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At least 595 records · Page 33

Structural tuning of nanogaps using electromigration induced by field emission current with bipolar biasing

We report a new method for fabrication of Ni nanogaps based on electromigration induced by a field emission current. This method is called “activation” and is demonstrated here using a current source with alternately reversing polarities. The activation procedure with alternating current bias, in which the current source polarity alternates between positive and negative bias conditions, is performed with planar Ni nanogaps defined on SiO{sub 2}/Si substrates at room temperature. During negative biasing, a Fowler-Nordheim field emission current flows from the source (cathode) to the drain (anode) electrode. The Ni atoms at the tip of the drain electrode are thus activated and then migrate across the gap from the drain to the source electrode. In contrast, in the positive bias case, the field emission current moves the activated atoms from the source to the drain electrode. These two procedures are repeated until the tunnel resistance of the nanogaps is successively reduced from 100 TΩ to 48 kΩ. Scanning electron microscopy and atomic force microscopy studies showed that the gap separation narrowed from approximately 95 nm to less than 10 nm because of the Ni atoms that accumulated at the tips of both the source and drain electrodes. These results show that the alternately biased activation process, which is a newly proposed atom transfer technique, can successfully control the tunnel resistance of the Ni nanogaps and is a suitable method for formation of ultrasmall nanogap structures.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Spin-Controllable Dynamics in Defect-Engineered Carbon Nanotubes as Single Photon Emitters: Data-Driven Modeling and Computations

Quantum technologies, such as quantum computing and sensing, require efficient single-photon emission (SPE) sources that operate at room temperature in telecom wavelengths. While several materials can serve as SPE sources, no single platform meets all the criteria for efficiency, ambient operation, and scalability. Single-walled carbon nanotubes (SWCNTs) with covalently attached molecules offer a promising solution. Their SPE can be easily tuned via modifications of the SWCNT's diameter, chirality, and bonded molecules, enabling emission across near-IR to telecom wavelengths at ambient conditions. However, to fully realize the potential of SWCNTs and unlock their quantum capabilities, a deeper understanding of how structural defects from molecular adducts affect their emission and competing photoexcited processes is essential. To address this gap in our knowledge, this project combined quantum chemistry calculations with data-driven methods of cheminformatics (QSAR) and machine learning (ML). The developed computational approaches have provided several design strategies for covalent functionalization of SWCNTs to improve their optical response. The collaboration with Los Alamos National Lab (LANL) enabled direct comparison of computational and experimental data, facilitating method validation. This partnership was enhanced through access to LANL's Center for Integrated Nanotechnologies (CINT) utilizing User Facility Program and summer internships, which provided three NDSU graduate students with hands-on experience at LANL. The outcomes of this project included (1) Advancing the current stage of computational methods in accurate modeling of non-adiabatic spin-dependent photoexcited dynamics and its applicability to nanosystems consisting of thousands of atoms, realized as open-access codes linked to existing DFT-based software; (2) Establishing the relationship between the structure of adducts and SWCNTs and intrinsic excitonic and spin properties of defect states for guiding novel synthetic strategies and experimental probes of chemically functionalized SWCNTs as near-IR emitting materials; (3) Generating virtual libraries of hypothetical functionalized SWCNTs for virtual screening of their chemical structures and optical properties, leveraging new functionalities of SWCNTs; (4) Offering a unique experience for NDSU graduate students that prepared them for future scientific careers related to materials modeling and big data processing. These results were summarized in 12 published journal papers and 3 recently submitted papers. One of a key finding is that the position of defect sites on the SWCNT surface primarily drives the emission redshift (up to 100 meV), while the polarity of the defect-inducing molecules has a much smaller effect (~10 meV). However, the electron-donating or withdrawing properties of a molecule influence selecting reactivity of defect sites. These insights important for optimizing synthetic protocols for desired emissions in SWCNTs. We also revealed that the interaction between two defects at various positions on the SWCNT enhances the redshift and optical activity of states, favoring strong near-IR emission. This suggests that manipulations in defect concentrations is a promising strategy for controlling efficient emission. Mostly important, the defect position was found controllable by the spin states of photoexcited intermediates: Excited aromatic molecules form ortho defects with SWCNTs at their singlet states in the presence of oxygen, while oxygen-free conditions favor para defects via the triplet-state mechanism. Additionally, a heat-activated [2+2] cycloaddition reaction facilitates divalent defect formation with fewer bonding positions that narrows emission bands. These groundbreaking findings have been experimentally validated and significantly advance our understanding of defect chemistry in SWCNTs. Using a novel encoding technique and 3D-MoRSE descriptors, we developed highly accurate ML/QSAR models to predict both the 3D structure and optical properties of SWCNTs with chemical defects. This model enabled the creation of a virtual library of 125,556 structures, providing new insights into the relationship between SWCNT-defect structure and emission.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Imprint of the Sun’s Evolving Polar Winds on IBEX Energetic Neutral Atom All-sky Observations of the Heliosphere

With 7 years of Interstellar Boundary Explorer ( IBEX ) measurements of energetic neutral atoms (ENAs), IBEX has shown a clear correlation between dynamic changes in the solar wind and the heliosphere’s response in the formation of ENAs. In this paper, we investigate temporal variations in the latitudinal-dependent ENA spectrum from IBEX and their relationship to the solar wind speed observed at 1 au. We find that the variation in latitude of the transition in ENA spectral indices between low (≲1.8) and high (≳1.8) values, as well as the distribution of ENA spectral indices at high and low latitudes, correlates well with the evolution of the fast and slow solar wind latitudinal structure observed near 1 au. This correlation includes a delay due to the time it takes the solar wind to propagate to the termination shock and into the inner heliosheath, and for ENAs to be generated via charge-exchange and travel back toward 1 au. Moreover, we observe a temporal asymmetry in the steepening of the ENA spectrum in the northern and southern hemispheres, consistent with asymmetries observed in the solar wind and polar coronal holes. While this asymmetry is observed near the upwind direction of the heliosphere, it is not yet observed in the tail direction, suggesting a longer line-of-sight integration distance or different processing of the solar wind plasma downstream of the termination shock.

79 ASTRONOMY AND ASTROPHYSICS↗

Imprint of the Sun’s Evolving Polar Winds on IBEX Energetic Neutral Atom All-sky Observations of the Heliosphere

With 7 years of Interstellar Boundary Explorer (IBEX) measurements of energetic neutral atoms (ENAs), IBEX has shown a clear correlation between dynamic changes in the solar wind and the heliosphere’s response in the formation of ENAs. In this paper, we investigate temporal variations in the latitudinal-dependent ENA spectrum from IBEX and their relationship to the solar wind speed observed at 1 au. We find that the variation in latitude of the transition in ENA spectral indices between low (≲1.8) and high (≳1.8) values, as well as the distribution of ENA spectral indices at high and low latitudes, correlates well with the evolution of the fast and slow solar wind latitudinal structure observed near 1 au. This correlation includes a delay due to the time it takes the solar wind to propagate to the termination shock and into the inner heliosheath, and for ENAs to be generated via charge-exchange and travel back toward 1 au. Moreover, we observe a temporal asymmetry in the steepening of the ENA spectrum in the northern and southern hemispheres, consistent with asymmetries observed in the solar wind and polar coronal holes. While this asymmetry is observed near the upwind direction of the heliosphere, it is not yet observed in the tail direction, suggesting a longer line-of-sight integration distance or different processing of the solar wind plasma downstream of the termination shock.

Local interstellar matter↗

NASA Tech Briefs, September 2006

Topics covered include: Improving Thermomechanical Properties of SiC/SiC Composites; Aerogel/Particle Composites for Thermoelectric Devices; Patches for Repairing Ceramics and Ceramic- Matrix Composites; Lower-Conductivity Ceramic Materials for Thermal-Barrier Coatings; An Alternative for Emergency Preemption of Traffic Lights; Vehicle Transponder for Preemption of Traffic Lights; Automated Announcements of Approaching Emergency Vehicles; Intersection Monitor for Traffic-Light-Preemption System; Full-Duplex Digital Communication on a Single Laser Beam; Stabilizing Microwave Frequency of a Photonic Oscillator; Microwave Oscillators Based on Nonlinear WGM Resonators; Pointing Reference Scheme for Free-Space Optical Communications Systems; High-Level Performance Modeling of SAR Systems; Spectral Analysis Tool 6.2 for Windows; Multi-Platform Avionics Simulator; Silicon-Based Optical Modulator with Ferroelectric Layer; Multiplexing Transducers Based on Tunnel-Diode Oscillators; Scheduling with Automated Resolution of Conflicts; Symbolic Constraint Maintenance Grid; Discerning Trends in Performance Across Multiple Events; Magnetic Field Solver; Computing for Aiming a Spaceborne Bistatic- Radar Transmitter; 4-Vinyl-1,3-Dioxolane-2-One as an Additive for Li-Ion Cells; Probabilistic Prediction of Lifetimes of Ceramic Parts; STRANAL-PMC Version 2.0; Micromechanics and Piezo Enhancements of HyperSizer; Single-Phase Rare-Earth Oxide/Aluminum Oxide Glasses; Tilt/Tip/Piston Manipulator with Base-Mounted Actuators; Measurement of Model Noise in a Hard-Wall Wind Tunnel; Loci-STREAM Version 0.9; The Synergistic Engineering Environment; Reconfigurable Software for Controlling Formation Flying; More About the Tetrahedral Unstructured Software System; Computing Flows Using Chimera and Unstructured Grids; Avoiding Obstructions in Aiming a High-Gain Antenna; Analyzing Aeroelastic Stability of a Tilt-Rotor Aircraft; Tracking Positions and Attitudes of Mars Rovers; Stochastic Evolutionary Algorithms for Planning Robot Paths; Compressible Flow Toolbox; Rapid Aeroelastic Analysis of Blade Flutter in Turbomachines; General Flow-Solver Code for Turbomachinery Applications; Code for Multiblock CFD and Heat-Transfer Computations; Rotating-Pump Design Code; Covering a Crucible with Metal Containing Channels; Repairing Fractured Bones by Use of Bioabsorbable Composites; Kalman Filter for Calibrating a Telescope Focal Plane; Electronic Absolute Cartesian Autocollimator; Fiber-Optic Gratings for Lidar Measurements of Water Vapor; Simulating Responses of Gravitational-Wave Instrumentation; SOFTC: A Software Correlator for VLBI; Progress in Computational Simulation of Earthquakes; Database of Properties of Meteors; Computing Spacecraft Solar-Cell Damage by Charged Particles; Thermal Model of a Current-Carrying Wire in a Vacuum; Program for Analyzing Flows in a Complex Network; Program Predicts Performance of Optical Parametric Oscillators; Processing TES Level-1B Data; Automated Camera Calibration; Tracking the Martian CO2 Polar Ice Caps in Infrared Images; Processing TES Level-2 Data; SmaggIce Version 1.8; Solving the Swath Segment Selection Problem; The Spatial Standard Observer; Less-Complex Method of Classifying MPSK; Improvement in Recursive Hierarchical Segmentation of Data; Using Heaps in Recursive Hierarchical Segmentation of Data; Tool for Statistical Analysis and Display of Landing Sites; Automated Assignment of Proposals to Reviewers; Array-Pattern-Match Compiler for Opportunistic Data Analysis; Pre-Processor for Compression of Multispectral Image Data; Compressing Image Data While Limiting the Effects of Data Losses; Flight Operations Analysis Tool; Improvement in Visual Target Tracking for a Mobile Robot; Software for Simulating Air Traffic; Automated Vectorization of Decision-Based Algorithms; Grayscale Optical Correlator Workbench; "One-Stop Shopping" for Ocean Remote-Sensing and Model Data; State Analysis Database Tool; Generating CAHV and CAHVOmages with Shadows in ROAMS; Improving UDP/IP Transmission Without Increasing Congestion; FORTRAN Versions of Reformulated HFGMC Codes; Program for Editing Spacecraft Command Sequences; Flight-Tested Prototype of BEAM Software; Mission Scenario Development Workbench; Marsviewer; Tool for Analysis and Reduction of Scientific Data; ASPEN Version 3.0; Secure Display of Space-Exploration Images; Digital Front End for Wide-Band VLBI Science Receiver; Multifunctional Tanks for Spacecraft; Lightweight, Segmented, Mostly Silicon Telescope Mirror; Assistant for Analyzing Tropical-Rain-Mapping Radar Data; and Anion-Intercalating Cathodes for High-Energy- Density Cells.

Source record↗

Description, Usage, and Validation of the MVL-15 Modified Vortex Lattice Analysis Capability

MVL-15 is the most recent version of the Modified Vortex-Lattice (MVL) code developed within the Aerodynamics Systems Analysis Branch (ASAB) at NASA LaRC. The term "modified" refers to the primary modification of the core vortex-lattice methodology: inclusion of viscous aerodynamics tables that are linked to the linear solution via iterative processes. The inclusion of the viscous aerodynamics inherently converts the MVL-15 from a purely analytic linearized method to a semi-empirical blend which retains the rapid execution speed of the linearized method while empirically characterizing the section aerodynamics at all spanwise lattice points. The modification provides a means to assess non-linear effects on lift that occur at angles of attack near stall, and provides a means to determine the drag associated with the application of design strategies for lift augmentation such as the use of flaps or blowing. The MVL-15 code is applicable to the analyses of aircraft aerodynamics during cruise, but it is most advantageously applied to the analysis of aircraft operating in various high-lift configurations. The MVL methodology has been previously conceived and implemented; the initial concept version was delivered to the ASAB in 2001 (van Dam, C.), subsequently revised (Gelhausen, P. and Ozoroski, T. 2002 / AVID Inc., Gelhausen, P., and Roberts, M. 2004), and then overhauled (Ozoroski, T., Hahn, A. 2008). The latest version, MVL-15 has been refined to provide analysis transparency and enhanced to meet the analysis requirements of the Environmentally Responsible Aviation (ERA) Project. Each revision has been implemented with reasonable success. Separate applications of the methodology are in use, including a similar in-house capability, developed by Olson, E. that is tailored for structural and acoustics analyses. A central premise of the methodology is that viscous aerodynamic data can be associated with analytic inviscid aerodynamic results at each spanwise wing section, thereby providing a pathway to map viscous data to the inviscid results. However, a number of factors can sidetrack the analysis consistency during various stages of this process. For example, it should be expected that the final airplane lift curve and drag polar results depend strongly on the geometry and aerodynamics of the airfoil section; however, flap deflections and flap chord extensions change the local reference geometry of the input airfoil, the airplane wing, the tabulated non-dimensional viscous aerodynamics, and the spanwise links between the linear and the viscous aerodynamics. These changes also affect the bound circulation and therefore, calculation and integration of the induced angle of attack and induced drag. MVL-15 is configured to ensure these types of challenges are properly addressed. This report is a comprehensive manual describing the theory, use, and validation of the MVL-15 analysis tool. Section 3 summarizes theoretical, procedural, and characteristic features of MVL-15, and includes a list of the files required to setup, execute, and summarize an analysis. Section 4, Section 5, Section 6, and Section 7 combine to comprise the User's Guide portions of this report. The MVL-15 input and output files are described in Section 4 and Section 5, respectively; the descriptions are supplemented with example files and information about the file formats, parameter definitions, and typical parameter values. Section 6 describes the Wing Geometry Setup Utility and the 2d-Variants Utility files that simplify and assist setting up a consistent set of MVL-15 geometry and aerodynamics input parameters and input files. Section 7 describes the use of the 3d-Results Presentation Utility file that can be used to automatically create summary tables and charts from the MVL-15 output files. Section 8 documents the Validation Results of an extensive and varied validation test matrix, including results of an airplane analysis representative of the ERA Program. A start-to-finish example of the airplane analysis procedure is described in Section 7.

Ozoroski, Thomas A.↗

Thin Sea-Ice Thickness as Inferred from Passive Microwave and In Situ Observations

Since microwave radiometric signals from sea-ice strongly reflect physical conditions of a layer near the ice surface, a relationship of brightness temperature with thickness is possible especially during the early stages of ice growth. Sea ice is most saline during formation stage and as the salinity decreases with time while at the same time the thickness of the sea ice increases, a corresponding change in the dielectric properties and hence the brightness temperature may occur. This study examines the extent to which the relationships of thickness with brightness temperature (and with emissivity) hold for thin sea-ice, approximately less than 0.2 -0.3 m, using near concurrent measurements of sea-ice thickness in the Sea of Okhotsk from a ship and passive microwave brightness temperature data from an over-flying aircraft. The results show that the brightness temperature and emissivity increase with ice thickness for the frequency range of 10-37 GHz. The relationship is more pronounced at lower frequencies and at the horizontal polarization. We also established an empirical relationship between ice thickness and salinity in the layer near the ice surface from a field experiment, which qualitatively support the idea that changes in the near-surface brine characteristics contribute to the observed thickness-brightness temperature/emissivity relationship. Our results suggest that for thin ice, passive microwave radiometric signals contain, ice thickness information which can be utilized in polar process studies.

Naoki, Kazuhiro↗

Over 50% reduction in the formation energy of Co-based Heusler alloy films by two-dimensional crystallisation

Crystalline formation of high magnetic-moment thin films through low-temperature annealing processes compatible with current semiconductor technologies is crucial for the development of next generation devices, which can utilise the spin degree of freedom. Utilising in-situ aberration corrected electron microscopy, we report a 235 °C crystallisation process for a Co-based ternary Heusler-alloy film whose initial nucleation is initiated by as few as 27 unit cells. The crystallisation occurs preferentially in the 〈111〉 crystalline directions via a two-dimensional (2D) layer-by-layer growth mode; resulting in grains with [110] surface normal and [111] plane facets. This growth process was found to reduce the crystallisation energy by more than 50% when compared to bulk samples whilst still leading to the growth of highly ordered grains expected to give a high degree of spin-polarisation. Our findings suggest that the 2D layer-by-layer growth minimises the crystallisation energy allowing for the possible implementation of highly spin-polarised alloy films into current chip and memory technologies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A Visual Understanding of Circular Dichroism Spectroscopy

Mapping chemical and structural properties to electronic and magnetic responses is critical to many applications such as quantum information science, where the precise storage and transmission of unique information is paramount. Specifically, constructing molecules and materials that provide strong polarized responses at tunable frequencies and with large anisotropies is key to optical processing of quantum information. Chiral molecules provide chiroptical response to circularly polarized light, making them attractive for quantum information science and other applications related to sensing, polarized photodetectors, and spintronics. Predicting a molecular design, a priori, with large anisotropies to circularly polarized light is challenging due to the complex interplay between electric and magnetic components of the optical response. In this work, we explore a visual representation of the electronic chiroptical response by decomposing the rotary strength into its constituent components. Here, we make use of the intuitive electronic oscillator framework to develop classical intuition regarding the rotary strength and its constituents. We explore three model chemical systems that exhibit local and global chirality. Our analysis reveals that local chirality necessarily exhibits competition between the local chiral center and chirality induced in other fragments of the molecule, resulting in both unexpected nonmonotonic trends and sign flips in chemically adjacent geometries. Furthermore, we can visually distinguish between local and global chirality via examination of the transition chiral tensor. Interestingly, we make strong connections to ferromagnetic and antiferromagnetic spin systems in that chiroptically inactive transitions exhibit antiferromagnetic-like alternating orbital patterns while active transitions show domain formation in an ferromagnetic-like alignment that produces a net chiroptical response.

36 MATERIALS SCIENCE↗

ARM: KASACRCFRQC

The Ka-Band Scanning ARM Cloud Radar (KASACR) records cloud properties. ARM's scanning cloud radars are dual-frequency, dual-polarization Doppler radars mounted on a common scanning pedestal. Each pedestal includes a Ka-band radar (2kW peak power) and the deployment location determines whether the second radar is a W-band (1.7 kW peak power) or an X-band (20 kW peak power). Beamwidths for Ka-bands paired with W-bands are roughly matched at 0.3 degrees. The X-band beamwidth is approximately 1 degree. Due to the narrow antenna beamwidth, ARM’s scanning cloud radars use scanning strategies unlike typical weather radars. Rather than focusing on plan position indicator, or PPI, scans, the KASACR uses range height indicator, or RHI, scans at numerous azimuths to obtain cloud volume data. Measurements collected with the KASACR are copolar and cross-polar radar reflectivity, Doppler velocity, spectra width and spectra when not scanning, and linear depolarization ratio. KASACR data from the 2018–2019 Cloud, Aerosol, and Complex Terrain Interactions (CACTI) field campaign in Argentina are now available as b1-level products. Building on the original CACTI operational data, the b1-level products feature improved data quality resulting from extensive analyses and corrections. The data are cross-calibrated to a common point, datastreams are corrected for operational issues that occurred during the campaign, and several data quality masks and basic derived products are incorporated. For more information, read the CACTI radar b1-level processing report.

54 ENVIRONMENTAL SCIENCES↗

Relaxation behavior in low-frequency complex conductivity of sands caused by bacterial growth and biofilm formation by Shewanella oneidensis under a high-salinity condition

Complex electrical conductivity is increasingly used to monitor subsurface processes associated with microbial activities because microbial cells mostly have surface charges and thus electrical double layers. Although highly saline environments are frequently encountered in coastal and marine sediments, there are limited data available on the complex conductivity associated with microbial activities under a high-salinity condition. Therefore, we have developed the spectral responses of complex conductivity of sand associated with bacterial growth and biofilm formation under a highly saline condition of approximately 1% salinity and approximately 2 S/m pore water conductivity with an emphasis on relaxation behavior. A column test is performed, in which the model bacteria Shewanella oneidensis MR-1 are stimulated for cell growth and biofilm formation in a sand pack, whereas the complex conductivity is monitored from 0.01 Hz to 10 kHz. The test results indicate that the real conductivity increases in the early stage due to the microbial metabolites and the increased surface conduction with cell growth but soon begin to decrease because of the reduction of charge passages due to bioclogging. However, the imaginary conductivity significantly increases with time, and clear bell-shaped relaxation behaviors are observed with the peak frequency of 0.1–1 Hz, associated with the double-layer polarization of cells and electrically conductive pili and biofilms. The Cole-Cole relaxation model appears to capture such relaxation behaviors well, and the modeling results indicate gradual increases in normalized chargeability and decreases in relaxation time during bacterial growth and biofilm formation in the highly saline condition. Comparison with previous literature confirms that the high-salinity condition further increases the normalized chargeability, whereas it suppresses the phase shift and thus the imaginary conductivity. Our results suggest that the complex conductivity can effectively capture microbial biomass formation in sands under a highly saline condition.

58 GEOSCIENCES↗

Optical Measurements and Modeling to Estimate Concentrations and Fluxes of Organic Matter in the Southern Ocean

This project was a collaboration between two Principal Investigators, Dr. Dariusz Stramski and Dr. Greg Mitchell of Scripps Institution of Oceanography, University of California San Diego. Our overall goal was to conduct optical measurements and modeling to estimate concentrations of organic matter in the Southern Ocean in support of the U.S. JGOFS Process Study in this region. Key variables and processes of high relevance to accomplish the JGOFS goals include time and space resolution of phytoplankton pigments, particulate organic carbon, and the formation and export of organic carbon. Our project focused on establishing the fundamental relationships for parameterization of these variables and processes in terms of the optical properties of seawater, and developing understanding of why the Southern Ocean differs from other low-latitude systems, or has differentiation within. Our approach builds upon historical observations that optical properties provide a useful proxy for key reservoirs of organic matter such as chlorophyll alpha (Chl) and particulate organic carbon (POC) concentrations, which are of relevance to the JGOFS objectives. We carried out detailed studies of in situ and water sample optical properties including spectral reflectance, absorption, beam attenuation, scattering, and backscattering coefficients. We evaluated the ability to estimate Chl from the spectral reflectance (ocean color) in the Southern Ocean. We examined relationships between the ocean optical properties and particulate organic carbon. We developed, for the first time, an algorithm for estimating particulate organic carbon concentration in the surface ocean from satellite imagery of ocean color. With this algorithm, we obtained maps of POC distribution in the Southern Ocean showing the seasonal progression of POC in the austral spring-summer season. We also developed a semianalytical reflectance model for the investigated polar waters based on our field measurements of absorption and backscattering coefficients and Chl-dependent parameterizations of these coefficients. With this model, libraries of expected reflectance spectra for various chlorophyll concentrations can be generated with high spectral resolution for specific oceanic regions. In addition, our semianalytical reflectance model provided insight into the mechanisms which drive the empirical relationships between the ocean color and chlorophyll concentration. Our optical approach to the study of pigment and carbon concentrations will be directly relevant to development of system models and long-term monitoring of the Southern Ocean.

Stramski, Dariusz↗

Cooperative H 2 Activation across a Metal–Metal Multiple Bond and Hydrogenation Reactions Catalyzed by a Zr/Co Heterobimetallic Complex

In the quest for active and selective catalysts featuring nonprecious metals, bimetallic cooperativity poses a unique opportunity to promote catalytic reactions and influence selectivity. While examples of stoichiometric H 2 activation across metal–metal bonds have been reported, there have been limited advances toward the incorporation of a well-defined cooperative bimetallic H 2 activation process into a catalytic cycle for the hydrogenation of unsaturated hydrocarbons. We demonstrate that facile activation of H 2 by two nonprecious metals is facilitated by metal–metal cooperativity in the coordinatively unsaturated Zr/Co bis(phosphinoamide) complexes (THF)(I)Zr(XylNP i Pr 2 ) 2 CoPR 3 (3-PMe 3 and 3-PMePh 2 , Xyl =3,5-dimethylphenyl), which feature highly polar Zr–Co triple bonds. Owing to the stabilizing nature of the metal–metal bond, the H 2 activation products (THF)(I)Zr(μ-H)(XylNP i Pr 2 ) 2 Co(H)(PR 3 ) (4-PMe 3 and 4-PMePh 2 ), which feature one terminally bound Co hydride and one hydride bridging the two metals, have been isolated and crystallographically characterized. The Zr/Co bimetallic complex 3-PMePh 2 is an active catalyst for the hydrogenation of alkenes and semihydrogenation of alkynes, and relevant intermediates including 4-PMePh 2 and alkene (5) and alkyne (6) adducts have been identified spectroscopically in situ and isolated and characterized through independent synthesis. The alkyne semihydrogenation reaction catalyzed by 3-PMePh 2 exhibits high selectivity for alkene over alkane products and generates an unselective distribution of (E)- and (Z)-alkenes via direct formation of both stereoisomers. These findings lend insight into the roles that metal–metal bonding and cooperativity play in the activation of small molecules and the promotion and selectivity of subsequent catalytic transformations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Soil developments in polar deserts: Implications for exobiology and future Mars missions

Chemical alterations, weathering, and diagenesis of soil profiles from the dry valleys of Antarctica were studied as analogs of regolith development for the Martian regolith. Chemical weathering processes play an important part in soil development within the dry valleys of Antarctica. A suite of core samples were studied which were taken within the valley floors in addition to samples taken in the vicinity of evaporite and brine ponds. Analysis of water soluable cations and anions from core samples were performed along with petrographic analysis of selected samples. It was shown that ionic transport processes operate primarily above the permafrost zone. Abundances of the water soluable ions reflect the nature of secondary minerals produced by evaporation and weathering. Chloride, calcium, and sodium abundances for soils from the cores within the North and South Forks of Wright Valley, reflect the secondary mineralogy of the soil columns. Calculations for Na, Ca, and Cl abundances reflect the appearance of halite and antarcticite. In areas where excess Ca is present, X-ray diffraction studies show the presence of gypsum. It is well known that the Martian surface conditions may be favorable for chemical weathering. Primary silicates would be expected to be reactive with any ground water. It seems likely that Martian subsurface water is available to assist in the weathering of the primary minerals. Such weathering could result in the formation of clays, sulfates, carbonates, hydrates, halides, and zeolites. The dry valley cores have shown that they maybe excellent analogs to weathering processes on the near-surface of Mars. Since movement of water within the near-surface region clearly results in chemical weathering, leaching, and salt formation in the dry valleys, similar processes are probably operating within the Martian regolith.

Gibson, Everett K., Jr.↗

Lunar and Planetary Science XXXVI, Part 19

The topics include: 1) The abundances of Iron-60 in Pyroxene Chondrules from Unequilibrated Ordinary Chondrites; 2) LL-Ordinary Chondrite Impact on the Moon: Results from the 3.9 Ga Impact Melt at the Landing Site of Appolo 17; 3) Evaluation of Chemical Methods for Projectile Identification in Terrestrial and Lunar Impactites; 4) Impact Cratering Experiments in Microgravity Environment; 5) New Achondrites with High-Calcium Pyroxene and Its implication for Igneous Differentiation of Asteroids; 6) Climate History of the Polar Regions of Mars Deduced form Geologic Mapping Results; 7) The crater Production Function for Mars: A-2 Cumulative Power-Law Slope for Pristine Craters Greater than 5 km in Diameter Based on Crater Distribution for Northern Plains Materials; 8) High Resolution Al-26 Chronology: Resolved Time Interval Between Rim and Interior of a Highly Fractionated Compact Type a CAI from Efremovka; 9) Assessing Aqueous Alteration on Mars Using Global Distributions of K and Th; 10) FeNi Metal Grains in LaPaz Mare Basalt Meteorites and Appolo 12 Basalts; 11) Unique Properties of Lunar Soil for In Situ Resource Utilization on the Moon; 12) U-Pb Systematics of Phosphates in Nakhlites; 13) Measurements of Sound Speed in Granular Materials Simulated Regolith; 14) The Effects of Oxygen, Sulphur and Silicon on the Dihedral Angles Between Fe-rich Liquid Metal and Olivine, Ringwoodite and Silicate Perovskite: Implications for Planetary Core Formation; 15) Seismic Shaking Removal of Craters 0.2-0.5 km in Diameter on Asteroid 433 Eros; 16) Focused Ion Beam Microscoopy of ALH84001 Carbonate Disks; 17) Simulating Micro-Gravity in the Laboratory; 18) Mars Atmospheric Sample Return Instrument Development; 19) Combined Remote LIBS and Raman Spectroscopy Measurements; 20) Unusual Radar Backscatter Properties Along the Northern Rim of Imbrium Basin; 21) The Mars Express/NASAS Project at JPL; 22) The Geology of the Viking 2 Lander Site Revisited; 23) An Impact Genesis for Loki Patera? 24) Mars Polar Cap Edges Tracked over 3 Full Mars Years; 25) Elemental Abundance in Presolar SiC: Comparing Grains Separated by Acid Residue and Gently Separation Procedures; 26) First Results from the Descent Imager/Spectral Radiometer (DISR) Experiment on the Huygens Entry Probe of Titan; 27) Minor Element Behavior of Pallasite Olivine: Understanding Pallasite Thermal History and Chronology; 28) Canonical Anorthite in a Grosnaja Forsterite-bearing CAI; 29) Experimental Evidence for Condensation of 'Astrophysical' Carbonate; 30) Distribution and Classification of Multiple Coronae on Venus; 31) Recognition of Rayed Craters on Mars in THEMIS Thermal Infrared Imagery: Implications for Martian Meteorite Source Regions; 32) Geochemical Modeling of Evaporites on Mars: Insight from Meridiani Planum; 33) Hadean Crustal Processes Revealed from Oxygen Isotopes and U-Th-Pb Depth Profiling of Pre-4.0 Ga Detrital Zircons from Western Australia; 34) On Modeling the Seepage of Water into the Martian Subsurface; 35) Martial Gullies and Groundwater: A Series of Unfortunate Exceptions; 36) Olivine and Carbonate Globules in ALH84001: A Terrestrial Analog, and Implications for Water on Mars; 37) A Reevaluation of Mass Movements Within the Valles Marineris Region of Mars Using MOLA and MOC Data; 38) Evidence of Hydrated 109P/Swift-Tuttle Meteoroids from Meteor Spectroscopy; 39) Cr-54 Anomalies in the Solar System: Their Extent and Origin; 40) Reevaluation of the Mn-53-Cr-53 Systematic in the Basaltic Achondrites; 41) Effective Liquid Metal-Silicate Mixing Upon Shock by Power-Law Droplet Size Scaling in Richtmyer-Meshkov Like Perturbations; 42) Post-Impact Deformation of Impact Craters: Towards a Better Understanding Through the Study of Mjolnir Crater; 43) Cutting Silica Aerogel for Particle Extraction; 44) Liquid Hydrocarbons on Titan's Surface? How Cassini ISS Observations Fit into the Story (So Far); and 45) Mesoscale Simulations of Polar Circulations: Late Spring to Late Summe

Source record↗

Calipso Observations of the Dependence of Homo- and Heterogeneous Ice Nucleation in Cirrus Clouds on Latitude, Season and Surface Condition

There are two fundamental mechanisms through which cirrus clouds form; homo- and heterogeneous ice nucleation (henceforth hom and het). The relative contribution of each mechanism to ice crystal production often determines the microphysical and radiative properties of a cirrus cloud. A new satellite remote sensing method is described in this study to estimate cirrus cloud ice particle number concentration and the relative contribution of hom and het to cirrus cloud formation as a function of altitude, latitude, season and surface type (e.g. land vs. ocean). This method uses co-located observations from the Infrared Imaging Radiometer (IIR) and from the CALIOP (Cloud and Aerosol Lidar with Orthogonal Polarization) lidar aboard the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) polar orbiting satellite, employing IIR channels at 10.6 μm and 12.05 μm. The method is applied here to single-layered clouds of visible optical depth between about 0.3 and 3. Two years of Version 3 data have been analyzed for the years 2008 and 2013, with each season characterized in terms of 532 nm cirrus cloud centroid altitude and temperature, the cirrus cloud ice particle number concentration, effective diameter, layer-average ice water content and visible optical depth. Using a conservative criterion for hom cirrus, on average, the sampled cirrus clouds formed through hom occur about 43% of the time in the Arctic and 50% of the time in the Antarctic, and during winter at mid-latitudes in the Northern Hemisphere, hom cirrus occur 37% of the time. Elsewhere (and during other seasons in the Northern Hemisphere mid-latitudes), this hom cirrus fraction is lower. Processes that could potentially explain these observations are discussed, as well as the potential relevancy of these results to ice nucleation studies, climate modeling and jet-stream dynamics.

Mitchell, David L.↗

Charge-Transport Mechanisms in CuInSe x S 2– x Quantum-Dot Films

Colloidal quantum dots (QDs) have attracted considerable attention as promising materials for solution-processable electronic and optoelectronic devices. Copper indium selenium sulfide (CuInSe x S 2–x or CISeS) QDs are particularly attractive as an environmentally benign alternative to the much more extensively studied QDs containing toxic metals such as Cd and Pb. Carrier transport properties of CISeS-QD films, however, are still poorly understood. Here, we aim to elucidate the factors that control charge conductance in CISeS QD solids and, based on this knowledge, develop practical approaches for controlling the polarity of charge transport and carrier mobilities. To this end, we incorporate CISeS QDs into field-effect transistors (FETs) and perform detailed characterization of these devices as a function of the Se/(Se+S) ratio, surface treatment, thermal annealing, and the identity of source and drain electrodes. We observe that as-synthesized CuInSe x S 2–x QDs exhibit degenerate p-type transport, likely due to metal vacancies and CuIn’’ anti-site defects (Cu 1+ on an In 3+ site) that act as acceptor states. Moderate-temperature annealing of the films in the presence of indium source and drain electrodes leads to switching of the transport polarity to nondegenerate n-type, which can be attributed to the formation of In-related defects such as In Cu •• (an In 3+ cation on a Cu 1+ site) or In i ••• (interstitial In3+) acting as donors. We observe that the carrier mobilities increase dramatically (by 3 orders of magnitude) with increasing Se/(Se+S) ratio in both n- and p-type devices. To explain this observation, we propose a two-state conductance model, which invokes a high-mobility intrinsic band-edge state and a low-mobility defect-related intragap state. These states are thermally coupled, and their relative occupancies depend on both QD composition and temperature. Here, our observations suggest that the increase in the relative fraction of Se moves conduction- and valence band edges closer to low-mobility intragap levels. This results in increased relative occupancy of the intrinsic band-edge states and a corresponding growth of the measured mobility. Further improvement in charge-transport characteristics of the CISeS QD samples as well as their stability is obtained by infilling the QD films with amorphous Al 2 O 3 using atomic layer deposition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Crustal structure of Mars from gravity and topography

Mars Orbiter Laser Altimeter (MOLA) topography and gravity models from 5 years of Mars Global Surveyor (MGS) spacecraft tracking provide a window into the structure of the Martian crust and upper mantle. We apply a finite-amplitude terrain correction assuming uniform crustal density and additional corrections for the anomalous densities of the polar caps, the major volcanos, and the hydrostatic flattening of the core. A nonlinear inversion for Moho relief yields a crustal thickness model that obeys a plausible power law and resolves features as small as 300 km wavelength. On the basis of petrological and geophysical constraints, we invoke a mantle density contrast of 600 kg m-3; with this assumption, the Isidis and Hellas gravity anomalies constrain the global mean crustal thickness to be >45 km. The crust is characterized by a degree 1 structure that is several times larger than any higher degree harmonic component, representing the geophysical manifestation of the planet's hemispheric dichotomy. It corresponds to a distinction between modal crustal thicknesses of 32 km and 58 km in the northern and southern hemispheres, respectively. The Tharsis rise and Hellas annulus represent the strongest components in the degree 2 crustal thickness structure. A uniform highland crustal thickness suggests a single mechanism for its formation, with subsequent modification by the Hellas impact, erosion, and the volcanic construction of Tharsis. The largest surviving lowland impact, Utopia, post-dated formation of the crustal dichotomy. Its crustal structure is preserved, making it unlikely that the northern crust was subsequently thinned by internal processes.

Neumann, G. A.↗