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Composition dependence of atomic order in strain-relaxed, metastable GeSn alloys
Extended x-ray absorption fine structure (EXAFS) measurements of single-crystal Ge/GeSn radial heterostructure nanowires are used to examine the effects of composition on both short-range order (SRO) and longer-range disorder in GeSn alloys. GeSn has prompted significant interest because it can achieve a direct band gap for sufficient Sn concentrations beyond the equilibrium solid solubility limit in an all-group IV system. Short-range order in this material is particularly interesting as it has been predicted to affect the band gap independent of average composition or strain effects. By independently controlling the Sn composition and GeSn thickness during chemical vapor deposition of misfitting GeSn shells around ultrathin, elastically compliant, Ge core nanowires, the elastic misfit strain in the GeSn is minimized for Sn compositions over the studied range ≈Ge 0.96 Sn 0.04 to Ge 0.88 Sn 0.12 . The degree of SRO was found to decrease with increasing Sn composition. Additionally, damping of the EXAFS signal was observed as the Sn content increased, particularly for increasingly distant atomic shells about the absorbing atom, even for scattering paths not involving Sn atoms. This result is quantified as an increase in the mean-squared relative displacement parameters of the shells. These measurements reveal the accommodation of local strain due to the presence of the highly size-mismatched Sn atoms in the Ge diamond cubic lattice (≈14%), which may have effects on the band structure of the material in addition to the influence of short-range atomic order. Comparison among the nanowire samples allows for calculation of the topological rigidity parameter, a ∗∗ , for the first-neighbor bond lengths. Furthermore, these exhibit chemically distinct values for Ge-Ge, Ge-Sn, and Sn-Sn, and they are consistent with the value a ∗∗ = 0.75 ± 0.07 confirming the general applicability of the model to alloys with both large amounts of natural misfit strain and the potential for short-range order.
Ultrastructural pathogenesis of lesions produced by exposure to oxygen difluoride with correlative light microscopy
The lungs of rats exposed to OF2 were examined by light and electron microscopy. The exposures were for 30 to 60 minutes to an average of 4.5 ppm OF2, the minimal lethal dose. Animals were sacrificed after 30 (group 1) and 60 minutes (group 2) exposure and 1 (group 3) and 2 (group 4) hours following 60 minutes exposure. Mild gross changes were observed in groups 3 and 4, but no light microscopic lesions were found. Alterations were noted in all four groups using electron microscopy. These were mostly indicative of fluid change and consisted of blebbing of the endothelial and epithelial layers of the alveolocapillary wall and rarification of the cytoplasm of these cells. The lamellar bodies of the Type II cells showed an increasing and consistent loss of matrix structure and density. These fine structural changes increased in quantity and severity as time of exposure or post-exposure period increased. (Modified author abstract)
Fine-scale structure of a cold hydrogen layer
Neutral-hydrogen absorption-line interferometer observations are reported for five continuum radio sources situated behind an extensive layer of cold interstellar H I gas. In contrast to low-spatial-resolution emission-line observations reported earlier which show the large-scale uniformity of the layer, the high-spatial-resolution absorption-line observations reveal variations in the velocity and density within the layer. The new results together with the old indicate the apparent coexistence of a large-scale mechanism for triggering the formation of cold hydrogen and an instability mechanism leading to small-scale irregularities.
Fine-scale structure of the Jovian magnetotail current sheet
During the outbound leg of its passage through the Jovian magnetosphere in the Voyager 2 spacecraft observed 50 traversals of the magnetotail current sheet during a 10 day period at distances between 30 and 130 R sub j. Analysis of these observations shown that the Jovian tail sheet tends to lie approximately parallel to the ecliptic plane and to oscillate about the tail axis with the 10 hour planetary rotation period. The magnetic structure near and within the current sheet was variable with time and distance from Jupiter, but generally corresponded to one of the following: (1) simple rotation of field across the sheet, with an approximately southward direction in the sheet (generally northward beyond a distance from Jupiter of approximately 84 R sub j; (2) field having a southward component in a broad region near the sheet, but northward in a restricted region at the sheet itself; or (3) a clear bipolar variation of the sheet normal field component as the sheet was crossed (i.e., the field became northward and then southward, or vice versa, in crossing the sheet).
Fine time structure in the 1979 March 5 gamma ray burst
Data on the impulsive phase of the 1979 March 5 gamma ray burst, taken by three identical detectors aboard the Prognoz 7, Venera 11, and Venera 12 spacecraft with 2 ms time resolution, are presented. The first 200 ms of the time history may be described by an exponential decay with time constant of approximately 120 ms up to approximately 100 ms, and time constant of approximately 30 ms thereafter; at low energies, a pulsating component with a period of approximately 23 ms appears. The data could be consistent with torsional vibrations of a neutron star, the rotation of a rapidly spinning neutron star, or oscillations caused by interactions between hot plasma and a magnetic field.
Fine-scale structure of the Jovian magnetotail current sheet
New evidence concerning the detailed structure of the magnetic field in and near the Jovian tail sheet is presented, and nonunique temporal variations in the sheet structure are deduced. Data from Voyagers 1 and 2 are used to show that the local sheet structure, while tending to vary with time and distance from Jupiter, generally corresponds to one of four general types. The four types are classified using examples, and possible geometries associated with each type are identified. The locations of the different types of sheet crossings are pointed out and discussed. The possibility of reconnection occurring at the current sheet is discussed through analogy with the terrestrial magnetotail. It is concluded that the results support the view that reconnection occurs in the Jovian magnetotail as a time-dependent, and possibly spatially localized, process.
Correspondence between solar fine-scale structures in the corona, transition region, and lower atmosphere from collaborative observations
The Soft X-Ray Imaging Payload and the High Resolution Telescope and Spectrograph (HRTS) instrument were launched from White Sands on 11 December 1987 in coordinated sounding rocket flights to investigate the correspondence of coronal and transition region structures, especially the relationship between X-ray bright points (XBPs) and transition region small spatial scale energetic events. The coaligned data from X-ray images are presented along with maps of sites of transition region energetic events observed in C IV (100,000 K), HRTS 1600 A spectroheliograms of the T sub min region and ground based magnetogram and He I 10830 A images.
Fine-scale structure in the -185 kilometers per second absorption by HCO(+) in the Galactic center
We present a high-resolution study of the HCO(+) (J = 1-0) absorption by the 'high-velocity gas' at velocities between -170 and -200 km/s in Sgr A West. The absorption against the continuum radiation from the ionized gas features in Sgr A West (in particular the 'bar') is stronger than it is against Sgr A which is separated from the ionized gas by a few arcseconds. The positions of peak HCO(+) opacity coincide with the positions of Ne II emission at these velocities. These observations suggest that, even though emission is detected from gas at these high velocities over several arcminutes, some of the absorbing molecular gas may be mixed in with the ionized gas close to Sgr A. Simple calculations show that sufficient shielding can exist in the ionized features to allow molecules to survive very close to the ionizing source.
Ultra Fine-Scale Structure in the Inner Corona
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Additive Manufactured Ultra-Fine Lattice Structures for Propulsion Catalysts
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Overview of Selected Solar Fine-Scale Structures: Chromospheric Spicules and Coronal Jets
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Fine Harmonic Structure of Equatorial Noise with a Quasiperiodic Modulation
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Ligand-coordination effects on the selective hydrogenation of acetylene in single-site Pd-ligand supported catalysts
The selective hydrogenation of acetylene to ethylene is a critical step in the synthesis of polyethylenes. Achieving high conversion to ethylene without over-hydrogenation to ethane is a challenge that requires control of the transition metal site, which we achieve through a ligand-coordinated supported catalyst (LCSC) strategy. Using Pd catalysts coordinated to 1,10-phenanthroline-5,6-dione (PDO) ligands on CeO2 supports, we have discovered that the reaction selectivity depends strongly on the ligand:metal ratio with higher selectivity when more ligand is present in the catalyst. Catalyst structure was examined by extended X-ray absorption fine structure spectroscopy, transmission electron microscopy, and CO adsorption, which indicate single-atom character of the Pd. The ligand:metal ratio is determined by Xray photoelectron spectroscopy measurements and correlated with hydrogenation reactions under steady-state flow conditions to examine trends in hydrogenation activity and selectivity. Those trends can be better understood by density functional theory calculations that indicate hydrogen binding on the ligand to guide reaction selectivity toward the desired ethylene hydrogenation product. Here these results demonstrate the importance of considering the dynamic character of LCSCs and inform the design of future single-site heterogeneous catalysts.
Fine and hyperfine structure of the 3 super 2 P term in lithium.
Fine and hyperfine structure of term in 3p level of lithium studied by level-crossing spectroscopy technique, determining fine structure separation value
Calcium-Uranyl-Carbonato Species Kinetically Limit U(VI) Reduction by Fe(II) and Lead to U(V)-Bearing Ferrihydrite
Reaction conditions and mechanisms promoting or inhibiting U reduction exert a central control on U solubility and, therefore, U transport and its associated risks. Here, we vary and track common aqueous uranium species to show that a kinetic restriction inhibits homogeneous reduction of the calcium-uranyl-carbonato species (CaUO$_2$(CO$_3$)$_3$$^{2–}$ and Ca$_2$UO$_2$(CO$_3$)$_3$) by Fe(II)$_{(aq)}$, while ferrihydrite surface-catalyzed reduction of all aqueous uranyl by Fe(II) proceeds. Using U L$_3$ high energy resolution fluorescence detection (HERFD) X-ray absorption near edge structure (XANES) spectroscopy, U L$_3$ extended X-ray absorption fine structure (EXAFS) spectroscopy, and transmission electron microscopy (TEM), we also show that U(V) is generated and incorporated into ferrihydrite formed from homogeneous U(VI) reduction by Fe(II)(aq). Through elucidation of the mechanisms that inhibit reduction of the calcium-uranyl-carbonato species and promote stabilization of U(V), we advance our understanding of the controls on U solubility and thus improve prediction of U transport in surface and subsurface systems.
High manganese redox variability and manganate predominance in temperate soil profiles as determined by X-ray absorption spectroscopy
Manganese speciation is a key to understanding the fate of contaminants, nutrients, and organic matter in soils. To date, quantification of Mn species in bulk soils has been performed mainly by sequential extraction methods and rarely supported by spectroscopic analysis. In order to obtain quantitative information on the Mn species inventory of soils, we investigated 46 soil horizons (<2-mm fraction, 45.1–2,280 mg/kg Mn) of nine typical Central European soils (Cambisols, Chernozems, Luvisols, Podzol, Stagnosol) by chemical Mn analyses and Mn K-edge X-ray absorption spectroscopy, and related speciation results to major soil properties. Amounts of Mn 2+ , Mn 3+ , and Mn 4+ and the average oxidation state of Mn were evaluated by linear combination fitting (LCF) of X-ray absorption near edge structure (XANES) spectra. Additionally, we used extended X-ray absorption fine structure (EXAFS) spectroscopy to identify and quantify major Mn species. For this, EXAFS spectra of 20 organic and mineral soil samples from five soils (Cambisols, Chernozem, Luvisol) were analyzed by LCF and shell fitting. XANES analyses revealed a high Mn redox variability in organic surface layers, with Mn 2+ being most abundant (≤100%, $\overline{x}$ = 54%), followed by Mn 3+ (≤80%, $\overline{x}$ = 32%) and Mn 4+ (≤55%, $\overline{x}$ = 14%). Mineral soil horizons contained significantly less Mn 2+ (≤56%, $\overline{x}$ = 23%), about equal quantities of Mn 3+ (≤68%, $\overline{x}$ = 31%), and were enriched in Mn 4+ (≤89%, $\overline{x}$ = 46%). EXAFS analyses implied the presence of six major Mn species groups: manganates, organically complexed Mn, Mn(III) oxyhydroxides, silicate-bound Mn, Mn oxides without tunnel- or layer structure, and physisorbed Mn. In litter horizons, Mn was mainly present in organic complexes (58–91%, $\overline{x}$ = 78%) and as physisorbed Mn (≤15%), but individual horizons also comprised manganates, Mn(III) oxyhydroxides, and silicate-bound Mn. Manganates, likely mixtures of phyllomanganates with hexagonal layer symmetry and tectomanganates, dominated in all mineral soil horizons (37–94%, $\overline{x}$ = 67%). Correlation analysis showed that manganates dissolve completely during dithionite-citrate and acid ammonium oxalate extractions, and suggested that Mn 4+ -rich manganates preferentially form under less acidic soil conditions, partly by oxidation of organically complexed Mn(II), and that they are enriched in the soil clay fraction. Mineral soil horizons also contained minor quantities of organically complexed Mn (≤39%, $\overline{x}$ = 11%), silicate-bound Mn (≤30%, $\overline{x}$ = 8%), Mn(III) oxyhydroxides (≤37%, $\overline{x}$ = 7%), Mn oxides without tunnel- or layer structure (≤18%, $\overline{x}$ = 5%), and physisorbed Mn (≤14%, $\overline{x}$ <1%). The detection of Mn(III) oxyhydroxides such as feitknechtite (β-MnOOH) or groutite (α-MnOOH) as well as the spinel hausmannite (Mn 3 O 4 ) in acidic soils is remarkable, since their formation is normally linked to neutral or alkaline pH conditions. Minor contributions of silicate-bound Mn indicate the release of Mn from primary minerals already at early stages of soil formation, and low concentrations of physisorbed Mn suggest that exchangeable Mn is rapidly converted into manganates in oxic soils. In conclusion, the predominance of manganates in mineral soils has far-reaching implications for the functioning of soils and biogeochemical element cycles, as these minerals play an important role in metal binding, plant nutrition, and redox-related processes.
Multielectronic and multiatomic effects in the U O 4,5 x-ray absorption spectroscopy of uranium dioxide
In order to explain all of the spectral features observed in the U O 4,5 x-ray absorption spectrum of uranium dioxide (UO 2 ), it is necessary to include both multielectron effects and multiatomic effects. The 5d (core hole)-5f (electron) angular momentum coupling that gives rise to the giant resonance has been treated within ligand field density functional theory, and the electron scattering that generates the extended x-ray absorption fine structure has been included via the spectral simulation program FEFF: both within a UO 8 fluorite cluster picture. An atomic model is insufficient to explain all of the observed spectral features.