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At least 541 records · Page 30

Plasma sheath and presheath development near a partially reflective surface

This work addresses one-dimensional evolution of a collisionless plasma next to a solid surface that is immersed into the plasma instantaneously. In particular, we consider how the self-similar rarefaction wave establishes dynamically and how the electron reflection from the surface modifies the structure of the rarefaction wave and the Debye sheath. Here, we demonstrate that a sufficiently strong reflection eliminates the Debye sheath and changes the wall potential and the plasma flow parameters significantly. The paper presents numerical results that illustrate the developed analytical theory.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Near IR Scanning Angle Total Internal Reflection Raman Spectroscopy at Smooth Gold Films

Total internal reflection (TIR) Raman and reflectivity spectra were collected for nonresonant analytes as a function of incident angle at sapphire or sapphire/smooth 50 nm gold interfaces using 785 nm excitation. For both interfaces, the Raman signal as a function of incident angle is well-modeled by the calculated interfacial mean square electric field (MSEF) relative to the incident field times the thickness of the layer being probed in the Raman measurement (D{sub RS}). The Raman scatter was reproducibly enhanced at the interface containing a gold film relative to the sapphire interface by a factor of 4.3–4.6 for aqueous pyridine or 2.2–3.7 for neat nitrobenzene, depending on the analyzed vibrational mode. The mechanism for the increased Raman signal is the enhanced MSEF at incident angles where propagating surface plasmons are excited in the metal film. The background from the TIR prism was reduced by 89–95% with the addition of the gold film, and the percent relative uncertainty in peak area was reduced from 15 to 1.7% for the 1347 cm–1 mode of nitrobenzene. Single monolayers of benzenethiol (S/N = 6.8) and 4-mercaptopyridine (S/N = 16.5) on gold films were measured by TIR Raman spectroscopy with 785 nm excitation (210 mW) without resonant enhancement in 1 min.

36 MATERIALS SCIENCE↗

Langmuir Films of n -Alkanethiol-Capped Gold Nanoparticles and n -Alkanes: Interfacial Mixing Scenarios Assessed by X-ray Reflectivity and Grazing Incidence Diffraction

A series of n-alkanes cospread with alkanethiol-stabilized gold nanoparticles (AuNP) were studied as Langmuir monolayers by synchrotron X-ray reflectivity and diffraction. Tetradecanethiol capped gold nanoparticles with core diameters close to 2 nm were used to make films at 20 °C, below the ligand order–disorder temperature. A variety of n-alkane chain lengths (Cn = C n H 2n+2 , where n = 12, 15 and 16) were tested to assess the interfacial assembly of nanoparticle films as a result of different mixing scenarios indicated in their surface pressure versus area isotherms. Synchrotron grazing incidence X-ray diffraction (GIXD) and reflectivity (XR) confirm that mixtures of n-alkane and AuNP exhibiting improved fluidity in their compression isotherm are indeed incorporating n-alkane into the AuNP ligand shell and stabilizing it at the air–water interface. The resulting films show a doubling of their correlation lengths and thus a significant improvement on their ordering, as well as increased lattice spacing that is dependent upon the n-alkane chain length. Mixtures that do not exhibit changes in their surface pressure vs area isotherm similarly show little change in the interfacial assembly of the nanoparticle films except to promote monolayer collapse and multilayer formation. Improvements to the film order are assigned to the initial formation of larger nanoparticle domains. Here, the nature of the chain length dependence and persistence of the n-alkane through compression suggest a favorable interaction with the nanoparticle ligand shell that results in the extension of methylene units of the longer alkanes beyond the thiol layer, which has implications for influencing nanoparticle interactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Quantitative Reflection Imaging for the Morphology and Dynamics of Live Aplysia californica Pedal Ganglion Neurons Cultured on Nanostructured Plasmonic Crystals

We describe a reflection imaging system that consists of a plasmonic crystal, a common laboratory microscope, and band-pass filters for use in the quantitative imaging and in situ monitoring of live cells and their substrate interactions. Surface plasmon resonance (SPR) provides a highly sensitive method to monitor changes in physicochemical properties occurring at metal-dielectric interfaces. Polyelectrolyte thin films deposited using the layer-by-layer (LBL) self-assembly method provide a reference system for calibrating the reflection contrast changes that occur when the polyelectrolyte film thickness changes and provide insight into the optical responses that originate from the multiple plasmonic features supported by this imaging system. Finitedifference time-domain (FDTD) simulations of the optical responses measured experimentally from the polyelectrolyte reference system are used to provide a calibration of the optical system for subsequent use in quantitative studies investigating live cell dynamics in cultures supported on a plasmonic crystal substrate. Live Aplysia californica pedal ganglion neurons cultured in artificial seawater were used as a model system through which to explore the utility of this plasmonic imaging technique. Here, the morphology of cellular peripheral structures ≲80 nm in thickness were quantitatively analyzed, and the dynamics of their trypsin-induced surface detachment were visualized. These results illustrate the capacities of this system for use in investigations of the dynamics of ultrathin cellular structures within complex bioanalytical environments.

47 OTHER INSTRUMENTATION↗

Interpreting Neutron Reflectivity Profiles of Diblock Copolymer Nanocomposite Thin Films Using Hybrid Particle-Field Simulations

Mixtures of block copolymers and nanoparticles (block copolymer nanocomposites) are known to microphase separate into a plethora of microstructures, depending on the composition, length scale and nature of interactions among its different constituents. Theoretical and experimental works on this class of nanocomposites have already high-lighted intricate relations among chemical details of the polymers, nanoparticles, and various microstructures. Confining these nanocomposites in thin films yields an even larger array of structures, which are not normally observed in the bulk. In contrast to the bulk, exploring various microstructures in thin films by the experimental route remains a challenging task. Here in this work, we construct a model for the thin films of lamellar forming diblock copolymers containing spherical nanoparticles based on a hybrid particle-field approach. The model is benchmarked by comparison with the depth profiles obtained from the neutron reflectivity experiments for symmetric poly(deuterated styrene-b-n butyl methacrylate) copolymers blended with spherical magnetite nanoparticles covered with hydrogenated poly(styrene) corona. We show that the model based on a hybrid particle-field approach provides details of the underlying microphase separation in the presence of the nanoparticles through a direct comparison to the neutron reflectivity data. This work benchmarks the application of the hybrid particle-field model to extract the interaction parameters for exploring different microstructures in thin films containing block copolymers and nanocomposites.

36 MATERIALS SCIENCE↗

A Polycrystalline Pd Surface Studied by Two-Dimensional Surface Optical Reflectance during CO Oxidation: Bridging the Materials Gap

Industrial catalysts are complex materials systems operating in harsh environments. The active parts of the catalysts are nanoparticles that expose different facets with different surface orientations at which the catalytic reactions occur. However, these facets are close to impossible to study in detail under industrially relevant operating conditions. Instead, simpler model systems, such as single crystals with a well-defined surface orientation, have been successfully used to study gas–surface interactions such as adsorption and desorption, surface oxidation, and oxidation/reduction reactions. To more closely mimic the many facets exhibited by nanoparticles and thereby close the so-called materials gap, there has also been a recent move toward using polycrystalline surfaces and curved crystals. However, these studies are limited either by the pressure or spatial resolution at realistic pressures or by the number of surfaces studied simultaneously. In this work, we demonstrate the use of reflectance microscopy to study a vast number of catalytically active surfaces simultaneously under realistic and identical reaction conditions. As a proof of concept, we have conducted an operando experiment to study CO oxidation over a Pd polycrystal, where the polycrystalline surface acts as a collection of many single-crystal surfaces. Finally, we visualized the resulting data by plotting the reflectivity as a function of surface orientation. We think the techniques and visualization methods introduced in this work will be key toward bridging the materials gap in catalysis.

36 MATERIALS SCIENCE↗

Time Resolved Reflectivity Measurements of Convective Clouds

National Aeronautics and Space Administration's Investigations of Convective Updrafts (INCUS) mission aims to document convective mass flux through changes in the radar reflectivity (ΔZ) in convective cores captured by a constellation of three Ka-band radars sampling the same convective cells over intervals of 30, 90, and 120 s. Here, high spatiotemporal resolution observations of convective cores from surface-based radars that use agile sampling techniques are used to evaluate aspects of the INCUS measurement approach using real observations. Analysis of several convective cells confirms that large coherent ΔZ structure with measurable signal (>5 dB) can occur in less than 30 s and are correlated with underlying convective motions. The analysis indicates that the INCUS mission radar footprint and along track sampling are adequate to capture most of the desirable ΔZ signals. This unique demonstration of reflectivity time-lapse provides the framework for estimating convective mass flux independent from Doppler techniques with future radar observations.

54 ENVIRONMENTAL SCIENCES↗

Grass Evolutionary Lineages Can Be Identified Using Hyperspectral Leaf Reflectance

Hyperspectral remote sensing has the potential to map numerous attributes of the Earth’s surface, including spatial patterns of biological diversity. Grasslands are one of the largest biomes on Earth. Accurate mapping of grassland biodiversity relies on spectral discrimination of endmembers of species or plant functional types. We focused on spectral separation of grass lineages that dominate global grassy biomes: Andropogoneae (C 4 ), Chloridoideae (C 4 ), and Pooideae (C 3 ). We examined leaf reflectance spectra (350–2,500 nm) from 43 grass species representing these grass lineages from four representative grassland sites in the Great Plains region of North America. Here, we assessed the utility of leaf reflectance data for classification of grass species into three major lineages and by collection site. Classifications had very high accuracy (94%) that were robust to site differences in species and environment. We also show an information loss using multispectral sensors, that is, classification accuracy of grass lineages using spectral bands provided by current multispectral satellites is much lower (accuracy of 85.2% and 61.3% using Sentinel 2 and Landsat 8 bands, respectively). Our results suggest that hyperspectral data have an exciting potential for mapping grass functional types as informed by phylogeny. Leaf-level hyperspectral separability of grass lineages is consistent with the potential increase in biodiversity and functional information content from the next generation of satellite-based spectrometers.

59 BASIC BIOLOGICAL SCIENCES↗

Constraining Black Carbon Aging in Global Models to Reflect Timescales for Internal Mixing

The radiative effects of black carbon depend critically on its atmospheric lifetime, which is controlled by the rate at which freshly emitted combustion particles become internally mixed with other aerosol components. Global aerosol models strive to represent this process, but the timescale for aerosol mixing is not easily constrained using observations. In this study, we apply a timescale parameterization derived from particle‐resolved simulations to quantify, in a global aerosol model, the timescale for internal mixing. We show that, while highly variable, the average timescale for internal mixing is approximately 3 hr, which is much shorter than the 24‐hr aging timescale traditionally applied in bulk aerosol models. We then use the mixing timescale to constrain the aging criterion in the Modal Aerosol Module. Our analysis reveals that, to best reflect timescales for internal mixing, modal models should assume that particles transition from the hydrophobic (fresh) to the hydrophilic (aged) class once they accumulate a coating thickness equal to four monolayers of sulfuric acid, as opposed to the model's current aging criterion of eight monolayers. We show that, in remote regions like the Arctic and Antarctic, predictions of black carbon loading and its seasonal variation are particularly sensitive to the model representation of aging. By constraining aging in global models to reflect mixing timescales simulated by the particle‐resolved model, we eliminate one of the free parameters governing black carbon's long‐range transport and spatiotemporal distribution.

54 ENVIRONMENTAL SCIENCES↗

Evidence for anisotropic spin-triplet Andreev reflection at the 2D van der Waals ferromagnet/superconductor interface

Fundamental symmetry breaking and relativistic spin–orbit coupling give rise to fascinating phenomena in quantum materials. Of particular interest are the interfaces between ferromagnets and common s-wave superconductors, where the emergent spin-orbit fields support elusive spin-triplet superconductivity, crucial for superconducting spintronics and topologically-protected Majorana bound states. Here, we report the observation of large magnetoresistances at the interface between a quasi-two-dimensional van der Waals ferromagnet Fe 0.29 TaS 2 and a conventional s-wave superconductor NbN, which provides the possible experimental evidence for the spin-triplet Andreev reflection and induced spin-triplet superconductivity at ferromagnet/superconductor interface arising from Rashba spin-orbit coupling. The temperature, voltage, and interfacial barrier dependences of the magnetoresistance further support the induced spin-triplet superconductivity and spin-triplet Andreev reflection. This discovery, together with the impressive advances in two-dimensional van der Waals ferromagnets, opens an important opportunity to design and probe superconducting interfaces with exotic properties.

36 MATERIALS SCIENCE↗

Sub-nanograin metal based high efficiency multilayer reflective optics for high energies

The present finding illuminates the physics of the formation of interfaces of metal based hetero-structures near layer continuous limit as an approach to develop high-efficiency W/B 4 C multilayer (ML) optics with ML periodicity varying d = 1.86–1.23 nm at a fixed number of layer pairs N = 400. The microstructure of metal layers is tailored near the onset of grain growth to control the surface density of grains resulting in small average sizes of grains to sub-nanometers. This generates concurrently desirable atomically sharp interfaces, high optical contrast, and desirable stress properties over a large number of periods, which have evidence through the developed ML optics. We demonstrate significantly high reflectivities of ML optics measured in the energy range 10–20 keV, except for d = 1.23 nm due to quasi-continuous layers. The reflectivities at soft gamma-rays are predicted.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Remote sensing of Pu in uranyl nitrate crystals using reflectance spectroscopy and chemometrics

Remote quantification of Pu(VI) (0–5 mol%) co-crystallized with U in uranyl nitrate hexahydrate (UNH) crystals was achieved in a glove box using reflectance spectroscopy coupled with chemometric modeling. Reflectance spectra were also acquired for Pu(IV) and Np(VI) (0–5 mol%) crystallized with UNH; revealing spectral features consistent with their solution-phase analogs. Principal component analysis revealed Pu(IV/VI) and Np(VI) concentrations as the primary source of variation in the data, informing the development of a supervised partial least squares regression model for Pu(VI). The resulting calibration demonstrated robust performance, with replicate root mean square errors near 10% and quantifiable limits near 0.2 mol% Pu(VI) relative to U. The Pu(VI) remained stable in the crystalline UNH matrix for at least one week with minimal reduction to Pu(IV). Notably, Pu(VI) and Np(VI) incorporation in UNH quenched U(VI) fluorescence while Pu(IV) did not. This study presents a noninvasive, spectroscopic approach for solid-state Pu quantification, with direct implications for material accountability and nuclear nonproliferation monitoring.

Sadergaski, Luke R. [Oak Ridge National Laboratory↗

A High-Reflectivity, Ambient-Stable Graphene Mirror for Neutral Atomic and Molecular Beams

We report a He and H{sub 2} diffraction study of graphene-terminated Ru(0001) thin films grown epitaxially on c-axis sapphire. Even for samples exposed for several weeks to ambient conditions, brief annealing in ultrahigh vacuum restored extraordinarily high specular reflectivities for He and H{sub 2} beams (23% and 7% of the incident beam, respectively). The quality of the angular distributions recorded with both probes exceeds the one obtained from in-situ prepared graphene on Ru(0001) single crystals. Our results for graphene-terminated Ru thin films represent a significant step toward ambient tolerant, high-reflectivity curved surface mirrors for He-atom microscopy.

36 MATERIALS SCIENCE↗

A reflective optical transport system for ultraviolet Thomson scattering from electron plasma waves on OMEGA

A reflective optical transport system has been designed for the OMEGA Thomson-scattering diagnostic. A Schwarzschild objective that uses two concentric spherical mirrors coupled to a Pfund objective provides diffraction-limited imaging across all reflected wavelengths. This enables the operator to perform Thomson-scattering measurements of ultraviolet (0.263 {mu}m) light scattered from electron plasma waves.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Making use of x-ray optical effects in photoelectron-, Auger electron-, and x-ray emission spectroscopies: Total reflection, standing-wave excitation, and resonant effects

We present a general theoretical methodology and related open-access computer program for carrying out the calculation of photoelectron, Auger electron, and x-ray emission intensities in the presence of several x-ray optical effects, including total reflection at grazing incidence, excitation with standing-waves produced by reflection from synthetic multilayers and at core-level resonance conditions, and the use of variable polarization to produce magnetic circular dichroism. Calculations illustrating all of these effects are presented, including in some cases comparisons to experimental results. Sample types include both semi-infinite flat surfaces and arbitrary multilayer configurations, with interdiffusion/roughness at their interfaces. These x-ray optical effects can significantly alter observed photoelectron, Auger, and x-ray intensities, and in fact lead to several generally useful techniques for enhancing surface and buried-layer sensitivity, including layer-resolved densities of states and depth profiles of element-specific magnetization. The computer program used in this study should thus be useful for a broad range of studies in which x-ray optical effects are involved or are to be exploited in next-generation surface and interface studies of nanoscale systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Angular distributions of surface produced H{sup −} ions for reflection and desorption processes

A numerical simulation code, Atomic Collision in Amorphous Target, has been run to clarify the effects due to the incident angle of hydrogen flux onto surface collision cascade in the subsurface region of a Cs covered Mo plasma grid. The code has taken into account the threshold energy for negative hydrogen (H{sup −}) ions to leave the surface. This modification has caused the shift of energy distribution functions of H{sup −} from that of hydrogen atoms leaving the surface. The results have shown that large incident angle of hydrogen particle tilt the angular distribution of reflection component, while it caused a small effect onto the angular distribution of desorption component. The reflection coefficient has increased, while the desorption yield has decreased for increased angle of incidence measured from the surface normal.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Total reflection infrared spectroscopy of water-ice and frozen aqueous NaCl solutions

Liquid-like and liquid water at and near the surface of water-ice and frozen aqueous sodium chloride films were observed using attenuated total reflection infrared spectroscopy (ATR-IR). The concentration of NaCl ranged from 0.0001 to 0.01 M and the temperature varied from the melting point of water down to 256 K. The amount of liquid brine at the interface of the frozen films with the germanium ATR crystal increased with salt concentration and temperature. Experimental spectra are compared to reflection spectra calculated for a simplified morphology of a uniform liquid layer between the germanium crystal and the frozen film. This morphology allows for the amount of liquid observed in an experimental spectrum to be converted to the thickness of a homogenous layer with an equivalent amount of liquid. These equivalent thickness ranges from a nanometer for water-ice at 260 K to 170 nm for 0.01 M NaCl close to the melting point. The amounts of brine observed are over an order of magnitude less than the total liquid predicted by equilibrium thermodynamic models, implying that the vast majority of the liquid fraction of frozen solutions may be found in internal inclusions, grain boundaries, and the like. Thus, the amount of liquid and the solutes dissolved in them that are available to react with atmospheric gases on the surfaces of snow and ice are not well described by thermodynamic equilibrium models which assume the liquid phase is located entirely at the surface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Propagating and reflecting of spin wave in permalloy nanostrip with 360° domain wall

By micromagnetic simulation, we investigated the interaction between propagating spin wave (or magnonic) and a 360° domain wall in a nanostrip. It is found that propagating spin wave can drive a 360° domain wall motion, and the velocity and direction are closely related to the transmission coefficient of the spin wave of the domain wall. When the spin wave passes through the domain wall completely, the 360° domain wall moves toward the spin wave source. When the spin wave is reflected by the domain wall, the 360° domain wall moves along the spin wave propagation direction. Moreover, when the frequency of the spin wave is coincident with that of the 360° domain wall normal mode, the 360° domain wall velocity will be resonantly enhanced no matter which direction the 360 DW moves along. On the other hand, when the spin wave is reflected from the moving 360° domain wall, we observed the Doppler effect clearly. After passing through a 360° domain wall, the phase of the spin wave is changed, and the phase shift is related to the frequency. Nevertheless, phase shift could be manipulated by the number of 360° domain walls that spin wave passing through.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗