for Thermal and Environmental Control

A key technology development driver in environmental control systems and next generation optics are discussed utilizing thin film development borrowed from the semiconductor industry. The optical and physical properties of spacecraft radiator coatings are dictated by orbital environmental conditions. For example, coatings must adequately dissipate charge buildup when orbital conditions, such as polar, geostationary or gravity neutral, result in surface charging. Current dissipation techniques include depositing a layer of ITO (indium tin oxide) on the radiator surface in a high temperature process. The application of these enhanced coatings must be such that the properties in question are tailored to mission-specific requirements. The multi-billion-dollar semiconductor industry has adopted Atomic Layer Deposition (ALD) for self-assembly and atomic-scale placement. ALD is a cost-effective nanoadditive-manufacturing technique that allows for the conformal coating of substrates with atomic control in a benign temperature and pressure environment. By using ALD, modification of these coatings can be accomplished during coating application preprocessing. The preprocessing is rendered directly on the coating dry pigment before binding. Through the introduction of paired precursor gases, thin films can be deposited on a myriad of substrates ranging from glass, polymers, aerogels, metals, powders, and other high aspect-ratio micro- and nano- structures. By providing atomic-level control, where single layers of atoms can be deposited, the fabrication of metal transparent films, precise nano-laminates, and coatings of nano-channels and pores is achievable. A method has been demonstrated for the ALD of In2O3 and films on a variety of substrates from Si(100) wafers, glass slides, and on Z93P pigments resulting in a direct spaceflight application. Results will be presented that verify the chemical composition of ALD pigments and charge dissipation properties when the pigment goes through its binding and coating process and we present early results of ALD for carbon nanotube formation and encapsulation.

Dwivedi, Vivek H.↗
NASA NTRS2019

Application and Development of Atomic Layer Deposition Techniques to Improve Thermo-Optical Coatings for Spacecraft Thermal Control and Advanced Optical Instruments

A key technology development driver in environmental control systems and next generation optics are discussed utilizing thin film development borrowed from the semiconductor industry. The optical and physical properties of spacecraft radiator coatings are dictated by orbital environmental conditions. For example, coatings must adequately dissipate charge buildup when orbital conditions, such as polar, geostationary or gravity neutral, result in surface charging. Current dissipation techniques include depositing a layer of ITO (indium tin oxide) on the radiator surface in a high temperature process. The application of these enhanced coatings must be such that the properties in question are tailored to mission-specific requirements. The multi-billion-dollar semiconductor industry has adopted Atomic Layer Deposition (ALD) for self-assembly and atomic-scale placement. ALD is a cost-effective nanoadditive-manufacturing technique that allows for the conformal coating of substrates with atomic control in a benign temperature and pressure environment. By using ALD, modification of these coatings can be accomplished during coating application preprocessing. The preprocessing is rendered directly on the coating dry pigment before binding. Through the introduction of paired precursor gases, thin films can be deposited on a myriad of substrates ranging from glass, polymers, aerogels, metals, powders, and other high aspect-ratio micro- and nano- structures. By providing atomic-level control, where single layers of atoms can be deposited, the fabrication of metal transparent films, precise nano-laminates, and coatings of nano-channels and pores is achievable. A method has been demonstrated for the ALD of In2O3 and films on a variety of substrates from Si(100) wafers, glass slides, and on Z93P pigments resulting in a direct spaceflight application. Results will be presented that verify the chemical composition of ALD pigments and charge dissipation properties when the pigment goes through its binding and coating process and we present early results of ALD for carbon nanotube formation and encapsulation.

Dwivedi, Vivek H.↗
DOE OSTI2015

Solvation thermodynamics of amino acid side chains on a short peptide backbone

The hydration process of side chain analogue molecules differs from that of the actual amino acid side chains in peptides and proteins owing to the effects of the peptide backbone on the aqueous solvent environment. A recent molecular simulation study has provided evidence that all nonpolar side chains, attached to a short peptide backbone, are considerably less hydrophobic than the free side chain analogue molecules. In contrast to this, the hydrophilicity of the polar side chains is hardly affected by the backbone. To analyze the origin of these observations, we here present a molecular simulation study on temperature dependent solvation free energies of nonpolar and polar side chains attached to a short peptide backbone. The estimated solvation entropies and enthalpies of the various amino acid side chains are compared with existing side chain analogue data. The solvation entropies and enthalpies of the polar side chains are negative, but in absolute magnitude smaller compared with the corresponding analogue data. The observed differences are large; however, owing to a nearly perfect enthalpy-entropy compensation, the solvation free energies of polar side chains remain largely unaffected by the peptide backbone. We find that a similar compensation does not apply to the nonpolar side chains; while the backbone greatly reduces the unfavorable solvation entropies, the solvation enthalpies are either more favorable or only marginally affected. This results in a very small unfavorable free energy cost, or even free energy gain, of solvating the nonpolar side chains in strong contrast to solvation of small hydrophobic or nonpolar molecules in bulk water. The solvation free energies of nonpolar side chains have been furthermore decomposed into a repulsive cavity formation contribution and an attractive dispersion free energy contribution. We find that cavity formation next to the peptide backbone is entropically favored over formation of similar sized nonpolar side chain cavities in bulk water, in agreement with earlier work in the literature on analysis of cavity fluctuations at nonpolar molecular surfaces. The cavity and dispersion interaction contributions correlate quite well with the solvent accessible surface area of the nonpolar side chains attached to the backbone. This correlation however is weak for the overall solvation free energies owing to the fact that the cavity and dispersion free energy contributions are almost exactly cancelling each other.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1989

Properties of grains derived from IRAS observations of dust

The authors used the results of Infrared Astronomy Satellite (IRAS) observations of diffuse medium dust to develop a theoretical model of the infrared properties of grains. Recent models based entirely on traditional observations of extinction and polarization include only particles whose equilibrium temperatures do not exceed 20 K in the diffuse interstellar medium. These classical grains, for which the authors have adopted the multipopulation model developed by Hong and Greenberg (1980), can explain only the emission in the IRAS 100 micron band. The measurements at shorter wavelengths (12, 25 and 60 microns) require two new particle populations. Vibrational fluorescence from aromatic molecules provides the most likely explanation for the emission observed at 12 microns, with polycyclic aeromatic hydrocarbons (PAHs) containing about 10 percent of cosmic carbon. A simplified model of the emission process shows that PAH molecules can also explain most of the emission measured by IRAS at 25 microns. The authors identified the warm particles responsible for the excess 60 microns emission with small (a approx. equals 0.01 microns) iron grains. A compilation of the available data on the optical properties of iron indicates that the diffuse medium temperature of small iron particles should be close to 50 K and implies that a large, possibly dominant, fraction of cosmic iron must be locked up in metallic particles in order to match the observed 60 microns intensities. The model matches the infrared fluxes typically observed by IRAS in the diffuse medium and can also reproduce the infrared surface brightness distribution in individual clouds. In particular, the combination of iron and classical cool grains can explain the surprising observations of the 60/100 microns flux ratio in clouds, which is either constant or increases slightly towards higher opacities. The presence of metallic grains has significant implications for the physics of the interstellar medium, including catalytic H2 formation, for which iron grains could be the main site; differences in depletion patterns between iron and other refractory elements (Mg, Si); and superparamagnetic behavior of large grains with embedded iron clusters giving rise to the observed high degree of alignment by the galactic magnetic field.

Wesselius, P. R.↗
NASA NTRS1994

Mars atmospheric loss and isotopic fractionation by solar-wind-induced sputtering and photochemical escape

We examine the effects of the loss of Mars atmospheric constituents by solar-wind-induced sputtering and by photochemical escape during the past 3.8 billion years. Sputtering is capable of efficiently removing species from the upper atmosphere, including the light noble gases; nitrogen and oxygen are removed by photochemical processes as well. Due to diffusive separation (by mass) above the homopause, removal from the top of the atmosphere will fractionate the isotopes of each species, with the lighter mass being preferentially lost. For carbon and oxygen, this allows us to determine the size of nonatmospheric reservoirs which mix with the atmosphere; these reservoirs can be CO2 adsorbed in the regolith and H2O in the polar ice caps. We have constructed both simple analytical models and time-dependent models of the loss of volatiles from and supply to the martian atmosphere. Both argon and neon require continued replenishment from outgassing over geologic time. For argon, sputtering loss explains the fractionation of (Ar-36)/(Ar-38) without requiring a distinct epoch of hydrodynamic escape (although fractionation of Xe isotopes still requires very early hydrodynamic loss). For neon, the current (Ne-22)/(Ne-20) ratio represents a balance between loss to space and continued resupply from the interior; the similarity of the ratio to the terrestrial value is coincidental. For nitrogen, the loss by both sputtering and photochemical escape would produce a fractionation of (N-15)/(N-14) larger than observed; an early, thicker carbon dioxide atmosphere could mitigate the nitrogen loss and produce the observed fractionation, as could continued outgassing of juvenile nitorgen. Based on the isotopic constraints, the total amount of carbon dioxide lost over geologic time is probably on the order of tens of millibars rather than a substantial fraction of a bar. The total loss from solar-wind-induced sputtering and photochemical escape, therefore, does not seem able to explain the loss of a putative thick, early atmosphere withput requiring formation of extensive surface carbonate deposits or other nonatmospheric reservoirs for CO2.

Jakosky, Bruce M.↗
DOE OSTI2017

Formation of gapless Z{sub 2} spin liquid phase manganites in the (Sm{sub 1–y}Gd{sub y}){sub 0.55}Sr{sub 0.45}MnO{sub 3} system in zero magnetic field: Topological phase transitions to states with low and high density of 2D-vortex pairs induced by the magnetic field

The evolution of the ground state of the manganese spin ensemble in the (Sm{sub 1–y}Gd{sub y}){sub 0.55}Sr{sub 0.45}MnO{sub 3} in the case of isovalent substitution of rare-earth samarium ions with large radii with gadolinium ions with significantly smaller radii is studied. The measured temperature dependences of the ac magnetic susceptibility and the field dependences of the dc magnetizations are analyzed using the Heisenberg–Kitaev model describing the transition from the ordered spin state with classical isotropic AFM exchange to the frustrated spin state with quantum highly anisotropic FM exchange. A continuous transition from the 3D ferromagnetic state of manganese spins in the initial sample with y = 0 to zigzag AFM ordering of CE-type spins in ab planes for y = 0.5, coexisting in samples with y = 0.5, 0.6, and 0.7 at temperatures below T{sub N} ≅ 48.5 K with a disordered phase such as a quantum Griffiths phase is identified. As the gadolinium concentration further increases, the CE-type zigzag AFM structure is molten, which leads to the appearance of an unusual phase in Gd{sub 0.55}Sr{sub 0.45}MnO{sub 3} in the temperature range close to the absolute zero. This phase has characteristic features of a gapless Z{sub 2} quantum spin liquid in zero external magnetic field. The step changes in the magnetization isotherms measured at 4.2 K in the field range of ±75 kOe are explained by quantum phase transitions of the Z{sub 2} spin liquid to a phase with topological order in weak magnetic fields and a polarized phase in strong fields. The significant difference between critical fields and magnetization jumps in isotherms indicates the existence of hysteretic phenomena in quantum spin liquid magnetization–demagnetization processes caused by the difference between localization–delocalization of 2D vortex pairs induced by a magnetic field in a quantum spin liquid with disorder.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

First Results from BISTRO: A SCUBA-2 Polarimeter Survey of the Gould Belt

We present the first results from the B-fields In STar-forming Region Observations (BISTRO) survey, using the Sub-millimetre Common-User Bolometer Array 2 camera, with its associated polarimeter (POL-2), on the James Clerk Maxwell Telescope in Hawaii. We discuss the survey’s aims and objectives. We describe the rationale behind the survey, and the questions that the survey will aim to answer. The most important of these is the role of magnetic fields in the star formation process on the scale of individual filaments and cores in dense regions. We describe the data acquisition and reduction processes for POL-2, demonstrating both repeatability and consistency with previous data. We present a first-look analysis of the first results from the BISTRO survey in the OMC 1 region. We see that the magnetic field lies approximately perpendicular to the famous “integral filament” in the densest regions of that filament. Furthermore, we see an “hourglass” magnetic field morphology extending beyond the densest region of the integral filament into the less-dense surrounding material, and discuss possible causes for this. We also discuss the more complex morphology seen along the Orion Bar region. We examine the morphology of the field along the lower-density northeastern filament. We find consistency with previous theoretical models that predict magnetic fields lying parallel to low-density, non-self-gravitating filaments, and perpendicular to higher-density, self-gravitating filaments.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2023

Methane, ethane, and propane production in Greenland ice core samples and a first isotopic characterization of excess methane

Air trapped in polar ice provides unique records of the past atmospheric composition ranging from key greenhouse gases such as methane (CH 4 ) to short-lived trace gases like ethane (C 2 H 6 ) and propane (C 3 H 8 ). Recently, the comparison of CH 4 records obtained using different extraction methods revealed disagreements in the CH 4 concentration for the last glacial in Greenland ice. Elevated methane levels were detected in dust-rich ice core sections measured discretely, pointing to a process sensitive to the melt extraction technique. To shed light on the underlying mechanism, we performed targeted experiments and analyzed samples for methane and the short-chain alkanes ethane and propane covering the time interval from 12 to 42 kyr. Here, we report our findings of these elevated alkane concentrations, which scale linearly with the amount of mineral dust within the ice samples. The alkane production happens during the melt extraction step of the classic wet-extraction technique and reaches 14 to 91 ppb of CH 4 excess in dusty ice samples. We document for the first time a co-production of excess methane, ethane, and propane, with the observed concentrations for ethane and propane exceeding their past atmospheric background at least by a factor of 10. Independent of the produced amounts, excess alkanes were produced in a fixed molar ratio of approximately 14 : 2 : 1, indicating a shared origin. The measured carbon isotopic signature of excess methane is (-47.0 ± 2.9) ‰ and its deuterium isotopic signature is (-326 ± 57) ‰. With the co-production ratios of excess alkanes and the isotopic composition of excess methane we established a fingerprint that allows us to constrain potential formation processes. This fingerprint is not in line with a microbial origin. Moreover, an adsorption–desorption process of thermogenic gas on dust particles transported to Greenland does not appear very likely. Instead, the alkane pattern appears to be indicative of abiotic decomposition of organic matter as found in soils and plant leaves.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic

Abstract. Few measurements of aerosol chemical composition have been made during the winter–spring transition (following polar sunrise) to constrain Arctic aerosol–cloud–climate feedbacks. Herein, we report the first measurements of individual particle chemical composition near Utqiaġvik (Barrow), Alaska, in winter (seven sample days in January and February 2014). Individual particles were analyzed by computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM-EDX, 24 847 particles), Raman microspectroscopy (300 particles), and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS, 290 particles). Sea spray aerosol (SSA) was observed in all samples, with fresh and aged SSA comprising 99 %, by number, of 2.5–7.5 µm diameter particles, 65–95 % from 0.5–2.5 µm, and 50–60 % from 0.1–0.5 µm, indicating SSA is the dominant contributor to accumulation and coarse-mode aerosol during the winter. The aged SSA particles were characterized by reduced chlorine content with 94 %, by number, internally mixed with secondary sulfate (39 %, by number, internally mixed with both nitrate and sulfate), indicative of multiphase aging reactions during transport. There was a large number fraction (40 % of 1.0–4.0 µm diameter particles) of aged SSA during periods when particles were transported from near Prudhoe Bay, consistent with pollutant emissions from the oil fields participating in atmospheric processing of aerosol particles. Organic carbon and sulfate particles were observed in all samples and comprised 40–50 %, by number, of 0.1–0.4 µm diameter particles, indicative of Arctic haze influence. Soot was internally mixed with organic and sulfate components. All sulfate was mixed with organic carbon or SSA particles. Therefore, aerosol sources in the Alaskan Arctic and resulting aerosol chemical mixing states need to be considered when predicting aerosol climate effects, particularly cloud formation, in the winter Arctic.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Accelerated Climate Model for Energy (ACME): Ocean and Sea-Ice Processes

The primary goal of this project was to understand the role of the ocean and sea-ice components in the evolution of the climate in both a high-resolution fully-coupled 1850 preindustrial control and present day transient climate simulations run using the Energy Exascale Earth System Model (E3SM), formerly known as the Accelerated Climate Model for Energy (ACME). Two distinct approaches to the initialization of the present day transients were tested: in the first, an ensemble of three transients used atmospheric reanalysis forced 0.1-degree ocean/sea-ice states, while a fourth transient was branched off the preindustrial control. Biases from the control were inherited by its successor transient, in particular, sea surface temperatures (SSTs) at high latitudes were too warm and too much northward meridional heat transport occurred in the North Atlantic Ocean. SSTs in the Northern Hemisphere and Atlantic meridional heat transport increased in the transients initialized from the ocean/sea-ice simulation over a 40-50 year period to largely resemble the transient branched off the control simulation. Excessive absorbed solar radiation (ASR) is considered to be responsible for the SST biases as well as the formation of mode waters in lighter density classes than in reality both in the Southern Ocean and the North Atlantic Ocean subtropical gyre. These mode waters ventilate the thermocline waters to the north of their formation sites explaining the excessive Atlantic meridional heat transport and some of the warming in the high-latitude North Atlantic Ocean after multiple decades.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2015

Identification of the formation phases of filamentary damage induced by nanosecond laser pulses in bulk fused silica

Employing a pump-probe polarization-based two-frame shadowgraphy setup, the formation of filamentary damage induced in bulk fused silica by a nanosecond pulse at 1064 nm is investigated with a picosecond probe. Three different phases are exhibited in the damage experiments. The first phase is the formation of a micrometric plasma channel along the laser direction during the beginning of the pulse likely caused by multi-photon ionization. This channel exhibits growth during ∼400 ps, and the newly grown plasma is discrete. Then, during the end of the pulse, this channel evolves into a tadpole-like morphology showing an elliptical head upstream the laser flux followed by a thin tail. This observed asymmetry is attributed to shielding effects caused by both the plasma and hot modified silica. Once the damage shows its almost final morphology, a last phase consists in the launch of a pressure wave enlarging it after the laser pulse. The physical mechanisms that might be involved in the formation of plasma channels are discussed. The experimental data are first confronted to the moving breakdown model which overestimates the filamentary damage length. Finally, taking into account the temporal shape of the laser pulses, the coupling between Kerr-induced self-focusing and stimulated Brillouin scattering is discussed to interpret the observations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Corrosion resistance of ZrO{sub 2}–TiO{sub 2} nanocomposite multilayer thin films coated on carbon steel in hydrochloric acid solution

This work reports the achievement of preparing of x% zirconia (ZrO{sub 2})–titania (TiO{sub 2}) composite coatings with different ZrO{sub 2} percent on the carbon steel by dipping substrates in sol–gel solutions. The prepared coated samples were investigated by various surface techniques including X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and energy dispersive X-ray spectroscopy (EDAX). Open-circuit potential (OCP), potentiodynamic polarization, and electrochemical impedance spectroscopy (EIS) methods were employed to investigate the corrosion resistance of the coated carbon steel substrates in 1.0 M HCl solution at 50 °C. The data showed that, the corrosion protection property is not always proportional to the percent of ZrO{sub 2}. It can be inferred that there is an optimum percent (10%ZrO{sub 2}) for beneficial effects of loading ZrO{sub 2} on the protection efficiency (98.70%), while higher loading percent of ZrO{sub 2} in the sol–gel coating leads to the formation of a fragile film with poor barrier properties. EDAX/SEM suggests that the metal surface was protected through coating with ZrO{sub 2}–TiO{sub 2} composite films. - Highlights: • Sol–gel TiO{sub 2} doped with ZrO{sub 2} films deposited on carbon steel substrate • XRD measurements of x wt.% ZrO{sub 2}–TiO{sub 2} showed the (101) peaks broader than that of TiO{sub 2}. • SEM results proved that, the cracking decreases with the number of layers. • The prepared films can improve the corrosion resistance of the carbon steel substrate. • 10%ZrO{sub 2} loading is the optimal percent for useful effects on the corrosion resistance.

36 MATERIALS SCIENCE↗
NASA NTRSDate not supplied

Advanced Al Mirrors Protected with LiF Overcoat to Realize Stable Mirror Coatings for Astronomical Telescopes

Pure Aluminum (Al) exhibits intrinsic high reflectance over the proposed Large UV/Optical/IR (LUVOIR) Surveyor observatory target spectral range (90-2500 nm). However, Al coatings have to be protected from oxygen exposure in order to prevent the formation of the naturally occurring Al2O3 oxide layer, which limit performance for use only above 160 nm. Aluminum protected with fluorides such as LiF or MgF2 have been the most commonly used solutions. But below 102 nm and down to 90 nm, no transparent material is available to protect Al and coating mirror reflectance stays below 40%. But even above 102 nm, the reflectance of protected Al is limited by the residual absorption of the fluoride overcoats. Hence, this paper will report on recent advances in producing enhanced Al-based mirror coatings with the highest possible far-ultraviolet (FUV) reflectance, while exhibiting a more stable LiF protection layer. The process starts with a bare optically smooth glass substrate that is coated with Al in an ultra-high vacuum chamber by using the physical vapor deposition (PVD) process, which has been shown to provide the best aluminum thin-films when compared to other approaches. The next step is done by in-situ exposure of the freshly made Al film to a reactive XeF2 gas that will grant a thin AlF3 overcoat (2-3 nm) to the Al film that prevents further oxidation. This fluorinated Al film is then coated with a final layer of a LiF metal-fluoride overcoat. The coating process is finalized with a second exposure to the XeF2 precursor gas. The preparation of these mirror coatings will be studied and analyzed as a function of the XeF2 exposure time and deposition rate of the LiF layer during the PVD process. This paper will present and discuss characterization of a number of Al+XeLiF witness coupons produced with this reactive PVD (rPVD) process. These studies include characterization of specular reflectance in the 90-2500 nm spectral range, micro-roughness, long-term stability, as well as polarization characteristics in the visible and near-infrared spectral regions. These studies have been performed in order to demonstrate the improved reflectance performance, longer durability, and less hygroscopic nature of protected Al mirrors produced with the rPVD process (through exposure to XeF2) and in comparison with the standard PVD process.

optics↗
DOE OSTI2017

Cross-polar transport and scavenging of Siberian aerosols containing black carbon during the 2012 ACCESS summer campaign

During the ACCESS airborne campaign in July 2012, extensive boreal forest fires resulted in significant aerosol transport to the Arctic. A 10-day episode combining intense biomass burning over Siberia and low-pressure systems over the Arctic Ocean resulted in efficient transport of plumes containing black carbon (BC) towards the Arctic, mostly in the upper troposphere (6–8 km). Here, a combination of in situ observations (DLR Falcon aircraft), satellite analysis and WRF-Chem simulations is used to understand the vertical and horizontal transport mechanisms of BC with a focus on the role of wet removal. Between the northwestern Norwegian coast and the Svalbard archipelago, the Falcon aircraft sampled plumes with enhanced CO concentrations up to 200 ppbv and BC mixing ratios up to 25 ng kg –1 . During transport to the Arctic region, a large fraction of BC particles are scavenged by two wet deposition processes, namely wet removal by large-scale precipitation and removal in wet convective updrafts, with both processes contributing almost equally to the total accumulated deposition of BC. Our results underline that applying a finer horizontal resolution (40 instead of 100 km) improves the model performance, as it significantly reduces the overestimation of BC levels observed at a coarser resolution in the mid-troposphere. According to the simulations at 40 km, the transport efficiency of BC (TE BC ) in biomass burning plumes was larger (60 %), because it was impacted by small accumulated precipitation along trajectory (1 mm). In contrast TE BC was small (< 30 %) and accumulated precipitation amounts were larger (5–10 mm) in plumes influenced by urban anthropogenic sources and flaring activities in northern Russia, resulting in transport to lower altitudes. TE BC due to large-scale precipitation is responsible for a sharp meridional gradient in the distribution of BC concentrations. Wet removal in cumulus clouds is the cause of modeled vertical gradient of TE BC , especially in the mid-latitudes, reflecting the distribution of convective precipitation, but is dominated in the Arctic region by the large-scale wet removal associated with the formation of stratocumulus clouds in the planetary boundary layer (PBL) that produce frequent drizzle.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2007

Spaceborne Autonomous and Ground Based Relative Orbit Control for the TerraSAR-X/TanDEM-X Formation

TerraSAR-X (TSX) and TanDEM-X (TDX) are two advanced synthetic aperture radar (SAR) satellites flying in formation. SAR interferometry allows a high resolution imaging of the Earth by processing SAR images obtained from two slightly different orbits. TSX operates as a repeat-pass interferometer in the first phase of its lifetime and will be supplemented after two years by TDX in order to produce digital elevation models (DEM) with unprecedented accuracy. Such a flying formation makes indeed possible a simultaneous interferometric data acquisition characterized by highly flexible baselines with range of variations between a few hundreds meters and several kilometers [1]. TSX has been successfully launched on the 15th of June, 2007. TDX is expected to be launched on the 31st of May, 2009. A safe and robust maintenance of the formation is based on the concept of relative eccentricity/inclination (e/i) vector separation whose efficiency has already been demonstrated during the Gravity Recovery and Climate Experiment (GRACE) [2]. Here, the satellite relative motion is parameterized by mean of relative orbit elements and the key idea is to align the relative eccentricity and inclination vectors to minimize the hazard of a collision. Previous studies have already shown the pertinence of this concept and have described the way of controlling the formation using an impulsive deterministic control law [3]. Despite the completely different relative orbit control requirements, the same approach can be applied to the TSX/TDX formation. The task of TDX is to maintain the close formation configuration by actively controlling its relative motion with respect to TSX, the leader of the formation. TDX must replicate the absolute orbit keeping maneuvers executed by TSX and also compensate the natural deviation of the relative e/i vectors. In fact the relative orbital elements of the formation tend to drift because of the secular non-keplerian perturbations acting on both satellites. The goal of the ground segment is thus to regularly correct this configuration by performing small orbit correction maneuvers on TDX. The ground station contacts are limited due to the geographic position of the station and the costs for contact time. Only with a polar ground station a contact visibility is possible every orbit for LEO satellites. TSX and TDX use only the Weilheim ground station (in the southern part of Germany) during routine operations. This station allows two scheduled contact per day for the nominal orbit configuration, meaning that the satellite conditions can be checked with an interval of 12 hours. While this limitation is usually not critical for single satellite operations, the visibility constraints drive the achievable orbit control accuracy for a LEO formation if a ground based approach is chosen. Along-track position uncertainties and maneuver execution errors affect the relative motion and can be compensated only after a ground station contact.

Ardaens, J. S.↗
DOE OSTI2022

Highly supercooled riming and unusual triple-frequency radar signatures over McMurdo Station, Antarctica

Abstract. Riming of ice crystals by supercooled water droplets is an efficient ice growth process, but its basic properties are still poorly known. While it has been shown to contribute significantly to surface precipitation at mid-latitudes, little is known about its occurrence at high latitudes. In Antarctica, two competing effects can influence the occurrence of riming: (i) the scarcity of supercooled liquid water clouds due to the extremely low tropospheric temperatures and (ii) the low aerosol concentration, which may lead to the formation of fewer and larger supercooled drops potentially resulting in an enhanced riming efficiency. In this work, by exploiting the deployment of an unprecedented number of multiwavelength remote sensing systems (including triple-frequency radar measurements) in West Antarctica, during the Atmospheric Radiation Measurements West Antarctic Radiation Experiment (AWARE) field campaign, we evaluate the riming incidence at McMurdo Station and find that riming occurs at much lower temperatures when compared to previous results in the mid-latitudes. This suggests the possible occurrence of a common atmospheric state over Antarctica that includes a rather stable atmosphere inhibiting turbulent mixing, and a high riming efficiency driven by large cloud droplets. We then focus on a peculiar case study featuring a persistent layer with a particularly pronounced riming signature in triple-frequency radar data but only a relatively modest amount of supercooled liquid water. In-depth analysis of the radar observations suggests that such signatures can only be explained by the combined effects of moderately rimed aggregates or similarly shaped florid polycrystals and a narrow particle size distribution (PSD). Simulations of this case study performed with a one-dimensional bin model indicate that similar triple-frequency radar observations can be reproduced when narrow PSDs are simulated. Such narrow PSDs can in turn be explained by two key factors: (i) the presence of a shallow homogeneous droplet or humidified aerosol freezing layer aloft seeding an underlying supercooled liquid layer, and (ii) the absence of turbulent mixing throughout a stable polar atmosphere that sustains narrow PSDs, as hydrometeors grow from the nucleation region aloft to ice particles of several millimeters in size, by vapor deposition and then riming.

54 ENVIRONMENTAL SCIENCES↗