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At least 613 records · Page 34

Probing Acceleration and Turbulence at Relativistic Shocks in Blazar Jets

Diffusive shock acceleration (DSA) at relativistic shocks is widely thought to be an important acceleration mechanism in various astrophysical jet sources, including radio-loud active galactic nuclei such as blazars. Such acceleration can produce the non-thermal particles that emit the broad-band continuum radiation that is detected from extragalactic jets. An important recent development for blazar science is the ability of Fermi-Large Area Telescope spectroscopy to pin down the shape of the distribution of the underlying non-thermal particle population. This paper highlights how multiwavelength spectra spanning optical to X-ray to gamma-ray bands can be used to probe diffusive acceleration in relativistic, oblique, magnetohydrodynamic (MHD) shocks in blazar jets. Diagnostics on the MHD turbulence near such shocks are obtained using thermal and non-thermal particle distributions resulting from detailed Monte Carlo simulations of DSA. These probes are afforded by the characteristic property that the synchrotron vF(sub v), peak energy does not appear in the gamma-ray band above 100 MeV. We investigate self-consistently the radiative synchrotron and inverse Compton signatures of the simulated particle distributions. Important constraints on the diffusive mean free paths of electrons, and the level of electromagnetic field turbulence are identified for three different case study blazars, Mrk 501, BL Lacertae and AO 0235+164. The X-ray excess of AO 0235+164 in a flare state can be modelled as the signature of bulk Compton scattering of external radiation fields, thereby tightly constraining the energy-dependence of the diffusion coefficient for electrons. The concomitant interpretations that turbulence levels decline with remoteness from jet shocks, and the probable significant role for non-gyroresonant diffusion, are posited.

Baring, Matthew G.↗

Extremely Slow Diffusion of Gold Nanoparticles under Confinement in Mesoporous Silica

Here, we report an X-ray photon correlation spectroscopy (XPCS) study of the mobility of colloidal gold nanoparticles with a diameter of approximately 4 nm in glycerol under confinement within the channels of SBA-15 mesoporous silica with pore diameters of approximately 6 and 12 nm. The XPCS correlation functions result from an effective heterodyne signal due to the mixing of the coherent scattering from the nanoparticles and the mesoporous silica. Over the range of wave vectors and hence length scales probed, the nanoparticle dynamics are well described by one-dimensional diffusion. The nanoparticle diffusivity varies with temperature in a manner expected based on the temperature-dependent viscosity of glycerol; however, the magnitudes of the diffusion coefficients are several orders of magnitude smaller than those of the nanoparticles in bulk glycerol. We consider mechanisms that might contribute to this reduction in diffusivity including enhancement in hydrodynamic drag under confinement, effects of nanoparticle adsorption to the pore walls, and slowing structural dynamics in glycerol due to the combination of the nanometer-scale confinement and the presence of the nanoparticles.

36 MATERIALS SCIENCE↗

A Data-driven, Physics-based Transport Model of Solar Energetic Particles Accelerated by Coronal Mass Ejection Shocks Propagating through the Solar Coronal and Heliospheric Magnetic Fields

Abstract In an effort to develop computational tools for predicting radiation hazards from solar energetic particles (SEPs), we have created a data-driven physics-based particle transport model to calculate the injection, acceleration, and propagation of SEPs from coronal mass ejection (CME) shocks traversing through the solar corona and interplanetary magnetic fields. The model runs on an input of corona and heliospheric plasma and magnetic field configuration from a magnetohydrodynamic model driven by solar photospheric magnetic field measurements superposed with observed CME shocks determined from coronagraph images. SEP source particles are injected at the shock using the result of diffusive shock acceleration formulation from a characteristic obliquity-dependent injection from a heated solar wind thermal tail population. With several advanced computation techniques involving stochastic simulation and integration, the model obtains the particle intensity at any location in interplanetary space through the rigorous solution to the time-dependent 5D focus transport equation in the phase space that includes perpendicular diffusion. We apply the model to the 2011 November 3 CME event. The calculation results reproduce multispacecraft SEP observations at Earth and STEREO-B reasonably well without normalization of particle flux. The observations at STEREO-A can be reproduced by rescaling particle energy or modified energy dependence of particle diffusion coefficients. This circumsolar SEP event seen by spacecraft at Earth, STEREO-A, and STEREO-B at widely separated longitudes can be explained by diffusive shock acceleration by a single CME shock with a moderate speed.

79 ASTRONOMY AND ASTROPHYSICS↗

Instability of ring current protons beyond the plasmapause during injection events.

The stability of ring current protons with an injection spectrum modeled by a loss cone distribution function is examined for typical ring current parameters. It is found that a quasi-electrostatic ion loss cone mode can be excited with frequencies just below and growth rates of the order of 0.01 times the ion plasma frequency. The instability is strongest in the moderate beta about equal to 1, low-density region just outside the plasmapause; for the beta much greater than 1 auroral regions and the high-density plasmasphere the mode is nearly stable. For the same ring current parameters the electromagnetic ion cyclotron wave is almost nonconvectively unstable, with growth rates of the order of 0.1 times the ion cyclotron frequency. The combination of the two unstable modes results in a large quasi-linear diffusion coefficient throughout most of the proton velocity space. Unless it is maintained by rapid inward convection, the ring current injection anisotropy will be reduced by diffusion toward the loss cone on time scales short in comparison to the minimum precipitation lifetime.

Coroniti, F. V.↗

The Fokker-Planck coefficient for pitch-angle scattering of cosmic rays

For the case of homogeneous, isotropic magnetic field fluctuations, it is shown that most theories which are based on the quasi-linear and adiabatic approximations yield the same integral for the Fokker-Planck coefficient for the pitch-angle scattering of cosmic rays. For example, despite apparent differences, the theories due to Jokipii and to Klimas and Sandri yield the same integral. It is also shown, however, that this integral in most cases has been evaluated incorrectly in the past. For small pitch angles, the errors in previous evaluations are fortuitously of minor importance. For large pitch angles, however, these errors become more significant; and for pitch angles of 90 deg, the actual Fokker-Planck coefficient contains a delta function which has been overlooked in the past. The implications of these corrections on the possibility of relating cosmic-ray diffusion coefficients to observed properties of the interplanetary magnetic field are discussed.

Fisk, L. A.↗

Zn diffusion in Al/0.7/Ga/0.3/As compared with that in GaAs

Zinc was diffused into 4 times 10 to the 17th per cu cm n-type Al(0.7)Ga(0.3)As grown by liquid-phase epitaxy and also into n-type 2 times 10 to the 17th per cu cm doped GaAs slices at 600, 650, and 750 C. The Zn diffusion coefficient in the Al(0.7)Ga(0.3)As was about one order of magnitude larger than in GaAs. The significance of this fact is that diffusion of Zn through a 0.5 micron Al(0.7)Ga(0.3)As layer appears to be possible with adequate control of the junction depth in the underlying GaAs.

Flat, A.↗

Diffusion of triglycine sulfate in aqueous solution

The diffusion coefficient of triglycine sulfate (TGS) in water was measured for several concentrations over a temperature range of 25 to 55 C. The activation energy for diffusion obtained from these measurements was 4180 cal/mol. No concentration dependence was seen. The maximum difference in D for the various ionic species present was determined by Raman spectroscopy to be about 5 percent.

Kroes, R. L.↗

Dynamic Theory of Relativistic Electrons Stochastic Heating by Whistler Mode Waves with Application to the Earth Magnetosphere

In the Hamiltonian approach an electron motion in a coherent packet of the whistler mode waves propagating along the direction of an ambient magnetic field is studied. The physical processes by which these particles are accelerated to high energy are established. Equations governing a particle motion were transformed in to a closed pair of nonlinear difference equations. The solutions of these equations have shown there exists the energetic threshold below that the electron motion is regular, and when the initial energy is above the threshold an electron moves stochastically. Particle energy spectra and pitch angle electron scattering are described by the Fokker-Planck-Kolmogorov equations. Calculating the stochastic diffusion of electrons due to a spectrum of whistler modes is presented. The parametric dependence of the diffusion coefficients on the plasma particle density, magnitude of wave field, and the strength of magnetic field is studies. It is shown that significant pitch angle diffusion occurs for the Earth radiation belt electrons with energies from a few keV up to a few MeV.

Khazanov, G. V.↗

A Data-driven, Physics-based Transport Model of Solar Energetic Particles Accelerated by Coronal Mass Ejection Shocks Propagating through the Solar Coronal and Heliospheric Magnetic Fields

In an effort to develop computational tools for predicting radiation hazards from solar energetic particles (SEPs), we have created a data-driven physics-based particle transport model to calculate the injection, acceleration, and propagation of SEPs from coronal mass ejection (CME) shocks traversing through the solar corona and interplanetary magnetic fields. The model runs on an input of corona and heliospheric plasma and magnetic field configuration from a magnetohydrodynamic model driven by solar photospheric magnetic field measurements superposed with observed CME shocks determined from coronagraph images. SEP source particles are injected at the shock using the result of diffusive shock acceleration formulation from a characteristic obliquity-dependent injection from a heated solar wind thermal tail population. With several advanced computation techniques involving stochastic simulation and integration, the model obtains the particle intensity at any location in interplanetary space through the rigorous solution to the time-dependent 5D focus transport equation in the phase space that includes perpendicular diffusion. We apply the model to the 2011 November 3 CME event. The calculation results reproduce multispacecraft SEP observations at Earth and STEREO-B reasonably well without normalization of particle flux. The observations at STEREO-A can be reproduced by rescaling particle energy or modified energy dependence of particle diffusion coefficients. This circumsolar SEP event seen by spacecraft at Earth, STEREO-A, and STEREO-B at widely separated longitudes can be explained by diffusive shock acceleration by a single CME shock with a moderate speed.

Solar energetic particles↗

Molecular-level insights into structure and dynamics in ionic liquids and polymer gel electrolytes

We report designing new electrolytes requires a better understanding of the correlation between their transport properties and their molecular structure. In this work, we present a detailed study of ionic liquids and polymer gel electrolytes probing their structure and dynamics by nuclear magnetic resonance (NMR) spectroscopy. In particular, ammonium- and phosphonium-based ionic liquids (ILs) are combined with different LiTFSI concentrations, and then with different ratios of poly(methylmethacrylate) polymer. The temperature dependence of self-diffusion coefficients of mobile species, D Li+ , D TFSI- and D P4441+ or D N4441+ , measured by pulsed field gradient (PFG) NMR spectroscopy obeys the Arrhenius equation. Diffusivity of [P4441][TFSI] ILs is found to be greater than those of the [N4441][TFSI] ILs in both liquid and gel electrolytes. Solid state NMR experiments including 13 C and 19 F MAS, 13 C{ 19 F}, 13 C{ 1 H} CPMAS probe the local structure and molecular-level interactions between ions and polymer in gel electrolytes, particularly for samples with higher PMMA content (≥25 wt%). Finally, the fast field cycling relaxometry has been used to unveil the rotational and translational dynamics of P4441 + or N4441 + and TFSI - by measuring 1 H and 19 F R 1 relaxation rate profiles at different temperatures. A comprehensive NMR analysis including relaxation studies at low magnetic field provides decisive new insights regarding the formation of ionic clusters and the interaction of ions with the polymer chain in the case of the gel electrolytes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Influences of Hydrogen Bonding-Based Stabilization of Bolaamphiphile Layers on Molecular Diffusion within Organic Nanotubes Having Inner Carboxyl Groups

This paper reports molecular diffusion behavior in two bolaamphiphile-based organic nanotubes having inner carboxyl groups with different inner dimeters (10 and 20 nm) and wall structures, COOH-ONT 10nm and COOH-ONT 20nm , using imaging fluorescence correlation spectroscopy (imaging FCS). Here, the results were compared to those previously obtained in a similar nanotube with inner amine groups (NH 2 -ONT 10nm ). COOH-ONT 10nm , as with NH 2 -ONT 10nm , were formed from a rolled bolaamphiphile layer incorporating triglycine moieties, whereas COOH-ONT 20nm consisted of four stacks of triglycine-free bolaamphiphile layers. Imaging FCS measurements were carried out for anionic sulforhodamine B (SRB), zwitterionic/cationic rhodamine B (RB) and cationic rhodamine-123 (R123) diffusing within ONTs (1–9 µm long) at different pH (3.4–8.4) and ionic strengths (1.6–500 mM). Diffusion coefficients (D) of these dyes in the ONTs were very small (0.01–0.1 µm 2 /s), reflecting the significant contributions of molecule-nanotube interactions to diffusion. The D of SRB was larger at higher pH and ionic strength, indicating the essential role of electrostatic repulsion that was enhanced by the deprotonation of the inner carboxyl groups. Importantly, the D of SRB was virtually independent of nanotube inner diameter and wall structure, indicating the diffusion of the hydrophilic molecule was controlled by short timescale adsorption/desorption processes onto the inner surface. In contrast, pH effects on D were less clear for relatively hydrophobic R123 and RB, suggesting the significant contributions of non-Coulombic interactions. Interestingly, the diffusion of these molecules in COOH-ONT 20nm was slower than in COOH-ONT 10nm . Slower diffusion in COOH-ONT20nm was attributable to relatively efficient partitioning of the hydrophobic dyes into the bolaamphiphile layers, which was reduced in COOH-ONT 10nm due to the stabilization of its layer by polyglycine-II-type hydrogen bonding networks. These results show that, by tuning the bolaamphiphile structures and their intermolecular interactions, unique environments can be created within the nanospaces for enhanced molecular separations and reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Correlating Solvation Free Energy to Electrolyte Properties for Lithium Metal Batteries

The electrolyte plays a critical role in lithium metal batteries. In particular, ion solvation profoundly impacts key electrolyte properties and battery performance. Here, in this study, we systematically investigate solvation-property relationships in a series of electrolytes with different solvent-diluent ratios. Through potentiometric techniques that measure the relative solvation free energies of electrolytes, we find that weaker solvation correlates with larger ion clusters, lower ionic conductivity and diffusion coefficient, and superior electrochemical stability. Weaker solvation leads to the formation of a small number of Li clusters with large hydrodynamic radii, which lowers the Li + diffusivity and ionic conductivity of the electrolyte. Concurrently, weaker solvation leads to improved electrochemical stability at both the cathode and anode interfaces. Understanding these solvation-property relationships and trade-offs is important to designing electrolytes for optimized lithium metal battery performance.

25 ENERGY STORAGE↗

Solar modulation of galactic cosmic rays. 3: Implications of the Compton-Getting coefficient

Spectra of modulated galactic cosmic rays are expressed in terms of the Compton-Getting coefficient C. This parameter can reveal the energy range over which the force field approximation is valid, and the range where convection effects dominate those of diffusion. A value of C near zero over an extended low energy range implies that the radial gradient at low energies can not be large. This small gradient may imply that the diffusion coefficient increases beyond 1 AU less rapidly than proportionally to heliocentric radial distance, and/or there is essentially no scattering for a sizeable distance from the Sun to earth. The behavior of C with rigidity (or energy) is discussed in terms of the omnidirectional distribution function f sub zero. Contours of constant f sub zero in the heliocentric distance vs rigidity plane are useful for illustrating the mean rigidity loss experienced by cosmic rays in the interplanetary medium.

Fisk, L. A.↗

A study of equatorial inner belt protons from 2 to 200 MeV

The diffusion theory of inner belt protons is extended to lower energies for comparison with the data of Hovestadt et al. The effects of Coulomb energy loss, nuclear inelastic scattering, and the secular decrease of the earth's magnetic field are included. The Farley and Walt solar cycle averaged atmosphere and a neutron source based on the most recent measurements are used. It is found that diffusion theory can account for the observed flux of low-energy protons provided that the diffusion coefficient increases at smaller values of the first invariant. This result is interpreted as additional evidence for the importance of electrostatic field fluctuations in causing radial diffusion.

Claflin, E. S.↗

Radial diffusion in Saturn's radiation belts - A modeling analysis assuming satellite and ring E absorption

A modeling analysis is carried out of six experimental phase space density profiles for nearly equatorially mirroring protons using methods based on the approach of Thomsen et al. (1977). The form of the time-averaged radial diffusion coefficient D(L) that gives an optimal fit to the experimental profiles is determined under the assumption that simple satellite plus Ring E absorption of inwardly diffusing particles and steady-state radial diffusion are the dominant physical processes affecting the proton data in the L range that is modeled. An extension of the single-satellite model employed by Thomsen et al. to a model that includes multisatellite and ring absorption is described, and the procedures adopted for estimating characteristic satellite and ring absorption times are defined. The results obtained in applying three representative solid-body absorption models to evaluate D(L) in the range where L is between 4 and 16 are reported, and a study is made of the sensitivity of the preferred amplitude and L dependence for D(L) to the assumed model parameters. The inferred form of D(L) is then compared with that which would be predicted if various proposed physical mechanisms for driving magnetospheric radial diffusion are operative at Saturn.

Hood, L. L.↗

A Guideline to Mitigate Interfacial Degradation Processes in Solid‐State Batteries Caused by Cross Diffusion

Abstract Diffusion of transition metals across the cathode–electrolyte interface is identified as a key challenge for the practical realization of solid‐state batteries. This is related to the formation of highly resistive interphases impeding the charge transport across the materials. Herein, the hypothesis that formation of interphases is associated with the incorporation of Co into the Li 7 La 3 Zr 2 O 12 lattice representing the starting point of a cascade of degradation processes is investigated. It is shown that Co incorporates into the garnet structure preferably four‐fold coordinated as Co 2+ or Co 3+ depending on oxygen fugacity. The solubility limit of Co is determined to be around 0.16 per formula unit, whereby concentrations beyond this limit causes a cubic‐to‐tetragonal phase transition. Moreover, the temperature‐dependent Co diffusion coefficient is determined, for example, D 700 °C = 9.46 × 10 −14 cm 2 s −1 and an activation energy E a = 1.65 eV, suggesting that detrimental cross diffusion will take place at any relevant process condition. Additionally, the optimal protective Al 2 O 3 coating thickness for relevant temperatures is studied, which allows to create a process diagram to mitigate any degradation with a minimum compromise on electrochemical performance. This study provides a tool to optimize processing conditions toward developing high energy density solid‐state batteries.

Chemistry↗

Ionic Liquid–Directed Nanoporous TiNb 2 O 7 Anodes with Superior Performance for Fast–Rechargeable Lithium–Ion Batteries

Nanoporous TiNb 2 O 7 (NPTNO) material is synthesized by a sol–gel method with an ionic liquid (IL) as the nanoporous structure directing template. NPTNO exhibits a high reversible capacity of 210 mAh g –1 even at the charging rate of 50 C and an excellent cyclability of half-cell capacity retention of 74% for 1000 cycles at 5 C and LiNi 0.5 Mn 1.5 O 4 -coupled full-cell capacity retentions of 81% and 87% for 1000 cycles at 1 C and 2 C, respectively. The studies of the 1000 cycled NPTNO electrode illustrate that the IL-directed mesoporous structure can enhance the cyclability of NPTNO cells due to the alleviation of repetitive mechanical stress and volume fluctuation induced by the repetitive Li + insertion-extraction processes. The measured Li + diffusion coefficients from the galvanostatic intermittent titration technique suggest that the IL-templating strategy indeed ensures the fast rechargeability of NPTNO cells based on the fast Li + diffusion kinetics. Benefitting from the nanoporous structure, NPTNO with unhindered Li + diffusion pathways achieves a superior rate capability in the titanium-based oxide materials and the best full-cell cyclability in the TNO materials. Furthermore, the templating potential of IL is demonstrated, and the superb electrochemical performance establishes the IL-directed NPTNO as a promising anode candidate for fast-rechargeable LIBs.

25 ENERGY STORAGE↗

Resolving atomic transport through iron oxide under irradiation using isotopic tracers

Structural materials in nuclear environments are exposed to complex and harsh conditions, including high temperatures, corrosive solutions, and irradiation. Material stability and likewise degradation are fundamentally controlled by atomic transport mechanisms. Here, we investigate the influence of radiation-induced, non-equilibrium point defect populations on mass transport within model oxide systems using isotopic tracers and atom probe tomography. An isotopically labelled hematite (a-Fe2O3) film was synthesized with 16O- and 18O-rich layers (>30nm and 10 nm, respectively) sequentially deposited via molecular beam epitaxy. One region of the film was proton irradiated to ~0.1 dpa at 450°C, and regions outside the beam spot provided a non-irradiated control of thermal annealing only. 3D APT was used to directly visualize the elemental and O-isotopic redistribution following both thermal and combined thermal and irradiation conditions. Complementary scanning transmission electron microscopy (STEM) was also employed to study the microstructural evolution. Error function fits of the 18O-concentration profiles enabled quantification of diffusion coefficients.

isotopic tracers, diffusion, proton irradiation, h↗