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At least 1,279 records · Page 71

Assembly of Building Blocks by Double-End-Anchored Polymers in the Dilute Regime Mediated by Hydrophobic Interactions at Controlled Distances

Hierarchical assembly of building blocks via competing, orthogonal interactions is a hallmark of many of nature’s composite materials that do not require highly specific ligand-receptor interactions. To mimic this assembly mechanism requires the development of building blocks capable of tunable interactions. In the present work, we explored the interplay between repulsive (steric and electrostatic) and attractive hydrophobic forces. The designed building blocks allow hydrophobic forces to effectively act at controlled, large distances, to create and tune the assembly of membrane-based building blocks under dilute conditions and affect their interactions with cellular membranes via physical cross-bridges. Specifically, we employed double-end-anchored poly(ethylene glycol)s (DEA-PEGs)—hydrophilic PEG tethers with hydrophobic tails on both ends. Using differential-interference-contrast optical microscopy, synchrotron small angle X-ray scattering (SAXS), and cryogenic electron microscopy, we investigated the ability of DEA-PEGs to mediate assembly in the dilute regime on multiple length scales and on practical time scales. The PEG length, anchor hydrophobicity, and molar fraction of DEA-PEG molecules within a membrane strongly affect the assembly properties. Additional tuning of the intermembrane interactions can be achieved by adding repulsive interactions via PEG-lipids (steric) or cationic lipids to the DEA-PEG-mediated attractions. Further, while the optical and electron microscope imaging methods provided qualitative evidence of the ability of DEA-PEGs to assemble liposomes, the SAXS measurements and quantitative line-shape analysis in dilute preparations demonstrated that the ensemble average of loosely organized liposomal assemblies maintains DEA-PEG concentration-dependent tethering on defined nanometer length scales. For cationic liposome–DNA nanoparticles (CL–DNA NPs), aggregation induced by DEA-PEGs decreased internalization of NPs by cells, but tuning the DEA-PEG-induced attractions by adding repulsive steric interactions via PEG-lipids limited aggregation and increased NP uptake. However, confocal microscopy imaging together with colocalization studies with Rab11 and LysoTracker as markers of intracellular pathways showed that modifying CL–DNA NPs with DEA-PEGs alters their interactions with the plasma and endosomal membranes.

- x-ray scattering↗

Milky Way white dwarfs as sub-GeV to multi-TeV dark matter detectors

Here, we show that Milky Way white dwarfs are excellent targets for dark matter (DM) detection. Using Fermi and H.E.S.S. Galactic center gamma-ray data, we investigate sensitivity to DM annihilating within white dwarfs into long-lived or boosted mediators and producing detectable gamma rays. Depending on the Galactic DM distribution, we set new constraints on the spin-independent scattering cross section down to 10 -45 -10 -41 cm 2 in the sub-GeV DM mass range, which is multiple orders of magnitude stronger than existing limits. For a generalized NFW DM profile, we find that our white dwarf constraints exceed spin-independent direct detection limits across most of the sub-GeV to multi-TeV DM mass range, achieving sensitivities as low as about 10 -46 cm 2 . In addition, we improve earlier versions of the DM capture calculation in white dwarfs, by including the low-temperature distribution of nuclei when the white dwarf approaches crystallization. This yields smaller capture rates than previously calculated by a factor of a few up to two orders of magnitude, depending on white dwarf size and the astrophysical system.

79 ASTRONOMY AND ASTROPHYSICS↗

Modelling the effects of turbulence on acoustic wave propagation

A review of recent theoretical modeling of the effects of turbulence on acoustic wave propagation is presented. The Born approximation limit of the smoothing method of Keller and of the kinetic theory method of Howe are compared with the classical perturbation results of Chernov. Secular growth is observed in the higher order terms of the kinetic theory method of Howe when multiple scaling is ignored. The forward propagation - beam broadening model of Brown and Clifford is discussed as well as the single scatter model of DeLoach and of Rudd. Each model is examined with respect to its prediction of conservation of energy.

Harris, W. L.↗

Quantum mechanical theory of a structured atom-diatom collision system - A + BC/1-Sigma/

The problem of a 2-p state atom colliding with a singlet sigma state diatom, which involves multiple potential surfaces, is investigated. Within a diabatic representation for the electronic degrees of freedom (plus spin-orbit interaction), coupled scattering equations are derived in both space-fixed and body-fixed coordinate systems. Coefficients, analogous to Percival-Seaton coefficients, are obtained. Approximations to the exact equations, including angular momenta decoupling approximations, are discussed for both the space-fixed and body-fixed formalisms.

Devries, P. L.↗

Prospects for altimetry and scatterometry in the 90's

Current NASA plans for altimetry and scatterometry of the oceans using spaceborne instrumentation are outlined. The data of interest covers geostrophic and wind-driven circulation, heat content, the horizontal heat flux of the ocean, and the interactions between atmosphere and ocean and ocean and climate. A proposed TOPEX satellite is to be launched in 1991, carrying a radar altimeter to measure the ocean surface topography. Employing dual-wavelength operation would furnish ionospheric correction data. Multibeam instruments could also be flown on the multiple-instrument polar orbiting platforms comprising the Earth Observation System. A microwave radar scatterometer, which functions on the basis of Bragg scattering of microwave energy off of wavelets, would operate at various view angles and furnish wind speeds accurate to 1.5 m/sec and directions accurate to 20 deg.

Townsend, W. F.↗

Effects of Inlet Flow Conditions on Crossflow Jet Mixing

An experimental investigation of the effects of mainstream turbulence, mainstream swirl and non-symmetric mass addition has been conducted for the isothermal mixing of multiple jets injected into a confined rectangular crossflow. Jet penetration and mixing in the near field was studied using planar Mie scattering to measure time-averaged mixture fraction distributions. Orifice configurations were used that were optimized for mixing performance based on previous experimental and computational results for a homogeneous approach flow. Mixing effectiveness, determined using a spatial unmixedness parameter based on the variance of the mean jet concentration distributions, was found to be minimally affected by free-stream turbulence but significantly influenced by the addition of swirl to the mainstream. The results for non-symmetric mass addition indicate that the concentration distribution of the flowfield can be tailored if desired.

Liscinsky, D. S.↗

Monitoring Delamination of Plasma-Sprayed Thermal Barrier Coatings by Reflectance-Enhanced Luminescence

Highly scattering plasma-sprayed thermal barrier coatings (TBCs) present a challenge for optical diagnostic methods to monitor TBC delamination because scattering attenuates light transmitted through the TBC and usually degrades contrast between attached and delaminated regions of the TBC. This paper presents a new approach where reflectance-enhanced luminescence from a luminescent sublayer incorporated along the bottom of the TBC is used to identify regions of TBC delamination. Because of the higher survival rate of luminescence reflecting off the back surface of a delaminated TBC, the strong scattering exhibited by plasma-sprayed TBCs actually accentuates contrast between attached and delaminated regions by making it more likely that multiple reflections of luminescence off the back surface occur before exiting the top surface of the TBC. A freestanding coating containing sections designed to model an attached or delaminated TBC was prepared by depositing a luminescent Eu-doped or Er-doped yttria-stabilized zirconia (YSZ) luminescent layer below a plasma-sprayed undoped YSZ layer and utilizing a NiCr backing layer to represent an attached substrate. For specimens with a Eu-doped YSZ luminescent sublayer, luminescence intensity maps showed excellent contrast between unbacked and NiCr-backed sections even at a plasma-sprayed overlayer thickness of 300 m. Discernable contrast between unbacked and NiCr-backed sections was not observed for specimens with a Er-doped YSZ luminescent sublayer because luminescence from Er impurities in the undoped YSZ layer overwhelmed luminescence originating form the Er-doped YSZ sublayer.

Eldridge, Jeffrey I.↗

Additive manufacturing of composite neutron absorbing components

Collimators and other components for use in neutron scattering experiments or to provide neutron shielding in nuclear reactors or accelerator based neutron sources are produced by additive manufacturing from multiple different types of material, such as boron carbide (B4C), steel, isotopically enriched boron carbide (10B4C), and blends thereof.

Anderson, David C.↗

Understanding and Manipulating Counterion Condensation within Charged Polymer Electrolytes for Selective and Low Resistant Membrane Separations

Polymeric ion-exchange membranes are found at the heart of numerous electrochemical systems spanning separations (electrodialysis and membrane capacitive deionization) and energy conversion and storage (flow batteries, fuel cells, and electrolyzers). The ion-exchange membrane separators need to be ion conducting but electron insulating, and in many scenarios selective for a particular ion to conduct. Because of their polymeric nature, the molecular architectures of ion-exchange membranes lack the molecular precision found in many inorganic materials. Plus, they contain numerous structural defects that impede ionic transport. As a result of their poor structure, it has been difficult to carefully probe the underlying physics that governs ion transport in ion-exchange membranes. We investigated counterion condensation phenomena in ion-exchange membranes and correlated it to bulk ionic charge transport and selectivity in precisely defined and long-range ordered materials afforded through the principles of directed self-assembly. A multi-faceted approach spanning i.) advanced metrology, two-dimensional atomic force microscopy, x-ray scattering, and ion-exchange equilibria, and ii.) molecular simulations (classical molecular dynamics and ab-inito molecular dynamics) that bridge multiple time and length scales, were employed to correlate the extent of counterion condensation to ionic conductivity and selectivity. After uncovering the extent of the condensation phenomena in this project, new macromolecular chemistries were employed to manipulate the ion pairing interactions of the condensed counterions to tethered ions on the polymer backbone so more facile and selective conduction rates can be attained. The research has aided in the rational design of polymeric ion-exchange membrane separators with high current density for electrochemical systems and subsequently better energy efficiency.

36 MATERIALS SCIENCE↗

Measurement of Inclusive Charged-Current $\barν_μ$ Scattering on C, CH, Fe, and Pb at $\langle E_{\barν}\rangle \sim$ 6 GeV with MINERvA

We report MINERvA's first measurement of inclusive charged-current $\barν_μ$ cross sections on carbon, hydrocarbon, iron, and lead, and their ratios to the cross section on hydrocarbon, as functions of the antimuon transverse momentum, $p_{\mathrm{T}}$. Using a wide-band $\barν_μ$ beam with mean energy $\sim 6~\text{GeV}$, these measurements probe all interaction modes, including the transition from resonance production to deep-inelastic scattering. The total uncertainties are typically $5-10\%$ for the absolute cross sections and $2-5\%$ for the ratios. Comparisons with multiple neutrino interaction models reveal significant discrepancies in the $p_{\mathrm{T}}$ dependence, particularly for heavier nuclei. The disagreements are most pronounced at low $p_{\mathrm{T}}$ but extend across the full $p_{\mathrm{T}}$ range, indicating missing or mis-modelled nuclear effects.

Klustová, A. [Imperial Coll., London] (ORCID:00000↗

Multiple experimental studies of pore structure and mineral grain sizes of the Woodford shale in southern Oklahoma, USA

Pore structure study is an important part of unconventional shale reservoir characterization, since the pore system provides the primary petroleum storage space and fluid flow pathways. Previous studies have suggested that the pore structure is related to the total organic carbon (TOC) content, mineral compositions, and the maturity of the organic matter (OM). However, few studies have focused on the mineral grains, the primary grains being deposited but before cementation, which are the building blocks of shale. Eight Woodford Shale outcrop samples from southern Oklahoma were chosen to study the effects of mineral grain size on the pore structure characterization, using multiple and complementary experimental approaches, including laser diffraction, mineralogy, TOC, pyrolysis, liquid immersion porosimetry, mercury intrusion porosimetry, gas physisorption, (ultra) small angle X-ray scattering, scanning electron microscopy, and spontaneous imbibition. The results from different experiments of eight samples show that the Woodford Shale has the mean mineral grain diameters at 3–6 μm, a wide range of porosity at 3–40% and pore diameters at 50–1,000 nm, and various pore connectivity. Grain size variation was probably caused by the sea-level fluctuation during its deposition, which affect the porosity, pore size distribution, and pore connectivity. With decreasing mineral grain sizes, the porosity tends to increase while the pore connectivity worsens. The results also indicate that OM and carbonates in this low-maturity Woodford Shale could block the pores and decrease the porosity. Coupling with the grain size analyses, the control of depositional environment on grain sizes and subsequent effects on pore structure is identified. The pore structure characteristics over a wide pore-diameter range provided by multiple experiments could improve the understanding of storage space and fluid flow in the Woodford Shale to further increase its petroleum production.

54 ENVIRONMENTAL SCIENCES↗

PtCoO 2 for Scaled Interconnects

Copper (Cu) interconnects are an increasingly important bottleneck in integrated circuits due to energy consumption and latency caused by the notable increase in Cu resistivity as dimensions decrease, primarily due to electron scattering at surfaces. Herein, the potential of a directional conductor, PtCoO 2 , which has a low bulk resistivity and a distinctive anisotropic structure that mitigates electron surface scattering is showcased. Thin films of PtCoO 2 of various thicknesses are synthesized by molecular beam epitaxy (MBE) coupled with a postdeposition annealing process and the superior quality of PtCoO 2 films is demonstrated by multiple characterization techniques. The thickness‐dependent resistivity curve illustrates that PtCoO 2 significantly outperforms effective Cu (Cu with TaN barriers) and Ru in resistivity below 20.0 nm with a more than 6x reduction compared to effective Cu below 6.0 nm, having a value of only 6.32 μΩ cm at 3.3 nm. It is determined that grain boundary scattering can still be improved for even lower resistivities in this material system through a combination of experiments and theoretical simulations. PtCoO 2 is therefore a highly promising alternative material for future interconnect technologies promising lower resistivities, better stability, and significant improvements in energy efficiency and latency for advanced integrated circuits.

Li, Yansong [Department of Electrical Engineering ↗

A global study of hygroscopicity-driven light-scattering enhancement in the context of other in situ aerosol optical properties

The scattering and backscattering enhancement factors (ƒ(RH) and ƒ b (RH)) describe how aerosol particle light scattering and backscattering, respectively, change with relative humidity (RH). They are important parameters in estimating direct aerosol radiative forcing (DARF). In this study we use the dataset presented in Burgos et al. (2019) that compiles ƒ(RH) and ƒ b (RH) measurements at three wavelengths (i.e., 450, 550 and 700 nm) performed with tandem nephelometer systems at multiple sites around the world. We present an overview of ƒ(RH) and ƒ b (RH) based on both long-term and campaign observations from 23 sites representing a range of aerosol types. The scattering enhancement shows a strong variability from site to site, with no clear pattern with respect to the total scattering coefficient. In general, higher ƒ(RH) is observed at Arctic and marine sites, while lower values are found at urban and desert sites, although a consistent pattern as a function of site type is not observed. The backscattering enhancement ƒ b (RH) is consistently lower than ƒ(RH) at all sites, with the difference between ƒ(RH) and ƒ b (RH) increasing for aerosol with higher ƒ(RH). This is consistent with Mie theory, which predicts higher enhancement of the light scattering in the forward than in the backward direction as the particle takes up water. Our results show that the scattering enhancement is higher for PM 1 than PM 10 at most sites, which is also supported by theory due to the change in scattering efficiency with the size parameter that relates particle size and the wavelength of incident light. At marine-influenced sites this difference is enhanced when coarse particles (likely sea salt) predominate. For most sites, ƒ(RH) is observed to increase with increasing wavelength, except at sites with a known dust influence where the spectral dependence of ƒ(RH) is found to be low or even exhibit the opposite pattern. The impact of RH on aerosol properties used to calculate radiative forcing (e.g., single-scattering albedo, ω 0 , and backscattered fraction, b) is evaluated. The single-scattering albedo generally increases with RH, while b decreases. The net effect of aerosol hygroscopicity on radiative forcing efficiency (RFE) is an increase in the absolute forcing effect (negative sign) by a factor of up to 4 at RH = 90 % compared to dry conditions (RH < 40 %). Because of the scarcity of scattering enhancement measurements, an attempt was made to use other more commonly available aerosol parameters (i.e., ω 0 and scattering Ångström exponent, α sp ) to parameterize ƒ(RH). The majority of sites (75 %) showed a consistent trend with ω 0 (higher ƒ(RH = 85 %) for higher ω 0 ), while no clear pattern was observed between ƒ(RH = 85 %) and αsp. This suggests that aerosol ω 0 is more promising than α sp as a surrogate for the scattering enhancement factor, although neither parameter is ideal. Nonetheless, the qualitative relationship observed between ω 0 and ƒ(RH) could serve as a constraint on global model simulations.

54 ENVIRONMENTAL SCIENCES↗

Constraints on Mars Aphelion Cloud Belt phase function and ice crystal geometries

This study constrains the lower bound of the scattering phase function of Martian water ice clouds (WICs) throughthe implementation of a new observation aboard the Mars Science Laboratory (MSL). The Phase Function SkySurvey (PFSS) was a multiple pointing all-sky observation taken with the navigation cameras (Navcam) aboardMSL. The PFSS was executed 35 times during the Aphelion Cloud Belt (ACB) season of Mars Year 34 over a solarlongitude range of Ls = 61:4 156:5. Twenty observations occurred in the morning hours between 06:00 and 09:30 LTST, and 15 runs occurred in the evening hours between 14:30 and 18:00 LTST, with an operationallyrequired 2.5 h gap on either side of local noon due the sun being located near zenith. The resultant WIC phasefunction was derived over an observed scattering angle range of 18.3-152.61, normalized, and compared with 9modeled phase functions: seven ice crystal habits and two Martian WIC phase functions currently being implementedin models. Through statistical chi-squared probability tests, the five most probable ice crystal geometriesobserved in the ACB WICs were aggregates, hexagonal solid columns, hollow columns, plates, and bullet rosetteswith p-values greater than or equal to 0.60, 0.57,0.56,0.56, and 0.55, respectively. Droxtals and spheres had pvaluesof 0.35, and 0.2, making them less probable components of Martian WICs, but still statistically possibleones. Having a better understanding of the ice crystal habit and phase function of Martian water ice cloudsdirectly benefits Martian climate models which currently assume spherical and cylindrical particles.

Cooper, Brittney↗

Effect of outer divertor leg detachment on the high field side scrape-off layer in DIII-D and ASDEX Upgrade

In this work, evidence is presented that detachment of the outer divertor leg leads to a reduction of electron density and neutral pressure in the high-field side (HFS) scrape-off layer (SOL) of the ASDEX Upgrade (AUG) and DIII-D tokamaks with ion $B$ x $∇B$ drift directed toward the X-point (favorable configuration). These results are observed across multiple diagnostics and without the use of impurity seeding to reach detachment. In AUG, outer divertor leg detachment correlates with a decrease in electron density near the separatrix at the inner midplane, measured with HFS reflectometry. A concurrent reduction in inner divertor density and neutral pressure at the inner target is observed using divertor Thomson scattering and neutral pressure gauges. These effects are present in both L- and H-mode plasmas. In DIII-D, a similar reduction is detected through analysis of line-integrated hydrogenic emission measured by multiple diagnostics in the HFS SOL close to the separatrix. The consistent trends in both devices indicate that high electron density and strong hydrogenic emissivity in the HFS SOL are common features of H-mode plasmas in the favorable configuration, independent of wall material and divertor geometry. In L-mode plasmas, the reduction in electron density and neutral pressure is not observed in DIII-D, possibly due to differences in wall material. These results emphasize the importance of the divertor state in determining the two-dimensional neutral distribution and edge fueling.

detachment↗

Nonequilibrium Thermodynamics of Colloidal Gold Nanocrystals Monitored by Ultrafast Electron Diffraction and Optical Scattering Microscopy

Metal nanocrystals exhibit important optoelectronic and photocatalytic functionalities in response to light. These dynamic energy conversion processes have been commonly studied by transient optical probes to date, but an understanding of the atomistic response following photoexcitation has remained elusive. In this paper, we use femtosecond resolution electron diffraction to investigate transient lattice responses in optically excited colloidal gold nanocrystals, revealing the effects of nanocrystal size and surface ligands on the electron–phonon coupling and thermal relaxation dynamics. First, we uncover a strong size effect on the electron–phonon coupling, which arises from reduced dielectric screening at the nanocrystal surfaces and prevails independent of the optical excitation mechanism (i.e., inter- and intraband). Second, we find that surface ligands act as a tuning parameter for hot carrier cooling. Particularly, gold nanocrystals with thiol-based ligands show significantly slower carrier cooling as compared to amine-based ligands under intraband optical excitation due to electronic coupling at the nanocrystal/ligand interfaces. Finally, we spatiotemporally resolve thermal transport and heat dissipation in photoexcited nanocrystal films by combining electron diffraction with stroboscopic elastic scattering microscopy. Taken together, we resolve the distinct thermal relaxation time scales ranging from 1 ps to 100 ns associated with the multiple interfaces through which heat flows at the nanoscale. Our findings provide insights into optimization of gold nanocrystals and their thin films for photocatalysis and thermoelectric applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Diurnal variation of thermal plasma in the plasmasphere

All of the OGO-5 light ion density measurements were used to determine the average global topology of the equatorial plasmasphere density distribution. The variation of the light ion equatorial density at L less than or equal to 3.2 with local time was deduced by determining the average density observed within one hour of a specific local time and within 0.1 of a given L coordinate. The average H(+) density showed a semidiurnal variation with peaks near noon and midnight. The He(+) observations also revealed multiple peaks throughout the day but with smaller amplitudes than those of H(+). At L above 3.2 plasma trough conditions increase the scatter of densities. The average variation of the H(+) density with L within the plasmasphere is found to be steepest near midnight and can be least-squares fitted equally well to either an exponential variation or to a power law.

Chen, A. J.↗

Improved Raman-Scattering Gas-Species Monitor

Improved Raman-scattering instrument provides real-time measurements of concentration of gas species of interest mixed with other gases. High efficiency achieved by multiple passes of laser beam, fast collection optics. Costs less, weighs less, and operates more easily. In original application, instrument used to determine whether flammable or explosive concentration of leaking hydrogen present in atmosphere that contains varying concentrations of helium, air, and possibly other gases in addition to hydrogen.

Adler-Golden, Steven↗