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DOE OSTI2020

Understanding the Structure and Dynamics of Complex Biomembrane Interactions by Neutron Scattering Techniques

The membrane is one of the key structural materials of biology at the cellular level. Composed predominantly of a bilayer of lipids with embedded and bound proteins, it defines the boundaries of the cell and many organelles essential to life and therefore is involved in almost all biological processes. Membrane-specific interactions, such as drug binding to a membrane receptor or the interactions of an antimicrobial compound with the lipid matrix of a pathogen membrane, are of interest across the scientific disciplines. Herein we present a review, aimed at nonexperts, of the major neutron scattering techniques used in membrane studies: small-angle neutron scattering, neutron membrane diffraction, neutron reflectometry, quasielastic neutron scattering, and neutron spin echo. Neutron scattering techniques are well suited to studying biological membranes. The nondestructive nature of cold neutrons means that samples can be measured for long periods without fear of beam damage from ultraviolet, electron, or X-ray radiation, and neutron beams are highly penetrating, thus offering flexibility in samples and sample environments. Most important is the strong difference in neutron scattering lengths between the two most abundant forms of hydrogen, protium and deuterium. Changing the relative amounts of protium/deuterium in a sample allows the production of a series of neutron scattering data sets, enabling the observation of differing components within complex membrane architectures. This approach can be as simple as using the naturally occurring neutron contrast between different biomolecules to study components in a complex by changing the solution H 2 O/D 2 O ratio or as complex as selectively labeling individual components with hydrogen isotopes. This review presents an overview of each experimental technique with the neutron instrument configuration, related sample preparation and sample environment, and data analysis, highlighted by a special emphasis on using prominent neutron contrast to understand structure and dynamics. This review gives researchers a practical introduction to the often enigmatic suite of neutron beamlines, thereby lowering the barrier to taking advantage of these large-facility techniques to achieve new understandings of membranes and their interactions with other molecules.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Seasonal Dependent Impact of Ice Cloud Longwave Scattering on the Polar Climate

Most climate models neglect cloud longwave (LW) scattering because scattering is considered negligible compared to strong LW absorption by clouds and greenhouse gases. While this rationale is valid for simulating extrapolar regions, it is questionable for the polar regions, where the atmosphere is dry and hence has weak absorption, and ice clouds that have strong scattering capability frequently occur. Using the slab-ocean Community Earth System Model, we show that ice cloud LW scattering can warm winter surface air temperature by 0.8–1.8 K in the Arctic and 1.3–1.9 K in the Antarctic, while this warming becomes much weaker in polar summer. Such scattering effect cannot be correctly assessed when sea surface temperature and sea ice are prescribed as this effect is manifested through a surface-atmosphere coupling. Furthermore, cloud LW scattering is a necessity for the correct simulation of polar climate and surface radiation budget, especially in the winter.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2012

Epitaxial Ag(001) grown on MgO(001) and TiN(001): Twinning, surface morphology, and electron surface scattering

Epitaxial Ag(001) layers were deposited on MgO(001) in order to study electron surface scattering. X-ray reflection indicates 3D layer nucleation with a high rms surface roughness of 1.0 nm for a layer thickness d = 3.5 nm. X-ray diffraction shows that {l_brace}111{r_brace} twins form at d < 11 nm, followed by 2nd generation twinning for 11 nm < d < 120 nm. Increasing the growth temperature from 25 to 150 deg. C suppresses 2nd generation twinning and reduces the twin density by 2 orders of magnitude. In situ deposition of epitaxial 2.5-nm-thick TiN(001) underlayers prior to Ag deposition results in twin-free single-crystal Ag(001) with 10 x smoother surfaces for d = 3.5 nm. This is attributed to a better wetting on the higher energy TiN(001) than MgO(001) surface, resulting in the absence of 3D nuclei with exposed {l_brace}111{r_brace} facets, which facilitate twin nucleation. The twinned Ag/MgO layers have a higher resistivity {rho} than the single crystal Ag/TiN layers at both 298 and 77 K, due to electron scattering at grain and twin boundaries. The {rho} for single-crystal Ag layers increases with decreasing d, which is well explained with known surface scattering models and provides specularity parameters for the Ag-vacuum and the Ag-air interfaces of p = 0.8 {+-} 0.1 and 0.4 {+-} 0.1, respectively. A comparison with corresponding epitaxial Cu(001) layers shows that {rho}{sub Ag} < {rho}{sub Cu} for d > 50 nm, consistent with known bulk values. However, {rho}{sub Ag} > {rho}{sub Cu} for d < 40 nm. This is attributed to the larger electron mean free path for electron-phonon scattering and a correspondingly higher resistivity contribution from surface scattering in Ag than Cu. In contrast, air exposure causes {rho}{sub Ag} < {rho}{sub Cu} for all d, due to diffuse scattering at the oxidized Cu surface and the correspondingly higher Cu resistivity.

36 MATERIALS SCIENCE↗

DOE OSTI2012

Landau damping effects on the scattering spin-asymmetry and channel preference in election-hole plasmas

The scattering spin-asymmetry and spin channel preference in electron collisions are investigated in electron-hole plasmas. It is found that the Landau damping effect enhances the scattering channel preference for the spin-singlet electron scattering and suppresses the spin-triplet electron scattering except the scattering angle {theta}={pi}/2. It is also found that the spin-singlet electron scattering decreases with an increase of the quantum shielding distance. In addition, the Landau damping effect on the spin-asymmetry parameter is found to be more significant in the intermediate domain of the quantum Debye length.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2014

Differential and integral cross sections for the rotationally inelastic scattering of methyl radicals with H{sub 2} and D{sub 2}

Comparisons are presented of experimental and theoretical studies of the rotationally inelastic scattering of CD{sub 3} radicals with H{sub 2} and D{sub 2} collision partners at respective collision energies of 680 ± 75 and 640 ± 60 cm{sup −1}. Close-coupling quantum-mechanical calculations performed using a newly constructed ab initio potential energy surface (PES) provide initial-to-final CD{sub 3} rotational level (n, k → n′, k′) integral and differential cross sections (ICSs and DCSs). The DCSs are compared with crossed molecular beam and velocity map imaging measurements of angular scattering distributions, which serve as a critical test of the accuracy of the new PES. In general, there is very good agreement between the experimental measurements and the calculations. The DCSs for CD{sub 3} scattering from both H{sub 2} and D{sub 2} peak in the forward hemisphere for n′ = 2–4 and shift more to sideways and backward scattering for n′ = 5. For n′ = 6–8, the DCSs are dominated by backward scattering. DCSs for a particular CD{sub 3} n → n′ transition have a similar angular dependence with either D{sub 2} or H{sub 2} as collision partner. Any differences between DCSs or ICSs can be attributed to mass effects because the PES is unchanged for CD{sub 3}−H{sub 2} and CD{sub 3}–D{sub 2} collisions. Further comparisons are drawn between the CD{sub 3}–D{sub 2} scattering and results for CD{sub 3}–He presented in our recent paper [O. Tkáč, A. G. Sage, S. J. Greaves, A. J. Orr-Ewing, P. J. Dagdigian, Q. Ma, and M. H. Alexander, Chem. Sci. 4, 4199 (2013)]. These systems have the same reduced mass, but are governed by different PESs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2014

The influence of the AlN barrier thickness on the polarization Coulomb field scattering in AlN/GaN heterostructure field-effect transistors

The electron mobility scattering mechanisms in AlN/GaN heterostuctures with 3 nm and 6 nm AlN barrier thicknesses were investigated by temperature-dependent Hall measurements. The effect of interface roughness (IFR) scattering on the electron mobility was found to be enhanced by increasing AlN barrier thickness. Moreover, using the measured capacitance-voltage and current-voltage characteristics of the fabricated heterostructure field-effect transistors (HFETs) with different Schottky areas on the two heterostuctures, the variations of electron mobility with different gate biases were investigated. Due to enhanced IFR scattering, the influence of polarization Coulomb field (PCF) scattering on electron mobility was found to decrease with increasing AlN barrier layer thickness. However, the PCF scattering remained an important scattering mechanism in the AlN/GaN HFETs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2014

Simulating x-ray Thomson scattering signals from high-density, millimetre-scale plasmas at the National Ignition Facility

We have developed a model for analysing x-ray Thomson scattering data from high-density, millimetre-scale inhomogeneous plasmas created during ultra-high pressure implosions at the National Ignition Facility in a spherically convergent geometry. The density weighting of the scattered signal and attenuation of the incident and scattered x-rays throughout the target are included using radial profiles of the density, opacity, ionization state, and temperature provided by radiation-hydrodynamics simulations. These simulations show that the scattered signal is strongly weighted toward the bulk of the shocked plasma and the Fermi degenerate material near the ablation front. We show that the scattered signal provides a good representation of the temperature of this highly nonuniform bulk plasma and can be determined to an accuracy of ca. 15% using typical data analysis techniques with simple 0D calculations. On the other hand, the mean ionization of the carbon in the bulk is underestimated. We suggest that this discrepancy is due to the convolution of scattering profiles from different regions of the target. Subsequently, we discuss modifications to the current platform to minimise the impact of inhomogeneities, as well as opacity, and also to enable probing of conditions more strongly weighted toward the compressed core.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2014

Effects of graded distribution of scattering centers on ballistic transport

The transmission coefficient of a two dimensional scattering region connected to ideal leads was calculated for the case of electrons interacting with an inhomogeneous distribution of repulsive or attractive scattering centers. The scattering centers with Gaussian profiles were positioned at regular intervals perpendicular to the transport direction, but were spaced according to a power law along this direction. The transmission function was obtained using a scattering formalism based on the R-matrix method. The simulations revealed that although, overall, the transmission coefficient decreases and becomes almost monotonously dependent on energy as the inhomogeneity of both attractive and repulsive scattering centers increases, the redistribution of transmission between open channels depends on the type of scattering centers.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2014

Deviational simulation of phonon transport in graphene ribbons with ab initio scattering

We present a deviational Monte Carlo method for solving the Boltzmann-Peierls equation with ab initio 3-phonon scattering, for temporally and spatially dependent thermal transport problems in arbitrary geometries. Phonon dispersion relations and transition rates for graphene are obtained from density functional theory calculations. The ab initio scattering operator is simulated by an energy-conserving stochastic algorithm embedded within a deviational, low-variance Monte Carlo formulation. The deviational formulation ensures that simulations are computationally feasible for arbitrarily small temperature differences, while the stochastic treatment of the scattering operator is both efficient and exhibits no timestep error. The proposed method, in which geometry and phonon-boundary scattering are explicitly treated, is extensively validated by comparison to analytical results, previous numerical solutions and experiments. It is subsequently used to generate solutions for heat transport in graphene ribbons of various geometries and evaluate the validity of some common approximations found in the literature. Our results show that modeling transport in long ribbons of finite width using the homogeneous Boltzmann equation and approximating phonon-boundary scattering using an additional homogeneous scattering rate introduces an error on the order of 10% at room temperature, with the maximum deviation reaching 30% in the middle of the transition regime.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Atom-diatom scattering dynamics of spinning molecules

We present full quantum mechanical scattering calculations using spinning molecules as target states for nuclear spin selective atom-diatom scattering of reactive D+H{sub 2} and F+H{sub 2} collisions. Molecules can be forced to rotate uni-directionally by chiral trains of short, non-resonant laser pulses, with different nuclear spin isomers rotating in opposite directions. The calculations we present are based on rotational wavepackets that can be created in this manner. As our simulations show, target molecules with opposite sense of rotation are predominantly scattered in opposite directions, opening routes for spatially and quantum state selective scattering of close chemical species. Moreover, two-dimensional state resolved differential cross sections reveal detailed information about the scattering mechanisms, which can be explained to a large degree by a classical vector model for scattering with spinning molecules.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2015

Influence of Dupree diffusivity on the occurrence scattering time advance in turbulent plasmas

The influence of Dupree diffusivity on the occurrence scattering time advance for the electron-ion collision is investigated in turbulent plasmas. The second-order eikonal method and the effective Dupree potential term associated with the plasma turbulence are employed to obtain the occurrence scattering time as a function of the diffusion coefficient, impact parameter, collision energy, thermal energy, and Debye length. The result shows that the occurrence scattering time advance decreases with an increase of the Dupree diffusivity. Hence, we have found that the influence of plasma turbulence diminishes the occurrence time advance in forward electron-ion collisions in thermal turbulent plasmas. The occurrence time advance shows that the propensity of the occurrence time advance increases with increasing scattering angle. It is also found that the effect of turbulence due to the Dupree diffusivity on the occurrence scattering time advance decreases with an increase of the thermal energy. In addition, the variation of the plasma turbulence on the occurrence scattering time advance due to the plasma parameters is also discussed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2016

Mesoporous multi-shelled ZnO microspheres for the scattering layer of dye sensitized solar cell with a high efficiency

Both light scattering and dye adsorbing are important for the power conversion efficiency PCE performance of dye sensitized solar cell (DSSC). Nanostructured scattering layers with a large specific surface area are regarded as an efficient way to improve the PCE by increasing dye adsorbing, but excess adsorbed dye will hinder light scattering and light penetration. Thus, how to balance the dye adsorbing and light penetration is a key problem to improve the PCE performance. Here, multiple-shelled ZnO microspheres with a mesoporous surface are fabricated by a hydrothermal method and are used as scattering layers on the TiO{sub 2} photoanode of the DSSC in the presence of N719 dye and iodine–based electrolyte, and the results reveal that the DSSCs based on triple shelled ZnO microsphere with a mesoporous surface exhibit an enhanced PCE of 7.66%, which is 13.0% higher than those without the scattering layers (6.78%), indicating that multiple-shelled microspheres with a mesoporous surface can ensure enough light scattering between the shells, and a favorable concentration of the adsorbed dye can improve the light penetration. These results may provide a promising pathway to obtain the high efficient DSSCs.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2016

Plasma characterization using ultraviolet Thomson scattering from ion-acoustic and electron plasma waves (invited)

Collective Thomson scattering is a technique for measuring the plasma conditions in laser-plasma experiments. Simultaneous measurements of ion-acoustic and electron plasma-wave spectra were obtained using a 263.25-nm Thomson-scattering probe beam. A fully reflective collection system was used to record light scattered from electron plasma waves at electron densities greater than 10{sup 21} cm{sup −3}, which produced scattering peaks near 200 nm. An accurate analysis of the experimental Thomson-scattering spectra required accounting for plasma gradients, instrument sensitivity, optical effects, and background radiation. Practical techniques for including these effects when fitting Thomson-scattering spectra are presented and applied to the measured spectra to show the improvements in plasma characterization.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2016

Validations of calibration-free measurements of electron temperature using double-pass Thomson scattering diagnostics from theoretical and experimental aspects

This paper evaluates the accuracy of electron temperature measurements and relative transmissivities of double-pass Thomson scattering diagnostics. The electron temperature (T{sub e}) is obtained from the ratio of signals from a double-pass scattering system, then relative transmissivities are calculated from the measured T{sub e} and intensity of the signals. How accurate the values are depends on the electron temperature (T{sub e}) and scattering angle (θ), and therefore the accuracy of the values was evaluated experimentally using the Large Helical Device (LHD) and the Tokyo spherical tokamak-2 (TST-2). Analyzing the data from the TST-2 indicates that a high T{sub e} and a large scattering angle (θ) yield accurate values. Indeed, the errors for scattering angle θ = 135° are approximately half of those for θ = 115°. The method of determining the T{sub e} in a wide T{sub e} range spanning over two orders of magnitude (0.01–1.5 keV) was validated using the experimental results of the LHD and TST-2. A simple method to provide relative transmissivities, which include inputs from collection optics, vacuum window, optical fibers, and polychromators, is also presented. The relative errors were less than approximately 10%. Numerical simulations also indicate that the T{sub e} measurements are valid under harsh radiation conditions. This method to obtain T{sub e} can be considered for the design of Thomson scattering systems where there is high-performance plasma that generates harsh radiation environments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2017

Heterodyne x-ray diffuse scattering from coherent phonons

Here, we report Fourier-transform inelastic x-ray scattering measurements of photoexcited GaAs with embedded ErAs nanoparticles. We observe temporal oscillations in the x-ray scattering intensity, which we attribute to inelastic scattering from coherent acoustic phonons. Unlike in thermal equilibrium, where inelastic x-ray scattering is proportional to the phonon occupation, we show that the scattering is proportional to the phonon amplitude for coherent states. The wavevectors of the observed phonons extend beyond the excitation wavevector. The nanoparticles break the discrete translational symmetry of the lattice, enabling the generation of large wavevector coherent phonons. Elastic scattering of x-ray photons from the nanoparticles provides a reference for heterodyne mixing, yielding signals proportional to the phonon amplitude.

36 MATERIALS SCIENCE↗

DOE OSTI2018

RHEGAL: Resistive heating gas enclosure loadframe for in situ neutron scattering

In situ neutron scattering is a powerful tool to reveal materials atomic structural response such as phase transformation, lattice straining, and texture under external stimuli. The advent of a high flux neutron source such as the Spallation Neutron Source (SNS) allows fast measurement in even non-equilibrium conditions, i.e., phase transformation in steels. However, the commercial fast heating apparatus such as commercial physical simulation equipment is not designed for in situ neutron scattering, which limits its application to in situ materials research by using neutrons. Here we present a resistive heating gas enclosure loadframe (RHEGAL) for non-equilibrium phase transformation studies by using in situ neutron scattering, which takes the advantage of high flux neutron sources like SNS. RHEGAL enables fast resistive heating of metal samples to 1200 °C at a rate up to 60 °C/s in an inert atmosphere. It provides both horizontal and vertical positions for scattering optimization. The mechanical loading capability also allows in situ high temperature tension above the oxidation temperature limit. The optimized translucent neutron scattering window by silicon allows both reflection and transmission measurements, making this equipment applicable for neutron diffraction, small angle scattering, and imaging. Furthermore, to demonstrate the fast heating capability, the phase transformations of an example of advanced high strength steel heated at 3 °C/s and 30 °C/s were measured with the VULCAN engineering diffractometer, and the different phase transformation kinetics by neutron diffraction were presented.

47 OTHER INSTRUMENTATION↗

DOE OSTI2018

Multi-angle multi-pulse time-resolved Thomson scattering on laboratory plasma jets

A single channel sub-nanosecond time-resolved Thomson scattering system used for pulsed power-driven high energy density plasma measurements has been upgraded to give electron temperatures at two different times and from two different angles simultaneously. This system was used here to study plasma jets created from a 15 μm thick radial Al foil load on a 1 MA pulsed power machine. Two laser pulses were generated by splitting the initial 2.3 ns duration, 10 J, 526.5 nm laser beam into two pulses, each with 2.5 J, and delaying one relative to the other by between 3 and 14 ns. Time resolution within each pulse was obtained using a streak camera to record the scattered spectra from the two beams from two scattering angles. Analysis of the scattering profile showed that the electron temperature of the Al jet increased from 20 eV up to as much as 45 eV within about 2 ns by inverse bremsstrahlung for both laser pulses. The Thomson scattering results from jets formed with opposite current polarities showed different laser heating of the electrons, as well as possibly different ion temperatures. The two-angle scattering determined that the electron density of the plasma jet was at least 2 × 10 18 cm -3 .

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2018

First step toward a synthetic diagnostic for magnetic fluctuation measurements using cross-polarization scattering on DIII-D

Cross-polarization scattering (CPS) provides localized magnetic fluctuation ($\tilde{B}$) measurements in fusion plasmas based on the process where $\tilde{B}$ scatters electromagnetic radiation into the orthogonal polarization. The CPS system on DIII-D utilizes the probe beam of a Doppler backscattering (DBS) diagnostic combined with a cross-view CPS receiver system, which allows simultaneous density and $\tilde{B}$ measurements with good spatial and wavenumber coverage. The interpretation of the signals is challenging due to the complex plasma propagation of the DBS probe beam and CPS receive beams. A synthetic diagnostic for CPS is therefore essential to interpret data and perform detailed validation tests of non-linear turbulence simulations. This work reports a first step toward a synthetic diagnostic for CPS utilizing GENRAY, a 3-D ray tracing code, to simulate the propagation of the probe and scattered rays. The local $\tilde{B}$ wavenumber is calculated from the local O- and X-mode wavenumbers using the wave vector matching scattering condition. The CPS wavenumber values and spatial locations are determined by a complex consideration that includes the local density and $\tilde{B}$ level, receive antenna pattern and orientation, scattering volume, wavenumber values detected at the various scattering centers, and alignment of the magnetic wave vector with the plane perpendicular to the magnetic field. The issue of a spurious CPS signal due to polarization mismatches for launch and receive is also discussed. It is suggested that simultaneous O- and X-mode DBS measurements should be utilized for better understanding of the CPS signal contamination when the cutoff locations for both polarizations are close.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗