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At least 613 records · Page 34

Tuning Magnetic Symmetry and Properties in the Olivine Series Li 1–x Fe x Mn 1–x PO 4 through Selective Delithiation

In this work, we present the first in-depth study of the nuclear and magnetic structures of the fully lithiated LiFe x Mn 1–x PO 4 solid solutions as well as the partially delithiated Li 1– xFe x Mn 1–x PO 4 series using neutron powder diffraction. By using a weak oxidizing solution that only oxidizes Fe 2+ , we find that lithium can be removed from these olivines in a stepwise manner. Representational analysis was performed on the observed magnetic reflections and found that the lithiated solid solutions order in the magnetic space group Pnma', which is identical to triphylite (LiFePO 4 ). We report that, even when removing 20% of the lithium from the hcp lattice, the magnetic structure changes and multiple magnetic contributions are needed to fully encompass the observed magnetic order. We find that the partially delithiated x = 0.2 and 0.3 have a magnetic structure P2 1 '/n11, and when x surpasses 0.3, the magnetic structure changes to P2 1 2 1 2 1 . We give a detailed report on the effect of delithiation on magnetic order, bond distances/angles, and the super- and supersuperexchange interactions in the material. The symmetries of the magnetic order of these solid solutions are then discussed with regard to their potential as ferrotoroidic candidates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Strain-induced structural defects and their effects on the electrochemical performances of silicon core/germanium shell nanowire heterostructures

Here we report on strain-induced structural defect formation in core Si nanowire of Si/Ge core/shell nanowire heterostructure and influences of the structural defects on the electrochemical performances in lithium-ion battery anodes based on Si/Ge core/shell nanowire heterostructures. The induced structural defects consisting of stacking faults and dislocations in the core Si nanowire were observed for the first time. The generation of stacking faults in Si/Ge core/shell nanowire heterostructure is observed to prefer settling in either only Ge shell region or in both Ge shell and Si core regions and is associated with the increase of the shell volume fraction. The relax of misfit strain in [112] oriented core/shell nanowire heterostructure leads to subsequent gliding of Shockley partial dislocations, preferentially forming the twins. The observation of cross-over defect formation is of great importance for the understanding of heteroepitaxy in radial heterostructures at nanoscale and building the three dimensional heterostructures for the various applications. In addition, the effect of the defect formation on nanomaterial’s functionality is investigated by electrochemical performance test. The Si/Ge core/shell nanowire heterostructures enhance the gravimetric capacity of lithium ion battery anodes under fast charging/discharging rates compared to Si nanowires. However, the induced structural defects hamper lithiation of the Si/Ge core/shell nanowire heterostructure.

36 MATERIALS SCIENCE↗

Comparison of divertor behavior and plasma confinement between argon and neon seeding in EAST

The exhaust of excessively high heat and particle fluxes on the divertor target is crucial for EAST long-pulse operation. In the recent EAST experiments, stable partial energy detachment around the upper outer strike point with H 98,y2 ~ 1 was achieved with either Ne or Ar seeding from the upper outer divetor target in the upper single null configuration with ITER-like tungsten divertor. With either Ar or Ne seeding, the electron temperature around the upper outer strike point (T et,UOSP ) was maintained at around 5 eV, the peak temperature of divertor target surface around the upper outer strike point (T div,UO ) decreased significantly, and material sputtering was well suppressed. Here, it was observed that there was less Ar seeding needed for partial energy detachment onset than Ne seeding, which shows that Ar is more efficient in the cooling of T et on the upper outer divertor than Ne. However, there was no detachment on the upper inner divertor with T et around strike point (T et,UISP ) remaining >10 eV with either Ar or Ne seeding from the upper outer divertor. Accompanied with the disappearance of double peak phenomenon of ion flux density on the upper inner divertor target (j s,UI ), the peak T div,UI around the strike point increased to around 300 °C. Although the heat flux on the upper inner divertor target (q t,UI ) is still in the acceptable level, either Ar or Ne seeding only from the upper outer divertor target is not enough to protect the upper inner divertor target from sputtering under current EAST conditions. On the other hand, Ar seeding always causes confinement degradation in the partial energy detachment state. It was observed that there is a slight confinement improvement (~10%) with Ne seeding, which may be due to density peaking, dilution effects and stabilization of the ion temperature gradient mode.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

The role of hydrogen during Pt–Ga nanocatalyst formation

Hydrogen is a critical element during the in situ assembly of tailored catalytic materials, and serves as key ingredient in multifarious chemical reactions promoted by these catalysts. Despite intensive debate for several decades, the existence and nature of hydrogen-involved mechanisms – such as hydrogen-spillover, surface migration – have not been unambiguously proven and elucidated up to date. In this work, Pt–Ga alloy formation is used as a probe reaction to study the behavior and atomic transport of H and Ga, starting from Pt nanoparticles on hydrotalcite-derived Mg(Ga)(Al)O x supports. In situ XANES spectroscopy, time-resolved TAP kinetic experiments, HAADF-STEM imaging and EDX mapping are combined to probe Pt, Ga and H in a series of H 2 reduction experiments up to 650 °C. Mg(Ga)(Al)O x by itself dissociates hydrogen, but these dissociated hydrogen species do not induce significant reduction of Ga 3+ cations in the support. Only in the presence of Pt, partial reduction of Ga 3+ into Ga δ+ is observed, suggesting that different reaction mechanisms dominate for Pt- and Mg(Ga)(Al)O x -dissociated hydrogen species. This partial reduction of Ga 3+ is made possible by Pt-dissociated H species which spillover onto non-reducible Mg(Al)O x or partially reducible Mg(Ga)(Al)O x and undergo long-range transport over the support surface. Moderately mobile Ga δ+ O x migrates towards Pt clusters, where Ga δ+ is only fully reduced to Ga 0 on condition of immediate stabilization inside Pt–Ga alloyed nanoparticles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Solvent-mediated charge separation drives alternative hydrogenation path of furanics in liquid water

Compared to the vapour phase, liquid-phase heterogeneous catalysis provides additional degrees of freedom for reaction engineering, but the multifaceted solvent effects complicate analysis of the reaction mechanism. Here, using furfural as an example, we reveal the important role of water-mediated protonation in a typical hydrogenation reaction over a supported Pd catalyst. Depending on the solvent, we have observed different reaction orders with respect to the partial pressure of H 2 , as well as distinct selectivity towards hydrogenation of the conjugated C=O and C=C double bonds. Free energy calculations show that H 2 O participates directly in the kinetically relevant reaction step and provides an additional channel for hydrogenation of the aldehyde group, in which hydrogen bypasses the direct surface reaction via a hydrogen-bonded water network. In conclusion, this solution-mediated reaction pathway shows the potential role of the solvent for tuning the selectivity of metal-catalysed hydrogenation when charge separation on the metal surface is feasible.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Microwave Polarized Signatures Generated within Cloud Systems: SSM/I Observations Interpreted with Radiative Transfer Simulations

Special Sensor Microwave /Imager (SSM/I) observations in cloud systems are studied over the tropics. Over optically thick cloud systems, presence of polarized signatures at 37 and 85 GHz is evidenced and analyzed with the help of cloud top temperature and optical thickness extracted from visible and IR satellite observations. Scattering signatures at 85 GHz (TbV(85) less than or = 250 K) are associated with polarization differences greater than or = 6 K, approx. 50%, of the time over ocean and approx. 40% over land. In addition. over thick clouds the polarization difference at 37 GHz is rarely negligible. The polarization differences at 37 and 85 GHz do not stem from the surface but are generated in regions of relatively homogeneous clouds having high liquid water content. To interpret the observations, a radiative transfer model that includes the scattering by non-spherical particles is developed. based on the T-matrix approach and using the doubling and adding method. In addition to handling randomly and perfectly oriented particles, this model can also simulate the effect of partial orientation of the hydrometeors. Microwave brightness temperatures are simulated at SSM/I frequencies and are compared with the observations. Polarization differences of approx. 2 K can be simulated at 37 GHz over a rain layer, even using spherical drops. The polarization difference is larger for oriented non-spherical particles. The 85 GHz simulations are very sensitive to the ice phase of the cloud. Simulations with spherical particles or with randomly oriented non-spherical ice particles cannot replicate the observed polarization differences. However, with partially oriented non-spherical particles, the observed polarized signatures at 85 GHz are explained, and the sensitivity of the scattering characteristics to the particle size, asphericity, and orientation is analyzed. Implications on rain and ice retrievals are discussed.

Prigent, Catherine↗

Comparative Analysis of the Luminescence of Ge:Sb Layers Grown on Ge(001) and Si(001) Substrates

Comparative studies of the luminescence properties of Sb-doped Ge layers grown on Ge(001) and Si(001) substrates are carried out. It is shown that, in contrast to the case of Ge:Sb layers grown on Si, a considerable contribution to the photoluminescence signal from Ge:Sb/Ge(001) layers is made by indirect optical transitions. This fact is attributed to the longer charge-carrier lifetime in Ge:Sb/Ge homoepitaxial structures because of the lack of crystal-lattice defects related to the relaxation of elastic strains in such structures. It is shown that the experimentally observed significant increase in the contribution of direct optical transitions to the total photoluminescence signal with increasing doping level of Ge:Sb/Ge(001) layers results from an increase in the population of electron states in the Γ valley. At Sb concentrations much higher than the equilibrium solubility of Sb in Ge, partial electrical activation of the impurity is observed, and in this case, a profound effect on the emission properties of Ge:Sb layers grown on different substrates is produced by nonradiative-recombination centers, whose role can be played by clusters of impurity atoms.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

THE COEVOLUTION OF NUCLEAR STAR CLUSTERS, MASSIVE BLACK HOLES, AND THEIR HOST GALAXIES

Studying how nuclear star clusters (NSCs) form and how they are related to the growth of the central massive black holes (MBHs) and their host galaxies is fundamental for our understanding of the evolution of galaxies and the processes that have shaped their central structures. We present the results of a semi-analytical galaxy formation model that follows the evolution of dark matter halos along merger trees, as well as that of the baryonic components. This model allows us to study the evolution of NSCs in a cosmological context, by taking into account the growth of NSCs due to both dynamical-friction-driven migration of stellar clusters and star formation triggered by infalling gas, while also accounting for dynamical heating from (binary) MBHs. We find that in situ star formation contributes a significant fraction (up to ∼80%) of the total mass of NSCs in our model. Both NSC growth through in situ star formation and that through star cluster migration are found to generate NSC—host galaxy scaling correlations that are shallower than the same correlations for MBHs. We explore the role of galaxy mergers on the evolution of NSCs and show that observational data on NSC—host galaxy scaling relations provide evidence of partial erosion of NSCs by MBH binaries in luminous galaxies. We show that this observational feature is reproduced by our models, and we make predictions about the NSC and MBH occupation fraction in galaxies. We conclude by discussing several implications for theories of NSC formation.

79 ASTRONOMY AND ASTROPHYSICS↗

Changes of snow cover, temperature, and radiative heat balance over the Northern Hemisphere

Contemporary large-scale changes in satellite-derived snow cover were examined over the Northern Hemisphere extratropical land (NEL) areas. These areas encompass 55% of the land in the Northern Hemisphere. Snow cover (S) transient regions, the 'centers of action' relative to interannual variations of snow cover, were identified for the years 1972-1992. During these years a global retreat in snow cover extent (SE) occurred in the second half of the hydrologic year (April-September). Mean annual SE has decreased by 10% (2.3 x 10(exp 6) sq km). Negative trends account for one-third to one-half of the interannual continental variance of SE. The historical influence of S on the planetary albedo and outgoing longwave radiation (OLR) is investigated. The mean annual response of the S feedback on the radiative balance (RB) is negative and suggests a largescale heat redistribution. During autumn and early winter (up to January), however, the feedback of S on the planetary RB may be positive. Only by February does the cooling effect of S (due to albedo increase) dominate the planetary warming due to reduced OLR over the S. Despite a wintertime maximum in SE, the feedback in spring has the greatest magnitude. The global retreat of spring SE should lead to a positive feedback on temperature. Based on observed records of S, changes in RB are calculated that parallel an observed increase of spring temperature during the past 20 years. The results provide a partial explanation of the significant increase in spring surface air temperature observed over the land areas of the Northern Hemisphere during the past century. The mean SE in years with an El Nino and La Nina were also evaluated. El Nino events are generally accompanied by increased SE over the NEL during the first half of the hydrological year. In the second half of the hydrologic year (spring and summer), the El Nino events are accompanied by a global retreat of SE.

Groisman, Pavel YA.↗

First Measurements of the Double-Polarization Observables F , P , and H in ω Photoproduction off Transversely Polarized Protons in the N * Resonance Region

First measurements of double-polarization observables in ${\omega}$ photoproduction off the proton are presented here using transverse target polarization and data from the CEBAF Large Acceptance Spectrometer (CLAS) FROST experiment at Jefferson Lab. The beam-target asymmetry $F$ has been measured using circularly polarized, tagged photons in the energy range 1200–2700 MeV, and the beam-target asymmetries $H$ and $P$ have been measured using linearly polarized, tagged photons in the energy range 1200–2000 MeV. These measurements significantly increase the database on polarization observables. The results are included in two partial-wave analyses and reveal significant contributions from several nucleon (${N}^{*}$) resonances. In particular, contributions from new ${N}^{*}$ resonances listed in the Review of Particle Properties are observed, which aid in reaching the goal of mapping out the nucleon resonance spectrum.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

ENERGETIC PARTICLE PRESSURE AT INTERPLANETARY SHOCKS: STEREO-A OBSERVATIONS

We study periods of elevated energetic particle intensities observed by STEREO-A when the partial pressure exerted by energetic (≥83 keV) protons (P{sub EP}) is larger than the pressure exerted by the interplanetary magnetic field (P{sub B}). In the majority of cases, these periods are associated with the passage of interplanetary shocks. Periods when P{sub EP} exceeds P{sub B} by more than one order of magnitude are observed in the upstream region of fast interplanetary shocks where depressed magnetic field regions coincide with increases of energetic particle intensities. When solar wind parameters are available, P{sub EP} also exceeds the pressure exerted by the solar wind thermal population (P{sub TH}). Prolonged periods (>12 hr) with both P{sub EP} > P{sub B} and P{sub EP} > P{sub TH} may also occur when energetic particles accelerated by an approaching shock encounter a region well upstream of the shock characterized by low magnetic field magnitude and tenuous solar wind density. Quasi-exponential increases of the sum P{sub SUM} = P{sub B} + P{sub TH} + P{sub EP} are observed in the immediate upstream region of the shocks regardless of individual changes in P{sub EP}, P{sub B}, and P{sub TH}, indicating a coupling between P{sub EP} and the pressure of the background medium characterized by P{sub B} and P{sub TH}. The quasi-exponential increase of P{sub SUM} implies a radial gradient ∂P{sub SUM}/∂r > 0 that is quasi-stationary in the shock frame and results in an outward force applied to the plasma upstream of the shock. This force can be maintained by the mobile energetic particles streaming upstream of the shocks that, in the most intense events, drive electric currents able to generate diamagnetic cavities and depressed solar wind density regions.

79 ASTRONOMY AND ASTROPHYSICS↗

Electron thermal confinement in a partially stochastic magnetic structure

Using a high-repetition-rate Thomson scattering diagnostic, we observe a peak in electron temperature $T_e$ coinciding with the location of a large magnetic island in the Madison Symmetric Torus. Magnetohydrodynamic modeling of this quasi-single helicity plasma indicates that smaller adjacent islands overlap with and destroy the large island flux surfaces. The estimated stochastic electron thermal conductivity (≈30 m 2 /s) is consistent with the conductivity inferred from the observed $T_e$ gradient and ohmic heating power. Island-shaped $T_e$ peaks can result from partially stochastic magnetic islands.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Ocean Surface Carbon Dioxide Fugacity Observed from Space

We have developed and validated a statistical model to estimate the fugacity (or partial pressure) of carbon dioxide (CO2) at sea surface (pCO2sea) from space-based observations of sea surface temperature (SST), chlorophyll, and salinity. More than a quarter million in situ measurements coincident with satellite data were compiled to train and validate the model. We have produced and made accessible 9 years (2002-2010) of the pCO2sea at 0.5 degree resolutions daily over the global ocean. The results help to identify uncertainties in current JPL Carbon Monitoring System (CMS) model-based and bottom-up estimates over the ocean. The utility of the data to reveal multi-year and regional variability of the fugacity in relation to prevalent oceanic parameters is demonstrated.

Liu, W. Timothy↗

Ocean surface carbon dioxide fugacity observed from space

We have developed and validated a statistical model to estimate the fugacity (or partial pressure) of carbon dioxide (CO2) at sea surface (pCO2sea) from space-based observations of sea surface temperature (SST), chlorophyll, and salinity. More than a quarter million in situ measurements coincident with satellite data were compiled to train and validate the model. We have produced and made accessible 9 years (2002–2010) of the pCO2sea at 0.5 degree resolutions daily over the global ocean. The results help to identify uncertainties in current JPL Carbon Monitoring System (CMS) model-based and bottom-up estimates over the ocean. The utility of the data to reveal multi-year and regional variability of the fugacity in relation to prevalent oceanic parameters is demonstrated.

Xie, Xiaosu↗

A chemical study of individual green glasses and brown glasses from 15426 - Implications for their petrogenesis

Systematic chemical analyses of individual Apollo 15 green glasses were performed in order to: (1) study chemical variations among them; (2) understand their petrogenesis and source region; and (3) study their possible relationships with mare basalts in general. Brown glasses were also analyzed in order to study their chemical variations and their petrogenetic relationships to green glasses and mare basalts. The chemical composition of green and brown glasses is shown and variation diagrams of Sc, Cr2O3, FeO, and Co abundances in green glasses are presented. Igneous fractionation, two component magma mixing, and partial melting of heterogeneous source materials are alternate scenarios to explain strong observed correlations. The composition of green glasses indicates that they were derived by partial melting of the fractionated cumulate source materials formed from a magma ocean which had experienced certain degrees of olivine and plagioclase fractional crystallization.

Ma, M.-S.↗

Percepts of rigid motion within and across apertures

Humans consistently err in their percepts of rotational motion viewed through an aperture. Such errors provide insight into the constraints observers use to interpret retinal images. In the first of two experiments, Ss consistently perceived the fixed center of rotation for an unmarked line viewed through an aperture as located on the line, regardless of its actual location. Accuracy greatly improved with visible line endings. This finding was extended to explain why a square appears nonrigid when it rotates behind a partial occluder. This illusion may result from observers misperceiving the center of rotation of the unmarked square sides. In this situation, Ss seemed unable to apply an object rigidity constraint across apertures. These findings support a conceptualization of the visual system in which consistent local information must be clearly present before prior knowledge can be used to interpret retinal stimulation.

Shiffrar, Maggie↗

An alternative interpretation of Jupiter's 'plasmapause'

It has recently been suggested that Io is an important source of ions for the plasma detected by Pioneer 10 in the inner magnetosphere of Jupiter. Assuming this to be true, we show that near the orbit of Io the central collector of the Pioneer-10 plasma instrument could detect only inwardly diffusing ions created at a radial distance greater than that of the spacecraft. The rapid decrease in ion density observed beyond Io's orbit is attributed, at least partially, to this effect and thus may not represent a real plasma boundary such as a 'plasmapause'. Instead, the drop in observed ion density could correspond to a decrease in the density of Io-associated neutral particles orbiting Jupiter.

Neugebauer, M.↗