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DOE OSTI2023

Probing the Structure and Dynamics of Fluid Mixtures in Porous Materials Through Ultrafast Vibrational Spectro-Microscopy and Many-Body Molecular Dynamics

This research program focused on the characterization of both molecular structure and dynamics of aqueous solutions in various metal-organic frameworks (MOFs) and organic polymers that have recently been proposed for applications in water treatment technologies. This was accomplished by integrating ultrafast vibrational spectroscopy and microscopy, which are sensitive to local environments, molecular orientation, and dynamical couplings, with many-body molecular dynamics (MB-MD) simulations, which enable realistic modeling of aqueous systems and porous materials under different thermodynamic conditions. Our studies allowed for identifying the physical mechanisms and characterizing the underlying molecular interactions between water and host materials that determine the adsorption and transport processes of water in various MOFs and β-cyclodextrin polymers – prototypical examples of porous materials and polymers, that have recently been proposed for technological applications in water purification. By combining bulk- and surface-sensitive, spatially resolved ultrafast vibrational spectroscopy with MB-MD simulations, it was possible to gain broad insight into the structure and mobility of water under heterogeneous confinement at various length scales. In particular, measurements of surface- and bulk-sensitive vibrational spectra at single crystal level, integrated with MB-MD simulations were used to characterize domain-specific, structure–binding affinity relationships. Besides providing specific information about the behavior of aqueous solutions in prototypical MOFs and organic polymers for potential applications in water treatment technologies, our studies also provided fundamental insights into the properties of aqueous solutions in confined heterogeneous environments, which have broad implications in many areas, ranging from heterogeneous catalysis to oil recovery, ion transport processes, and reaction-diffusion processes in crowded systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1987

Spatial profile of thermoelectric effects during Peltier pulsing in Bi and Bi/MnBi eutectic

The spatial profile of the thermal transients that occur during and following the current pulsing associated with Peltier Interface Demarcation during directional solidification is studied. Results for pure Bi are presented in detail and compared with corresponding results for the Bi/MnBi eutectic. Significant thermal transients occur throughout the sample that can be accounted for by the Peltier effect, the Thomson effect, and Joule heating. These effects are separated and their behavior is studied as a function of time, current density, and position with respect to the solid/liquid interface.

Silberstein, R. P.↗

NASA NTRS1992

Mars: Wavelength-dependent dual polarization global scattering

During the 1988 and 1990 Mars oppositions, the first continuous-wave (CW) multi-wavelength radar observations were performed that include the entire echo in both polarizations. These observations, coordinated in subradar coverage when possible, were made with the Arecibo S-band (12.6 cm lambda) and Goldstone X-band (3.5 cm lambda) facilities. The CW spectra obtained during these oppositions have been studied using a variety of techniques to explore the spatial and wavelength dependence of both the Same-sense Circular (SC) and Opposite-sense Circular (OC) polarization returns. Earlier multi-wavelength comparisons dealt primarily with the quasispecular component of the echoes. Our work in contrast has much new information (at high signal-to-noise) for the SC 'depolarized component. The unique value of these radar observations lies in their potential for probing the subsurface scattering behavior in 'appropriate' terrain. The clearest case for wavelength dependence in the SC component is the scattering behavior over Tharsis, where the X-band features are significantly weaker than the S-band features. This hypothesis was advanced to account for the low thermal inertia of Tharsis, but also can explain the S/X differences if the layer is about 40 cm thick. In contrast to the Tharsis result, the depolarized echo from the heavily cratered terrain is actually stronger at X-band. The obvious interpretation is that more scatterers exist at the scale of the shorter wavelength, either at the surface or as a distributed subsurface scatterers. The strongest depolarized feature of the X-band spectra is associated with the south residual polar cap. The radar cross section of this feature corresponds to an equivalent full-disk albedo of unity.

Harmon, J. K.↗

NASA NTRS1998

Characterization of Clouds and the Anisotropy of Emitted and Reflected Radiances for the Purpose of Obtaining the Radiative Heating of the Atmosphere

The goal of the work supported through this grant was to assess the validity of the assumptions underlying the CERES Strategy for determining radiative fluxes. Specifically, the work focused on the determination of scene type and the use of anisotropic factors to derive radiative fluxes from observed broadband radiances. The work revealed a dependence of the anisotropy of reflected and emitted broadband radiances on the spatial resolution of the observations that had been overlooked in the formulation of the CERES strategy. This dependence on spatial resolution coupled with errors in scene identification led to view zenith angle dependent biases in the ERBE derived radiative fluxes. Scene identification will be greatly improved in CERES thereby alleviating somewhat the biases arising from the dependence of the anisotropy of the radiances on spatial resolution. Attention was then focused on the validity of plane-parallel radiative transfer theory which is relied on to characterize the scene types viewed by the CERES scanner. Again, viewing geometry dependent biases were found even for single-layered, overcast cloud systems. Such systems are taken to be the closest examples of plane-parallel clouds. At least some of the departures from plane-parallel behavior were evidently due to relatively small bumps on the tops of extensive stratus layers. The bumps cannot be resolved in the imagery that will be used to characterize the scenes viewed by the CERES scanner. As part of this investigation, the ice sheets of Greenland and Antarctica were shown to provide radiometrically stable targets for determining the visible and near infrared calibrations of radiometers. These targets were used to calibrate the reflected sunlight at visible wavelengths used in this study. Finally, the limitations of plane-parallel theory notwithstanding, the common practice of ignoring fractional cloud cover within the fields of view of imaging radiometers was shown to lead to biases in the retrieved cloud properties. The development of retrievals for pixel-scale cloud cover fraction is an attempt to reduce such bases. Work on these retrievals continues.

Coakley, James A., Jr.↗

NASA NTRS2000

Phase Shift Interferometer and Growth Set Up to Step Pattern Formation During Growth From Solutions. Influence of the Oscillatory solution Flow on Stability

We have assembled an experimental setup based on Michelson interferometry with the growing crystal surface as one of the reflective surfaces. The crystallization part of the device allows optical monitoring of a face of a crystal growing at temperature stable within 0.05 C in a flow of solution of controlled direction and speed. The reference arm of the interferometer contains a liquid crystal element that allows controlled shifts of the phase of the interferograms. We employ an image-processing algorithm, which combines five images with a pi/2 phase difference between each pair of images. The images are transferred to a computer by a camera capable of capturing 60 frames per second. The device allows data collection on surface morphology and kinetics during the face layers growth over a relatively large area (approximately 4 sq. mm) in situ and in real time during growth. The estimated depth resolution of the phase shifting interferometry is approximately 50 Angstroms. The data will be analyzed in order to reveal and monitor step bunching during the growth process. The crystal chosen as a model for study in this work is KH2PO4 (KDP). This optically non-linear material is widely used in frequency doubling applications. There have been a number of studies of the kinetics of KDP crystallization that can serve as a benchmark for our investigations. However, so far, systematic quantitative characteristics of step interaction and bunching are missing. We intend to present our first quantitative results on the onset, initial stages and development of instabilities in moving step trains on vicinal crystal surfaces at varying supersaturation, flow rate, and flow direction. Behavior of a vicinal face growing from solution flowing normal to the steps and periodically changing its direction in time was considered theoretically. It was found that this oscillating flow reduces both stabilization and destabilization effects resulted from the unidirectional solution flow directed up the step stream and down the step stream. This reduction of stabilization and destabilization comes from effective mixing which entangles the phase shifts between the spatially periodic interface perturbation and the concentration wave induced by this perturbation. Numerical results and simplified mixing criterion will be discussed.

Chernov, Alex A.↗

NASA NTRS2016

The Rhythm of Fairall 9. I. Observing the Spectral Variability With XMM-Newton and NuSTAR

We present a multi-epoch X-ray spectral analysis of the Seyfert 1 galaxy Fairall 9. Our analysis shows that Fairall 9 displays unique spectral variability in that its ratio residuals to a simple absorbed power law in the 0.510 keV band remain constant with time in spite of large variations in flux. This behavior implies an unchanging source geometry and the same emission processes continuously at work at the timescale probed. With the constraints from NuSTAR on the broad-band spectral shape, it is clear that the soft excess in this source is a superposition of two different processes, one being blurred ionized reflection in the innermost parts of the accretion disk, and the other a continuum component such as a spatially distinct Comptonizing region. Alternatively, a more complex primary Comptonization component together with blurred ionized reflection could be responsible.

galaxies: active↗

NASA NTRS2020

230Th Normalization: New Insights on an Essential Tool for Quantifying Sedimentary Fluxes in the Modern and Quaternary Ocean

230Th normalization is a valuable paleoceanographic tool for reconstructing high‐resolution sediment fluxes during the late Pleistocene (last ~500,000 years). As its application has expanded to ever more diverse marine environments, the nuances of 230Th systematics, with regard to particle type, particle size, lateral advective/diffusive redistribution, and other processes, have emerged. We synthesized over 1000 sedimentary records of 230Th from across the global ocean at two time slices, the late Holocene (0–5,000 years ago, or 0–5 ka) and the Last Glacial Maximum (18.5–23.5 ka), and investigated the spatial structure of 230Th‐normalized mass fluxes. On a global scale, sedimentary mass fluxes were significantly higher during the Last Glacial Maximum (1.79–2.17 g/sq.cmkyr, 95% confidence) relative to the Holocene (1.48–1.68 g/sq.cmkyr, 95% confidence). We then examined the potential confounding influences of boundary scavenging, nepheloid layers, hydrothermal scavenging, size‐dependent sediment fractionation, and carbonate dissolution on the efficacy of 230Th as a constant flux proxy. Anomalous 230Th behavior is sometimes observed proximal to hydrothermal ridges and in continental margins where high particle fluxes and steep continental slopes can lead to the combined effects of boundary scavenging and nepheloid interference. Notwithstanding these limitations, we found that 230Th normalization is a robust tool for determining sediment mass accumulation rates in the majority of pelagic marine settings (>1,000 m water depth).

Costa, Kassandra M.↗

NASA NTRSDate not supplied

Distortion of Perceived Visual Space after Eccentric Gaze Holding

Previous studies have shown that rebound nystagmus can be a behavioral probe into the adaptive properties of the gaze-holding mechanism, showing that after prolonged eccentric gaze holding and upon return to central gaze the eye tends to drift towards the previously held position. It is not known whether perception of visual space is also affected by similar adaptation mechanisms. The current study seeks to elucidate if eccentric gaze holding changes the perception of space in a relative spatial judgment task. To measure their spatial bias, twelve subjects were asked to report which among two short vertical lines flashed to the left or to the right of the display was closer to a third central line. Perception was assessed after holding eccentric gaze at 40 degrees towards the left or right and compared with control trials without eccentric gaze holding. Subjects showed a significant difference in spatial bias between the leftward and rightward gaze holding conditions (p = 0.04), suggesting that the visual space changes differently with respect to the side where gaze was held. While we did not observe an overall bias (p = 0.327) under no gaze holding we did observe a significant correlation between handedness and spatial bias (r2 = 0.4, p = 0.04). We conclude that gaze holding temporarily distorts the perception of space in a mechanism that may be related to the adaptation of the gaze holding mechanism.

perception↗

DOE OSTI2019

Embedded Fiber-Optic Sensors for In-Pile Applications

Qualification and commercialization of new nuclear fuels and materials requires a comprehensive set of data regarding behavior under irradiation. There are currently very limited options for in-situ monitoring of material evolution during irradiation due to the extremely harsh environment (i.e., high temperatures and intense radiation) of materials test reactors. This paper describes work being performed at Oak Ridge National Laboratory to embed metal-coated fiber-optic sensors into in-core irradiation experiments to enable measurement of radial dimensional changes and spatially distributed temperature and strain. Some critical issues that must be addressed before embedded fiber optics can be deployed in-core include (1) embedding of metal-coated fibers without failure or prohibitively large signal attenuation, (2) embedding in curved channels to allow for radial dimensional measurements, and (3) demonstrating that embedded fibers can survive the large stresses that result from differential thermal expansion between the glass fiber and the surrounding metal matrix. This work shows how optical fibers have been successfully embedded in aluminum and copper alloys in both straight and curved channels with various bend radii. The embedded fibers have also survived heating to temperatures of 500°C and cooling to room temperature. This paper presents some of the experimental results including measured light attenuation resulting from embedding with and without bends and high-temperature testing.

Petrie, Christian↗

DOE OSTI2019

Modeling fuel assembly distortion in light water reactors using BISON

Individual fuel rods in a light water reactor fuel assembly (FA) often have different power profiles that result in a spatial temperature gradient in the FA. This temperature gradient causes some rods to elongate more than others which could in turn distort the entire FA. Such FA distortion has been known to cause operational difficulties with refueling and with the insertion of control rods [1]. Numerical modeling of FA distortion due to differential elongation of fuel rods requires: (i) modeling the thermal elongation as well as the creep and irradiation induced elongation of the fuel rods, and (ii) modeling the bending response of the FA due to the differential elongation of the fuel rods. Past studies on this topic have been focused on the mechanical deformation of the FA with simplistic modeling of fuel rod elongation. In this paper, a simulation approach is presented that directly couples 2D axisymmetric fuel performance models of the individual fuel rods in a FA with structural beam models of the fuel rods in a FA using the Bison code [2]. This allows all of the mechanisms internal to the fuel rod leading to cladding elongation to be accounted for in the FA distortion model. To demonstrate this capability, the bowing of a simplified and idealized 6x6 FA (Fig. 1a), modeled using beam elements, is analyzed under different spatially varying power profiles. For this study, the guide tubes are rigidly connected to the spacer grid. Also, the fuel rods are rigidly connected to the spacer grid in all directions except the vertical direction (Y) along which slipping can occur between the fuel rods and spacer grids, depending on the friction coefficient between them. Coupling the thermo-mechanical response of individual fuel rods to the global mechanical behavior of the FA can shed light on the mechanisms that cause distortion of the FA and potential solutions to address this issue.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NASA NTRS1974

Transonic buffet behavior of Northrop F-5A aircraft

Flight tests were performed on an F-5A aircraft to investigate the dynamic buffet pressure distribution on the wing surfaces and the responses during a series of transonic maneuvers called wind-up turns. The conditions under which the tests were conducted are defined. The fluctuating buffet pressure data on the right wing of the aircraft were acquired by miniaturized semiconductor-type pressure transducers flush mounted on the wing. Processing of the fluctuating pressures and responses included the generation of the auto- and cross-power spectra, and of the spatial correlation functions. An analytical correlation procedure was introduced to compute the aircraft response spectra based on the measured buffet pressures.

Hwang, C.↗

DOE OSTI2021

Quantification of Deformation-Induced Concentration Fluctuations in Polymeric Liquids by Small-Angle Neutron Scattering

This study demonstrates how the large concentration fluctuations of polymeric liquids under deformation and flow can be quantitatively studied by applying the spherical harmonic expansion technique to small-angle neutron scattering. Using a series of binary polymer blends, it is shown that the emergence of the so-called butterfly patterns is caused by the change of sign in the leading anisotropic component of the small-angle spectrum, when the scattering is dominated by intermolecular correlation associated with flow-induced demixing. The increasing spatial fluctuations of concentration are evidenced by the enhancement of the isotropic component of the scattering spectrum in the zero-angle limit and peak shift of the leading anisotropic coefficients toward low Q. Additionally, the spherical harmonic expansion framework permits real-space analysis of anisotropic scattering length density correlation in a convenient form. The methodology described in this work provides a concrete venue for quantitative studies of phase behavior of fluids under deformation and flow via small-angle scattering techniques, where mainly qualitative approaches were previously employed.

Chemical structure↗

DOE OSTI2018

Local elasticity in nonlinear rheology of interacting colloidal glasses revealed by neutron scattering and rheometry

The flow of colloidal suspensions is ubiquitous in nature and industry. Colloidal suspensions showcase a wide range of rheological behavior, which should be closely related to the microscopic structure of the systems. With in situ small-angle neutron scattering complemented by rheological measurements, we investigated the deformation behavior of a charge-stabilized colloidal glass at particle level undergoing steady shear. A short-lived, localized elastic response at particle level, termed as the transient elasticity zone (TEZ), was identified from the neutron spectra. The existence of the TEZ, which could be promoted by the electrostatic interparticle potential, is a signature of deformation heterogeneity: the body of fluids under shear behaves like an elastic solid within the spatial range of the TEZ but like fluid outside the TEZ. The size of the TEZ shrinks as the shear rate increases in the shear thinning region, which shows that the shear thinning is accompanied by a diminishing deformation heterogeneity. More interestingly, the TEZ is found to be the structural unit that provides the resistance to the imposed shear, as evidenced by the quantitative agreement between the local elastic stress sustained by the TEZ and the macroscopic stress from rheological measurements at low and moderate shear rates. Our findings indicate an understanding on the nonlinear rheology of interacting colloidal glasses from a micro-mechanical view.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Flow field characteristics of a 127-pin rod bundle with hexagonal spacer grids

A determination of nominal flow phenomena in liquid metal fast reactor (LMFR) fuel assemblies is critical toward generation-IV reactor development. Axially positioned spacer grids are used to maintain the geometry of hexagonal rod bundles and simultaneously introduce perturbations in the flow. Three-dimensional (3D) printed asymmetric honeycomb spacer grids were installed in a prototypical 127-pin LMFR fuel assembly model to study complex fluid dynamics interactions induced by the spacer grid and rods. To characterize flow dynamics in this intricate geometry, time-resolved particle image velocimetry (TR-PIV) using the matched-index-of-refraction method was employed to obtain non-intrusive velocity measurements for three axial planes (one near-wall and two interior planes) at a Reynolds number of 6000. The statistical TR-PIV results compared sub-channel-dependent normalized time-averaged velocity, velocity fluctuations, Reynolds stress, vorticity, and turbulence kinetic energy distributions. TR-PIV line profiles characterized downstream spacer grid flow dynamics. Two-point spatial and spatial–temporal cross-correlation fields revealed local coherent structures and quantified convection velocities of traveling vortices. Spatial–temporal decomposition using dynamic mode decomposition (DMD) applied to the near-wall vorticity fields extracted turbulent structures and flow instabilities in the wake region of the spacer grid, along with their decay and frequency rates. Reduced-order velocity fields from DMD reconstructions identified the most energy-containing coherent structures persistent in the near-wall region. This research provides experimental data sets and analyses of flow behavior in rod bundles with hexagonal spacer grids. In conclusion, the results are critical toward LMFR design and geometry optimization, crucial for the validation of computational fluid dynamics and reduced-order flow models.

42 ENGINEERING↗

DOE OSTI2025

Azimuthal and axial structures in 3D particle-in-cell simulation of Penning discharge

We report the results of a 3D particle-in-cell simulation of cylindrical Penning discharge with the axial magnetic field in the so-called reflex configuration, where the cathode and anti-cathode are biased to the same negative potential. The discharge is supported by thermal electron emission from the cathode. Electron and ion collisions, including ionization, are fully accounted for. The emphasis is on a specific regime in which the plasma potential at the center of the discharge is positive with respect to the chamber walls, serving as an anode. Spatial and temporal scales of the observed azimuthal and axial fluctuations and structures are characterized. It is suggested that azimuthal structures are caused by the dissipative gradient-drift instability. We find that the axial fluctuations related to the plasma-beam instabilities are weakly correlated with the azimuthal perturbations of the density, so that the azimuthal modes rotate as a whole and do not show any axial shear. The behavior of the electric potential is more involved, demonstrating intermittent standing wave and propagating structures in the axial direction that modulate the electron transport, producing the standing wave pattern (along the z-direction) in the radial electron flux.

3D PIC simulation of discharge↗

DOE OSTI2019

Linking atmospheric pollution to cryospheric change in the Third Pole region: current progress and future prospects

ABSTRACT The Tibetan Plateau and its surroundings are known as the Third Pole (TP). This region is noted for its high rates of glacier melt and the associated hydrological shifts that affect water supplies in Asia. Atmospheric pollutants contribute to climatic and cryospheric changes through their effects on solar radiation and the albedos of snow and ice surfaces; moreover, the behavior and fates within the cryosphere and environmental impacts of environmental pollutants are topics of increasing concern. In this review, we introduce a coordinated monitoring and research framework and network to link atmospheric pollution and cryospheric changes (APCC) within the TP region. We then provide an up-to-date summary of progress and achievements related to the APCC research framework, including aspects of atmospheric pollution's composition and concentration, spatial and temporal variations, trans-boundary transport pathways and mechanisms, and effects on the warming of atmosphere and changing in Indian monsoon, as well as melting of glacier and snow cover. We highlight that exogenous air pollutants can enter into the TP’s environments and cause great impacts on regional climatic and environmental changes. At last, we propose future research priorities and map out an extended program at the global scale. The ongoing monitoring activities and research facilitate comprehensive studies of atmosphere–cryosphere interactions, represent one of China's key research expeditions to the TP and the polar regions and contribute to the global perspective of earth system science.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Quantum Quench Dynamics–Crossover Phenomena in Nonequilibrium Correlated Quantum Systems (Final Technical Report)

In this project we have developed analytical and numerical tools to study the interplay between interactions, dimensionality, fluctuations and disorder in quantum impurity systems. We have studied the transient dynamics following a quench, i.e. the sudden change in a control variable of the model Hamiltonian, which offers a unique way to examine the system’s spatial, temporal and energetic structure. Specifically, we have investigated how crossover scales, i.e. given by Kondo couplings, are affected by disorder. We have addressed a wide range of phenomena, such as the effects of static disorder on dynamical screening of magnetic impurities, and the influence of a fully time-fluctuating bath environment on the dephasing of system qubits. We have found that many of these systems exhibit fascinating counterintuitive behavior, such as e.g. the possibility of asymptotic unitary time evolution in specifically conditioned system-bath Hamiltonians. From a technical point of view, we have developed a supersymmetric formalism to analyze scaling functions of disordered quantum impurity spin chains, we generalized the strong-coupling real-space renormalization group method to probe the quench dynamics of higher-dimensional quantum impurity systems, and we devised a master equation approach that included the effects of a fully fluctuating environment. This way, we have addressed a very broad spectrum of transient phenomena in quantum impurity systems, with disorder ranging from the quenched to the annealed limit.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Partial connectomes of labeled dopaminergic circuits reveal non-synaptic communication and axonal remodeling after exposure to cocaine

Dopaminergic (DA) neurons exert profound influences on behavior including addiction. However, how DA axons communicate with target neurons and how those communications change with drug exposure remains poorly understood. We leverage cell type-specific labeling with large volume serial electron microscopy to detail DA connections in the nucleus accumbens (NAc) of the mouse (Mus musculus) before and after exposure to cocaine. We find that individual DA axons contain different varicosity types based on their vesicle contents. Spatially ordering along individual axons further suggests that varicosity types are non-randomly organized. DA axon varicosities rarely make specific synapses (<2%, 6/410), but instead are more likely to form spinule-like structures (15%, 61/410) with neighboring neurons. Days after a brief exposure to cocaine, DA axons were extensively branched relative to controls, formed blind-ended ‘bulbs’ filled with mitochondria, and were surrounded by elaborated glia. Finally, mitochondrial lengths increased by ~2.2 times relative to control only in DA axons and NAc spiny dendrites after cocaine exposure. We conclude that DA axonal transmission is unlikely to be mediated via classical synapses in the NAc and that the major locus of anatomical plasticity of DA circuits after exposure to cocaine are large-scale axonal re-arrangements with correlated changes in mitochondria.

59 BASIC BIOLOGICAL SCIENCES↗