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At least 541 records · Page 30
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Imaging Wavepackets in Real-Space & Disentangling Ultrafast Solvation Dynamics with High-Energy Ultrafast X-ray Scattering

The microscopic information of solute and solute-solvent motions can be measured using ultrafast diffuse x-ray scattering, and compared to molecular dynamics simulations, as demonstrated in studies of solvated molecular systems done in X-ray free-electron lasers. However, for the typical photon energies used in these experiments, the photon momentum transfer range was limited to lower Q values where the signals arising from different parts of the studied system overlap significantly. Recently, this limitation was greatly alleviated by extending the photon energy at the Linac Coherent Light-Source (LCLS), significantly increasing the accessible momentum transfer range. This improvement is transformative for ultrafast diffuse x-ray scattering measurements, enabling for the first time to disentangle the solute scattering difference signal, that persists to higher Q values, from the bulk solvent and solute-solvent cross-terms difference signals. In addition, it enhances the prediction ability of modeling and simulation methods such as the hybrid QM/MM approach. The extended Q range also opens the way to resolve in real-space details regarding coherent wavepackets motions beyond their center-of-mass positions. Here, we present the first results on high-energy (18keV) diffuse x-ray scattering in solution, demonstrating high fidelity time-resolved scattering and analysis of the photoexcited model photocatalysts PtPOP ([Pt2(POP)4]4-), and IrDimen ([Ir2(dimen)4]2+) in several solvents. These complexes provide ideal systems for demonstrating the ability of high-Q ultrafast scattering and QM/MM simulations to decompose ultrafast solvation dynamics into specific changes in the solute-solvent pair distribution function with a particular focus on how electronically excited states change the interaction between the solvent and photo-catalytically active metal sites. We introduce an approach to further utilize the high-energy capability and demonstrate a single-shot ultra-wide-angle X-ray Scattering modality using two perpendicular detectors, spanning a scattering angle range of more than 100 degrees, allowing to extend the accessible momentum transfer range up to Q~14 Å-1. We develop a model-free method to invert the x-ray scattering signals and enable the recovery of multiple pair-density motions that happen simultaneously, allowing us to directly measure in real-space nuclear wavepacket motions. . [1] Natan, Adi. "Real-Space Inversion and Super-Resolution of Ultrafast X-ray Scattering using Natural Scattering Kernels." arXiv preprint arXiv:2107.05576 (2021)

Natan, Adi↗
DOE OSTI2024

Electronic structure and lattice dynamics of 1⁢𝑇−VSe 2 : Origin of the three-dimensional charge density wave

To characterize in detail the charge density wave (CDW) transition of 1⁢𝑇−VSe 2 , its electronic structure and lattice dynamics are comprehensively studied by means of x-ray diffraction, muon spectroscopy, angle resolved photoemission (ARPES), diffuse and inelastic x-ray scattering, and state-of-the-art first-principles density functional theory calculations. Resonant elastic x-ray scattering does not show any resonant enhancement at either V or Se, indicating that the CDW peak at the 𝐾 edges describes a purely structural modulation of the electronic ordering. ARPES experiments identify (i) a pseudogap at 𝑇 > 𝑇⁢ CDW , which leads to a depletion of the density of states in the ML-M'L' plane at 𝑇 < 𝑇⁢ CDW , and (ii) anomalies in the electronic dispersion reflecting a sizable impact of phonons on it. A diffuse scattering precursor, characteristic of soft phonons, is observed at room temperature (RT) and leads to the full collapse of the low-energy phonon (𝜔 1 ) with propagation vector (0.25 0 −0.3) r.l.u. Here, we show that the frequency and linewidth of this mode are anisotropic in momentum space, reflecting the momentum dependence of the electron-phonon interaction (EPI), hence demonstrating that the origin of the CDW is, to a much larger extent, due to the momentum dependent EPI with a small contribution from nesting. The pressure dependence of the 𝜔 1 soft mode remains nearly constant up to 13 GPa at RT, with only a modest softening before the transition to the high-pressure monoclinic C2/m phase. The wide set of experimental data is well captured by our state-of-the art first-principles anharmonic calculations with the inclusion of van der Waals corrections in the exchange-correlation functional. The comprehensive description of the electronic and dynamical properties of VSe 2 reported here adds important pieces of information to the understanding of the electronic modulations in the family of transition-metal dichalcogenides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Room temperature sodium diffusion in sodium iron phosphate investigated with neutron scattering

Sodium iron phosphate, Na x FePO 4 , is currently one of the most promising cathode materials for sodium ion batteries. Here we employ a systematic approach using three neutron scattering techniques to investigate temperature dependent properties with a focus on the charge transfer processes. Two distinct Na + diffusive motions are observed with quasielastic neutron scattering, including room temperature motion. These processes correspond to rapid double jumps through extrinsic vacancy sites of ∼6 Å along with the more fundamental nearest neighbor jumps of 3.1 Å. Experimental observations of room temperature ionic diffusion are highly desirable, as the diffusion pathways are naturally well suited for efficient transport. Inelastic neutron scattering was used to probe the vibrational density of states that assist in the ionic and electronic (polaronic) transport processes, which are further supported with density functional theory. Neutron diffraction examines the disordering of the sodium sublattice upon transition to the solid-solution phase, which is believed to enhance the overall kinetics during sodium insertion/extraction. Finally, 57 Fe Mössbauer spectroscopy measurements probes polaron hopping and the local structural evolution that modifies the electron density surrounding the redox active iron sites. This study sheds light on the temperature induced atomic scale dynamics that occur in olivine Na x FePO 4 .

Novak, Eric [Swarthmore College, Swarthmore, PA (U↗
DOE OSTI2020

Turbulence-level dependence of cosmic ray parallel diffusion

ABSTRACT Understanding the transport of energetic cosmic rays belongs to the most challenging topics in astrophysics. Diffusion due to scattering by electromagnetic fluctuations is a key process in cosmic ray transport. The transition from a ballistic to a diffusive-propagation regime is presented in direct numerical calculations of diffusion coefficients for homogeneous magnetic field lines subject to turbulent perturbations. Simulation results are compared with theoretical derivations of the parallel diffusion coefficient’s dependences on the energy and the fluctuation amplitudes in the limit of weak turbulence. The present study shows that the widely used extrapolation of the energy scaling for the parallel diffusion coefficient to high turbulence levels predicted by quasi-linear theory does not provide a universally accurate description in the resonant-scattering regime. It is highlighted here that the numerically calculated diffusion coefficients can be polluted for low energies due to missing resonant interaction possibilities of the particles with the turbulence. Five reduced-rigidity regimes are established, which are separated by analytical boundaries derived in this work. Consequently, a proper description of cosmic ray propagation can only be achieved by using a turbulence-level-dependent diffusion coefficient and can contribute to solving the Galactic cosmic ray gradient problem.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2017

Inter-plume aerodynamics for gasoline spray collapse

The collapse or merging of individual plumes of direct-injection gasoline injectors is of fundamental importance to engine performance because of its impact on fuel–air mixing. But, the mechanisms of spray collapse are not fully understood and are difficult to predict. The purpose of this work is to study the aerodynamics in the inter-spray region, which can potentially lead to plume collapse. High-speed (100 kHz) particle image velocimetry is applied along a plane between plumes to observe the full temporal evolution of plume interaction and potential collapse, resolved for individual injection events. Supporting information along a line of sight is obtained using simultaneous diffused back illumination and Mie-scatter techniques. Experiments are performed under simulated engine conditions using a symmetric eight-hole injector in a high-temperature, high-pressure vessel at the “Spray G” operating conditions of the engine combustion network. Indicators of plume interaction and collapse include changes in counter-flow recirculation of ambient gas toward the injector along the axis of the injector or in the inter-plume region between plumes. Furthermore, the effect of ambient temperature and gas density on the inter-plume aerodynamics and the subsequent plume collapse are assessed. Increasing ambient temperature or density, with enhanced vaporization and momentum exchange, accelerates the plume interaction. Plume direction progressively shifts toward the injector axis with time, demonstrating that the plume interaction and collapse are inherently transient.

33 ADVANCED PROPULSION SYSTEMS↗
NASA NTRS1993

Acceleration of cometary H2O group pickup ions by obliquely propagating nonlinear magnetosonic waves

The observations made during the encounter with comet Giacobini Zinner show that the character of MHD turbulence is governed by the magnetosonic (MS) waves generated by the pickup ions via a resonant cyclotron instability. The interaction of cometary ions in the mass loaded solar wind with MS waves propagating away from the comet and oblique to the interplanetary magnetic field (IMF) is investigated using the test particle approach. Ion trajectories, distribution functions, widths of pitch angle scattering and energy diffusion are obtained. We have also investigated the relationship between pitch angle scattering and the three parameters, namely, alpha, the angle between the solar wind flow direction and the ambient magnetic field, theta(sub BK), the angle between the ambient magnetic field and the wave propagation vector, and the ion injection velocity.

Srivastava, Krishna M.↗
DOE OSTI2017

Diffusive Transport of Several Hundred keV Electrons in the Earth's Slot Region

Here, we investigate the gradual diffusion of energetic electrons from the inner edge of the outer radiation belt into the slot region. The Van Allen Probes observed slow inward diffusion and decay of ~200–600 keV electrons following the intense geomagnetic storm that occurred on 17 March 2013. During the 10 day nondisturbed period following the storm, the peak of electron fluxes gradually moved from L ~ 2.7 to L ~ 2.4, and the flux levels decreased by a factor of ~2–4 depending on the electron energy. We simulated the radial intrusion and decay of electrons using a three–dimensional diffusion code, which reproduced the energy–dependent transport of electrons from ~100 keV to 1 MeV in the slot region. At energies of 100–200 keV, the electrons experience fast transport across the slot region due to the dominance of radial diffusion; at energies of 200–600 keV, the electrons gradually diffuse and decay in the slot region due to the comparable rate of radial diffusion and pitch angle scattering by plasmaspheric hiss; at energies of E > 700 keV, the electrons stopped diffusing near the inner edge of outer radiation belt due to the dominant pitch angle scattering loss. In addition to plasmaspheric hiss, magnetosonic waves and VLF transmitters can cause the loss of high pitch angle electrons, relaxing the sharp “top–hat” shaped pitch angle distributions created by plasmaspheric hiss. Our simulation indicates the importance of balance between radial diffusion and loss through pitch angle scattering in forming the diffusive intrusion of energetic electrons across the slot region.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS1980

The interplanetary transport of solar cosmic rays

Numerical solutions are presented for the propagation of solar cosmic rays in interplanetary space, including the effects of pitch-angle scattering and adiabatic focusing. The intensity-time profiles can be well fitted by a simple radial spatial diffusion equation with scattering mean-free path lambda(fit). The radial mean-free path so obtained is significantly larger than the true scattering mean-free path for low-rigidity particles due to both adiabatic focusing and the inapplicability of the diffusive approximation early in the event. The well-known discrepancy between lambda(fit) and the theoretical predictions may be resolved by these calculations.

Gombosi, T. I.↗
NASA NTRS2002

Diffusion NMR methods applied to xenon gas for materials study

We report initial NMR studies of (i) xenon gas diffusion in model heterogeneous porous media and (ii) continuous flow laser-polarized xenon gas. Both areas utilize the pulsed gradient spin-echo (PGSE) techniques in the gas phase, with the aim of obtaining more sophisticated information than just translational self-diffusion coefficients--a brief overview of this area is provided in the Introduction. The heterogeneous or multiple-length scale model porous media consisted of random packs of mixed glass beads of two different sizes. We focus on observing the approach of the time-dependent gas diffusion coefficient, D(t) (an indicator of mean squared displacement), to the long-time asymptote, with the aim of understanding the long-length scale structural information that may be derived from a heterogeneous porous system. We find that D(t) of imbibed xenon gas at short diffusion times is similar for the mixed bead pack and a pack of the smaller sized beads alone, hence reflecting the pore surface area to volume ratio of the smaller bead sample. The approach of D(t) to the long-time limit follows that of a pack of the larger sized beads alone, although the limiting D(t) for the mixed bead pack is lower, reflecting the lower porosity of the sample compared to that of a pack of mono-sized glass beads. The Pade approximation is used to interpolate D(t) data between the short- and long-time limits. Initial studies of continuous flow laser-polarized xenon gas demonstrate velocity-sensitive imaging of much higher flows than can generally be obtained with liquids (20-200 mm s-1). Gas velocity imaging is, however, found to be limited to a resolution of about 1 mm s-1 owing to the high diffusivity of gases compared with liquids. We also present the first gas-phase NMR scattering, or diffusive-diffraction, data, namely flow-enhanced structural features in the echo attenuation data from laser-polarized xenon flowing through a 2 mm glass bead pack. c2002 John Wiley & Sons, Ltd.

NASA Discipline Life Sciences Technologies↗
DOE OSTI2013

Cosmic-ray parallel and perpendicular transport in turbulent magnetic fields

A correct description of cosmic-ray (CR) diffusion in turbulent plasma is essential for many astrophysical and heliospheric problems. This paper aims to present the physical diffusion behavior of CRs in actual turbulent magnetic fields, a model of which has been numerically tested. We perform test particle simulations in compressible magnetohydrodynamic turbulence. We obtain scattering and spatial diffusion coefficients by tracing particle trajectories. We find no resonance gap for pitch-angle scattering at 90°. Our result confirms the dominance of mirror interaction with compressible modes for most pitch angles, as revealed by the nonlinear theory. For cross-field transport, our results are consistent with normal diffusion predicted earlier for large scales. The diffusion behavior strongly depends on the Alfvénic Mach number and the particle's parallel mean free path. We, for the first time, numerically derive the dependence of M{sub A}{sup 4} for the perpendicular diffusion coefficient with respect to the mean magnetic field. We conclude that CR diffusion coefficients are spatially correlated to the local turbulence properties. On scales smaller than the injection scale, we find that CRs are superdiffusive. We emphasize the importance of our results in a wide range of astrophysical processes, including magnetic reconnection.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2019

Plasmonic absorption-induced haze suppression in random scattering media

Light propagation in random scattering media is a common phenomenon in many scientific and engineering fields. Because of light-matter interaction, part of the light transmitted through a random scattering medium is diffuse and causes haze. Previous approaches to manipulate haze in random media mainly focused on regulating scattering and paid little attention to absorption. In this work, we present a comprehensive analysis of absorption-scattering coupling as well as its impact on haze in random media. We introduce the haze-absorption sensitivity (HAS) spectrum, an intrinsic property of a scattering medium that quantifies the potential of absorption-induced haze suppression. We also investigate the effect of scatterer geometry and concentration on the HAS spectrum. To experimentally demonstrate the effect of absorption in random media, we utilized the plasmonic absorption of silver and gold nanoparticles to reduce haze in a silica nanoparticle aqueous solution as the scattering medium. We showed that 15% (absolute) of haze suppression is possible by carefully choosing the optimal absorber. The experimental results closely matched the theoretical predictions. This work provides new understandings of absorption and scattering coupling in random media. The fundamental mechanisms elucidated in this work can offer new pathways for regulating haze in a variety of random scattering media.

Zhao, Lin (ORCID:000000028865859X)↗
NASA NTRS2001

Comparison of Jovian and Terrestrial Lightning as Observed from Space

We compare the images of Jovian lightning taken by Galileo spacecraft with the images of terrestrial lightning observed by Lightning Imaging Spectrometer (LIS) onboard the TERRA spacecraft. Both data sets have good spatial resolution: Galileo's pixel is 25 km, or about half the atmospheric scale height, LIS pixel is 3-6 km, also about half of the scale height. This good resolution allows us to see that both Jovian and terrestrial lightning spots look diffuse because of the scattering in the clouds above. Previously we used the appearance of the diffuse spots on Jupiter to model lightning depths and the opacity and shape of the overlying clouds (Dyudina and Ingersoll, 2000). The comparison with LIS data allowed us to verify that the model is valid for terrestrial lightning. The irregular shapes of large terrestrial lightning suggests 30-km scale horizontal bolts. On Jupiter the spots, projected onto the horizontal plane, are nearly circular suggesting that the large size of the spots is mostly due to the horizontal diffusion of the photons scattered in the clouds. Unlike the Galileo observations, LIS has fine temporal resolution of 2 ms, or about 250 frames per single lightning flash. We will discuss the temporal evolution of terrestrial flashes and its implications for Jupiter.

Dyudina, Ulyana A.↗
NASA NTRS1975

A photometric function for diffuse reflection by particulate materials

A photometric function is proposed to describe the diffuse reflection of radiation by particulate materials. Both multiple scattering and the dominant effects of particle shadowing are included and the function is verified by comparisons with the photometries of laboratory surfaces. Brightness measurements of planetary and other diffusely scattering surfaces can be used to calculate the brightness for geometries other than those used in the measurements and for which the Minnaert function does not apply. The measurements also can be directly related to such surface characteristics as particle size, single-particle albedo, and compactness.

Meador, W. E.↗
NASA NTRS1982

Application of Kubelka-Munk theory of diffuse reflectance to geologic problems - The role of scattering

An understanding of the reflectance spectra of scattering media is vital for the appropriate interpretation of the reflectance spectra of planetary surfaces. When the absorption coefficient (k) and the mean size of the scattering centers are small, the Kubelka-Munk (K-M) theory of diffuse reflectance is valid. Since small values of k are characteristic of a wide variety of geologically important materials over a significant range of wavelength, the K-M theory should be applicable to appropriate portions of the reflectance spectra of these media if the dimensions of the scattering centers are sufficiently small. To test the utility of the K-M theory, a comparison is conducted of a set of theoretically generated spectra with a set of independently measured experimental spectra. The similarities found in the behavior of the two sets of spectra demonstrate the applicability of the K-M theory to the understanding of physical phenomena. Aspects of wavelength-dependent scattering are investigated.

Morris, R. V.↗
NASA NTRS1972

Laboratory simulation of diffuse reflectivity from a cloudy planetary atmosphere.

For the first time measurements in the multiple scattering regime of the diffuse reflectivity as a function of single scattering albedo have been made in a geometry that may be simulated by a plane parallel atmosphere of large optical depth. A comparison between the measurements and a theoretical computation of the diffuse reflectivity is presented. The measurements are within 1% agreement with the theoretical calculations for two different sizes of scattering particles which are larger than and smaller than the wavelength of the incident light, corresponding to the Mie and Rayleigh regimes, respectively.

Margolis, J. S.↗
NASA NTRS1996

Fundamental Concepts of Wave-Particle Interactions

Wave-particle interactions are fundamental to all collisionless plasmas, from the instabilitites generating the waves to the resonant interactions which cause pitch-angle scattering, particle energy diffusion and cross-field diffusion of particles.

wave particles plasmas collisionless plasmas scatt↗
NASA NTRS1975

Saturn's rings and Pioneer 11

Quantitative predictions of the diffuse reflection and transmission properties of Saturn's rings, relevant to the September 1979 Pioneer 11 flyby, are presented. Predictions are based on an elementary anisotropic scattering model. Interparticle separations are considered to be sufficiently large that mutual shadowing is negligible. Likely ranges in both the single scattering albedo and perpendicular optical thickness of the ring are considered. Situations of pronounced back-scattering and of isotropic scattering are treated individually. Spacecraft measurement of the radiation suffering diffuse scattering by the ring can provide a useful test of the basic ring model.

Price, M. J.↗