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At least 1,063 records · Page 59

Radar glory from buried craters on icy moons

Three ice-covered moons of Jupiter, in comparison with rocky planets and earth's moon, produce radar echoes of astounding strengths and bizarre polarizations. Scattering from buried craters can explain these and other anomalous properties of the echoes. The role of such craters is analogous to that of the water droplets that create the apparition known as 'the glory', the optically bright region surrounding an observer's shadow on a cloud. Both situations involve the electromagnetic phenomenon of total internal reflection at a dielectric interface, operating in a geometry that strongly favors exact backscattering. Dim surface craters are transformed into bright glory holes by being buried under somewhat denser material, thereby increasing the intensity of their echoes by factors of hundreds. The dielectric interface thus formed at the crater walls nicely accounts for the unusual polarizations of the echoes.

Eshleman, Von R.↗

Probing Dopant Redistribution, Phase Propagation, and Local Chemical Changes in the Synthesis of Layered Oxide Battery Cathodes

Achieving the targeted control of layered oxide properties calls for more fundamental studies to mechanistically probe their evolution during their synthesis. Herein, dopant distribution, phase propagation, and local chemical changes as well as their interplay in multielement-doped LiNiO 2 materials are investigated using spectroscopic, imaging, and scattering techniques. It is shown that dopants undergo dynamic redistribution in the Ni(OH) 2 host lattice at the early stage of calcination (below 300 °C). Such redistribution behavior exhibits strong dopant-dependent characteristics, allowing for targeted surface and bulk doping control. The Ni oxidation process exhibits depth-dependent characteristics and the most rapid Ni oxidation takes place between 300 and 700 °C. Using Ni oxidation state as the proxy for the phase transformation, the buildup of heterogenous phase propagation in the early stage of calcination is shown, especially along the radial direction of secondary particles. Furthermore, the radial heterogenous phase distribution gradually decreases upon completing the calcination. However, a high degree of mosaic-like heterogeneity may still be present in the final product, departing from the perfect layered oxide. Overall, the present study offers fundamental insights into manipulating multiscale materials properties during calcination for obtaining stable, high-energy layered oxide cathodes.

36 MATERIALS SCIENCE↗

Theoretical modeling of electron mobility in superfluid {sup 4}He

The Orsay-Trento bosonic density functional theory model is extended to include dissipation due to the viscous response of superfluid {sup 4}He present at finite temperatures. The viscous functional is derived from the Navier-Stokes equation by using the Madelung transformation and includes the contribution of interfacial viscous response present at the gas-liquid boundaries. This contribution was obtained by calibrating the model against the experimentally determined electron mobilities from 1.2 K to 2.1 K along the saturated vapor pressure line, where the viscous response is dominated by thermal rotons. The temperature dependence of ion mobility was calculated for several different solvation cavity sizes and the data are rationalized in the context of roton scattering and Stokes limited mobility models. Results are compared to the experimentally observed “exotic ion” data, which provides estimates for the corresponding bubble sizes in the liquid. Possible sources of such ions are briefly discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Pair-density waves, charge-density waves, and vortices in high- T c cuprates

A recent scanning tunneling microscopy (STM) experiment reports the observation of a charge-density wave (CDW) with a period of approximately 8a in the halo region surrounding the vortex core, in striking contrast to the approximately 4a period CDWs that are commonly observed in the cuprates. Inspired by this work, we study a model where a bidirectional pair-density wave (PDW) with period 8 is at play. This further divides into two classes: (1) where the PDW is a competing state of the d-wave superconductor and can exist only near the vortex core where the d-wave order is suppressed and (2) where the PDW is the primary order, the so-called “mother state” that persists with strong phase fluctuations to high temperature and high magnetic field and lies behind the pseudogap phenomenology. We study the charge-density wave structures near the vortex core in these models. We emphasize the importance of the phase winding of the d-wave order parameter. The PDW can be pinned by the vortex core due to this winding and become static. Furthermore, the period-8 CDW inherits the properties of this winding, which gives rise to a special feature of the Fourier transform peak, namely, it is split in certain directions. There is also a line of zeros in the inverse Fourier transform of filtered data. We propose that these are key experimental signatures that can distinguish between the PDW-driven scenario from the more mundane option that the period-8 CDW is primary. We discuss the pro's and con's of the options considered above. Lastly, we attempt to place the STM experiment in the broader context of pseudogap physics of underdoped cuprates and relate this observation to the unusual properties of x-ray scattering data on CDW carried out to very high magnetic field.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Stability of matrix equations arising in electromagnetics

Many problems in electromagnetics can be formulated as a Fredholm equation of the first kind. In these problems it is desired to determine some function f(x) from its integral transform g(y). Except for special cases for which an explicit inverse operator is known, the equation is usually discretized by the method of moments into a matrix equation Af = g, which is then solved on a computer. A method of calculating the sensitivity of the solution of Af = g due to errors in either the vector g or the matrix A is developed. The usefulness of this method is demonstrated with problems from antenna theory, scattering theory, and remote sensing.

Klein, C.↗

Consistent Pl Analysis of Aqueous Uranium-235 Critical Assemblies

The lethargy-dependent equations of the consistent Pl approximation to the Boltzmann transport equation for slowing down neutrons have been used as the basis of an IBM 704 computer program. Some of the effects included are (1) linearly anisotropic center of mass elastic scattering, (2) heavy element inelastic scattering based on the evaporation model of the nucleus, and (3) optional variation of the buckling with lethargy. The microscopic cross-section data developed for this program covered 473 lethargy points from lethargy u = 0 (10 Mev) to u = 19.8 (0.025 ev). The value of the fission neutron age in water calculated here is 26.5 square centimeters; this value is to be compared with the recent experimental value given as 27.86 square centimeters. The Fourier transform of the slowing-down kernel for water to indium resonance energy calculated here compared well with the Fourier transform of the kernel for water as measured by Hill, Roberts, and Fitch. This method of calculation has been applied to uranyl fluoride - water solution critical assemblies. Theoretical results established for both unreflected and fully reflected critical assemblies have been compared with available experimental data. The theoretical buckling curve derived as a function of the hydrogen to uranium-235 atom concentration for an energy-independent extrapolation distance was successful in predicting the critical heights of various unreflected cylindrical assemblies. The critical dimensions of fully water-reflected cylindrical assemblies were reasonably well predicted using the theoretical buckling curve and reflector savings for equivalent spherical assemblies.

Fieno, Daniel↗

Properties of echo spectra observed by MST radars

Turbulent scatter and Fresnel reflection are the fundamental echoing mechanisms to interpret the signals observed by Mesosphere-stratosphere-troposphere (MST) radars. Turbulent scattered echoes provide information about the turbulence structure and mean flow of the atmosphere. Observational results with VHF MST radars, however, show the importance of Fresnel reflection due to the infinite gradient of reflectivity at the edges of a scattering layer. This condition is excluded for the weak fluctuation models but it is still possible to include the observed aspect sensitivity by assuming an anisotropic structure of fluctuations. Another explanation of the aspect sensitivity observed by MST radars is advanced. Spectral estimates by the widely used periodogram were related to a four-dimensional spectrum of atmospheric fluctuations with anisotropic structure. Effects of the radar system such as antenna beam width, beam direction and Fast Fourier Transformations (FFT) data length were discussed for the anisotropic turbulent atmosphere. Echo parameters were also estimated.

Wakasugi, K.↗

Transient scattering from two-dimensional dielectric cylinders of arbitrary shape

In this work, the problem of transient scattering by arbitrary shaped two-dimensional dielectric cylinders is solved using the marching-on-in-time (MOT) technique. The dielectric problem is approached via the surface equivalence principle. A pair of coupled integral equations are derived by enforcing the continuity of the electric and magnetic fields which are solved by using the method of moments. Numerical results are presented for two cross sections, viz. a circle and a square, and compared with inverse discrete Fourier transform (IDFT) techniques. In each case, good agreement is obtained with the IDFT solution.

Vechinski, Douglas A.↗

Temperature controlled transformations of giant unilamellar vesicles of amphiphilic triblock copolymers synthesized via microfluidic mixing

We report on a simple approach for synthesis of temperature-responsive giant unilamellar vesicles (GUVs) from poly(N-vinylcaprolactam) 15 -block-poly(dimethylsiloxane) 65 -block-poly(N-vinylcaprolactam) 15 (PVCL 15 -PDMS65-PVCL 15 ) triblock copolymer and non-temperature responsive small and giant vesicles from novel poly(N-vinylpyrrolidone)-block-poly(dimethylsiloxane)-block-poly(N-vinylpyrrolidone) (PVPON 15 -PDMS 65 -PVPON 15 and PVPON 6- PDMS 30- PVPON 6 ) triblock copolymers using microfluidic mixing at 25 °C. We show that temperature-responsive PVCL 15 -PDMS 65- PVCL 15 GUVs with the average diameter of 1.4 ± 0.2 µm while being stable at room temperature for at least 14 days, transformed irreversibly into small vesicles of 168 ± 40 nm after incubation of their aqueous solution at 42 °C for 24 h. We hypothesized that this transformation is induced by local compressive stresses of the vesicle membrane due to the collapse of PVCL blocks above the copolymer lower critical solution temperature (LCST) leading to the decrease of the vesicle membrane thickness. Consequently, we found that the temperature-induced size transformation of the PVCL-based GUVs at 42°C can be suppressed by substituting PVCL with its hydrophilic homologue PVPON, or by suppressing the PVCL's LCST behavior through hydrogen-bonding with tannic acid molecules. In the former case, novel PVPON n -PDMS m -PVPON n triblock copolymers (n = 15, m = 65 and n = 6, m = 30) assemble into vesicles stable from 25 °C to 55 °C as confirmed by optical and electron microscopy, dynamic light scattering (DLS) and small-angle neutron scattering (SANS). In the latter, hydrogen bonding interactions of PVCL with the polyphenol tannic acid (TA) at room temperature resulted in stable PVCL-based GUVs at 42°C as confirmed by optical, electron, and atomic force microscopies. We also found that physical crosslinking of the PVCL corona through hydrogen bonding with TA in PVCL 15- PDMS 65- PVCL 15 GUVs will delay their low pH-induced degradation at 37°C by 48 h compared to non-modified GUVs. Our findings open opportunities for the development of temperature-regulated stable micro-vehicles that would change their structural characteristics in the physiologically relevant temperature range from 25 to 42°C and can be utilized for cell mimicking studies. The developed GUVs also have potential in theranostic drug delivery as substitutes for polymer microcapsules and lipid microbubbles as well as for stimuli-triggered sensing, protection, and rapid response in an aqueous environment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Tuning the Electrocatalytic Oxygen Reduction Reaction Activity of PtCo Nanocrystals by Cobalt Concentration with Atomic-Scale Understanding

The development of a suitable catalyst for the oxygen reduction reaction (ORR) – the cathode reaction of proton exchange membrane fuel cells (PEMFC) – is necessary to push this technology towards widespread adoption. There have been substantial efforts to utilize bimetallic Pt-M alloys that adopt the ordered face-centered tetragonal (L10) phase in order to reduce the usage of precious metal, enhance the ORR performance, and improve catalyst stability. In this work, monodisperse Pt-Co nanocrystals (NCs) with well-defined size (4-5 nm) and cobalt composition (25-75 at%) were synthesized via colloidal synthesis. The transformation from the chemically disordered A1 (face-centered cubic, fcc) to the L10 phase was achieved via thermal annealing using both a conventional oven and a rapid thermal annealing process. The structure of the Pt-Co catalysts was characterized by a variety of techniques, including transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy in high-angle annular dark-field scanning transmission electron microscopy (STEM-EDS), small-angle X-ray scattering (SAXS), X-ray diffraction (XRD), and inductively coupled plasma-optical emission spectrometry (ICP-OES). The effects of annealing temperature on the composition-dependent degree of ordering, and subsequent effect on ORR activity is described. This work provides insights regarding the optimal spatial distribution of elements at the atomic level to achieve enhanced ORR activity and stability.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Unexpected compositional and structural modification of CoPt 3 nanoparticles by extensive surface purification

We combined synchrotron small angle X-ray scattering, X-ray fluorescence and extended X-ray absorption fine structure spectroscopy to probe the structure of chemically synthesized CoPt 3 nanoparticles (NPs) after ligand removal via the commonly accepted solvent/nonsolvent approach. We showed that the improved catalytic activity of extensively purified NPs could not be explained only in terms of a “cleaner” surface. We found that extensive surface purification results in the substantial leaching of the Co atoms from the chemically synthesized CoPt 3 NPs transforming them into CoPt 3 /Pt core/shell structures with an unexpectedly thick (~0.5 nm) Pt shell. We indicated that the improved catalytic activity of extensively purified NPs in octyne hydrogenation reaction can be explained by the formation of CoPt 3 /Pt core/shell structures. Also, we demonstrated that drastic compositional and structural transformation of water transferred CoPt 3 NPs was rather a result of extensive removal of native ligands via a solvent/nonsolvent approach than leaching of cobalt atoms in aqueous media. We expect that these findings can be relevant to other transition metal based multicomponent NPs.

36 MATERIALS SCIENCE↗

Influence of Charge Block Length on Conformation and Solution Behavior of Polyampholytes

In this paper, we investigate the effect of charge block length on polyampholyte chain conformation and phase behavior using small-angle X-ray scattering (SAXS) and implicit-solvent molecular simulations. To this end, we use solid phase peptide synthesis to precision-tailor a series of polyampholytes consisting of l-glutamic acid (E) and l-lysine (K) monomers arranged in alternating blocks from 2 to 16 monomers. We observe that the polyampholytes tend to phase separate as block size increases. With addition of NaCl, phase separated polyampholytes exhibit a salting-in effect dependent on charge block length. Fourier-transform infrared (FTIR) spectroscopy reveals the presence of intramolecular hydrogen bonds that are disrupted upon the addition of NaCl, implicating both electrostatic interactions and hydrogen bonding in the phase behavior. SAXS spectra at no-added salt conditions show minimal dependence of charge block length on the radius of gyration (R g ) for soluble polyampholytes, but local chain stiffening is found to be dependent on charge block length. With increasing NaCl, consistent with electrostatic screening, all polyampholytes expand and behave as neutral or swollen chains in good solvent conditions. Molecular simulations are qualitatively consistent with experiments. Implications for understanding intracellular condensates and material design are noted.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Digital Speckle Photography of Subpixel Displacements of Speckle Structures Based on Analysis of Their Spatial Spectra

We have investigated the capabilities of the method of digital speckle interferometry for determining subpixel displacements of a speckle structure formed by a displaceable or deformable object with a scattering surface. An analysis of spatial spectra of speckle structures makes it possible to perform measurements with a subpixel accuracy and to extend the lower boundary of the range of measurements of displacements of speckle structures to the range of subpixel values. The method is realized on the basis of digital recording of the images of undisplaced and displaced speckle structures, their spatial frequency analysis using numerically specified constant phase shifts, and correlation analysis of spatial spectra of speckle structures. Transformation into the frequency range makes it possible to obtain quantities to be measured with a subpixel accuracy from the shift of the interference-pattern minimum in the diffraction halo by introducing an additional phase shift into the complex spatial spectrum of the speckle structure or from the slope of the linear plot of the function of accumulated phase difference in the field of the complex spatial spectrum of the displaced speckle structure. The capabilities of the method have been investigated in natural experiment.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Bessel Weighted Asymmetries

We review the concept of Bessel weighted asymmetries for semi-inclusive deep inelastic scattering and focus on the cross section in Fourier space, conjugate to the outgoing hadron’s transverse momentum, where convolutions of transverse momentum dependent parton distribution functions and fragmentation functions become simple products. Individual asymmetric terms in the cross section can be projected out by means of a generalized set of weights involving Bessel functions. The procedure is applied to studies of the double longitudinal spin asymmetry in semi-inclusive deep inelastic scattering using a new dedicated Monte Carlo generator which includes quark intrinsic transverse momentum within the generalized parton model. We observe a few percent systematic offset of the Bessel-weighted asymmetry obtained from Monte Carlo extraction compared to input model calculations, which is due to the limitations imposed by the energy and momentum conservation at the given energy and hard scale Q2. We find that the Bessel weighting technique provides a powerful and reliable tool to study the Fourier transform of TMDs with controlled systematics due to experimental acceptances and resolutions with different TMD model inputs.

Avakian, Harut↗

Ultrabroadband THz conductivity of gated graphene in- and out-of-equilibrium

We employ ultrabroadband terahertz (THz) spectroscopy to expose the high-frequency transport properties of Dirac fermions in monolayer graphene. By controlling the carrier concentration via tunable electrical gating, both equilibrium and transient optical conductivities are obtained for a range of Fermi levels. The frequency-dependent equilibrium response is determined through a combination of time-domain THz and Fourier-transform infrared spectroscopy for energies up to the near-infrared, which also provides a measure of the gate-voltage dependent Fermi level. Transient changes in the real and imaginary parts of the graphene conductivity are electro-optically resolved for frequencies up to 15 THz after near-infrared femtosecond excitation, both at the charge-neutral point and for higher electrostatic-doping levels. Modeling of the THz response provides insight into changes of the carrier spectral weights and scattering rates, and reveals an additional broad-frequency ($$\approx$$ 8 THz) component to the photo-induced response, which we attribute to the zero-momentum mode of quantum-critical transport observed here in large-area CVD graphene.

Coslovich, G↗

Evaluating the De Hoffmann-Teller Cross-Shock 2 Potential at Real Collisionless Shocks

Shock waves are common in the heliosphere and beyond. The collisionless nature of most astrophysical plasmas allows for the energy processed by shocks to be partitioned amongst particle sub-populations and electromagnetic fields via physical mechanisms that are not well understood. The electrostatic potential across such shocks is frame dependent. In a frame where the incident bulk velocity is parallel to the magnetic field, the deHoffmann-Teller frame, the potential is linked directly to the ambipolar electric field established by the electron pressure gradient. Thus measuring and understanding this potential solves the electron partition problem, and gives insight into other competing shock processes. Integrating measured electric fields in space is problematic since the measurements can have offsets that change with plasma conditions. The offsets, once integrated, can be as large or larger than the shock potential. Here we exploit the high-quality field and plasma measurements from NASA’s Magnetospheric Multiscale mission to attempt this calculation. We investigate recent adaptations of the deHoffmann-Teller frame transformation to include time variability, and conclude that in practice these face difficulties inherent in the 3D time-dependent nature of real shocks by comparison to 1D simulations. Potential estimates based on electron fluid and kinetic analyses provide the most robust measures of the deHoffmann-Teller potential, but with some care direct integration of the electric fields can be made to agree. These results suggest that it will be difficult to independently assess the role of other processes, such as scattering by shock turbulence, in accounting for the electron heating.

Steven J Schwartz↗

Requirements and sensitivity analysis for temporally- and spatially-resolved thermometry using neutron resonance spectroscopy

Neutron resonance spectroscopy (NRS) has been used extensively to make temperature measurements that are accurate, absolute, and nonperturbative within the interior of material samples under extreme conditions applied quasistatically. Yet NRS has seldom been used in dynamic experiments. There is a compelling incentive to do so because of the significant shortcomings of alternative techniques. An important barrier to adopting dynamic NRS thermometry is the difficulty in fielding it with conventional spallation neutron sources. To enable time-dependent and spatially resolved temperature measurements in dynamic environments, more compact neutron sources that can be used at user facilities in conjunction with other diagnostic probes (such as x-ray light sources) are required. Such sources may be available using ultrafast high-intensity optical lasers. We evaluate such possibilities by determining the sensitivities of the temperature estimate on neutron-beam and diagnostic parameters. Based on that evaluation, requirements are set on a pulsed neutron-source and diagnostics to make a meaningful dynamic temperature measurement. Dynamic thermometry measurements are examined in this context when driven by two alternative fast-neutron sources: the Los Alamos Neutron Scattering Center (LANSCE) proton accelerator driving isotropic spallation neutrons as a baseline and a laser-plasma ion accelerator driving a neutron beam from deuterium breakup. Strategies to close the gap between the required and demonstrated performance of laser-based fast-neutron sources are presented. A short-pulse high-intensity laser with state-of-the-art pulse contrast and an energy of a few hundred Joules would drive a compact neutron source suitable for NRS thermometry that could transform the dynamic study of materials.

47 OTHER INSTRUMENTATION↗