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DOE OSTI2021

Role of water model on ion dissociation at ambient conditions

In this work, we study ion pair dissociation in water at ambient conditions using a combination of classical and ab initio approaches. The goal of this study is to disentangle the sources of discrepancy observed in computed potentials of mean force. In particular, we aim to understand why some models favor the stability of solvent-separated ion pairs vs contact ion pairs. We found that some observed differences can be explained by non-converged simulation parameters. However, we also unveil that for some models, small changes in the solution density can have significant effects on modifying the equilibrium balance between the two configurations. We conclude that the thermodynamic stability of contact and solvent-separated ion pairs is very sensitive to the dielectric properties of the underlying simulation model. In general, classical models are very robust in providing a similar estimation of the contact ion pair stability, while this is much more variable in density functional theory-based models. The barrier to transition from the solvent-separated to contact ion pair is fundamentally dependent on the balance between electrostatic potential energy and entropy. This reflects the importance of water intra- and inter-molecular polarizability in obtaining an accurate description of the screened ion–ion interactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1993

(abstract) The SIR-C/X-SAR Mission

The Shuttle Imaging Radar-C and X-Band Synthetic Aperture Radar (SIR-C/X-SAR) is a cooperative experiment between the National Aeronautics and Space Administration (NASA), the German Space Agency (DARA), and the Italian Space Agency (ASI). The experiment is the next evolutionary step in NASA's Spaceborne Imaging Radar (SIR) program that began with the Seasat SAR in 1978, and continued with SAR -A in 1981 and SAR-B in 1984. The program will eventually lead to the Earth Observing System (EOS) SAR later in this decade. SIR-C will provide increased capability over Seasat, SIR-A, and SIR-B by acquiring polarimetric images simultaneously at two microwave frequencies: L-band (wavelength 24 cm) and C-band (wavelength 6 cm). X-SAR will operate at X-band (wavelength 3 cm) with VV polarization, resulting in a three-frequency capability. Because radar backscatter is most strongly influenced by objects comparable in size to the radar wavelength, this multifrequency capability will provide information about the Earth's surface over a wide range of scales not discernable with single-frequency experiments. The polarimetric data will yield quantitative information about the surface geometric structure, vegetation dielectric properties, and surface discontinuities. The first SIR-C/X-SAR flight is planned for early in 1994, with two subsequent flights in different seasons to enable data aquisition under different environmental conditions. SIR-C/X-SAR will collect data for a period of 6 to 9 days during each flight. The instrument will be flown in a 57(deg) inclination orbit with a nomimal orbit altitude of 215 km. This altitude will result in a slightly drifting orbit. The latest status of the SIR-C/X-SAR mission and instrument design, science activities, and expected results will be presented.

SIR-C/XSAR radar backscatter surface geometric str↗

DOE OSTI2021

Electromagnetic wave absorption of multifunctional cementitious composites incorporating polyvinyl alcohol (PVA) fibers and fly ash: Effects of microstructure and hydration

Highlights: • The cementitious composite shows excellent wide-band electromagnetic wave absorption in a frequency range of 2–18 GHz. • The PVA fibers and the fly ash change the dielectric properties of the cementitious composite by Debye polarization. • The iron oxide of the cementitious binders contributes to the magnetic properties of the composites. • The impacts of the microstructure and the hydration of the cementitious composite on its microwave absorption are analyzed. This paper devises a novel method for the adjustment of the pore structure and the hydration of cement to improve the electromagnetic wave absorption of the cementitious composites incorporating polyvinyl alcohol (PVA) fibers and fly ash in a frequency range of 2–18 GHz. The underlying mechanism of the absorption is investigated to explore the possibility of the structural and functional integration of these composites. The electromagnetic parameters of the prepared cementitious composites and those of the raw materials are analyzed in a frequency range of 0.5–18 GHz. Moreover, the pore structure and the chemical environment of the cementitious composites are examined by mercury intrusion porosimetry (MIP), back-scattered electron detector (BSE), and X-ray photoelectron spectroscopy (XPS). The results indicate that the PVA fibers and the high-volume fly ash have a positive effect on electromagnetic wave absorption of the cementitious composites through the adjustment of their pore structure and hydration.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Effect of organic electroactive crystallites in a dielectric matrix on the electrical properties of a polymer dielectric

In this work, the effects of inserting chargeable α-quaterthiophene (α4T) crystallites in polystyrene (PS) multilayers used as a transistor gate and capacitor dielectric were investigated. X-ray diffraction (XRD), scanning electron microscopy with energy dispersive x-ray spectroscopy (SEM/EDS), and confocal microscopy indicated the formation of α4T crystallites in the PS matrix. A modified saturation-regime current voltage relationship was used to estimate organic field-effect transistor (OFET) threshold voltage V TH shifting, and in turn the quantities of stored charge that were observed as a result of dielectric charging. The crystallites increased the maximum charge storage capacity as well as the charge retention capability of the dielectrics. Kelvin probe force microscopy (KPFM) showed that charges were localized near the α4T crystallites upon charging. Trilayer experiments validated the charge retention improvement of α4T crystallite-embedded PS dielectrics. The crystallites also improved breakdown characteristics in PS used as a capacitor dielectric, suggesting their application to storage capacitors in addition to OFET logic.

25 ENERGY STORAGE↗

DOE OSTI2021

Hybrid of multi‐dimensional fillers for thermally enhanced polyamide 12 composites fabricated by selective laser sintering

Abstract Selective laser sintering (SLS) is an additive manufacturing technology that can provide a novel strategy to manufacture complex polymer‐based composites with tailored properties. In this study, polyamide 12 (PA12) composite powders based on Al 2 O 3 , boron nitride (BN), and carbon nanotubes (CNTs) were prepared via a two‐step mixing approach. Morphology characterization techniques indicated that the fillers were uniformly dispersed in the PA12 matrix as expected. Under the optimum 3D‐printing parameters, the fabrication of SLS parts with high filler loading could be obtained. With 40 wt% Al 2 O 3 , 8 wt% BN, and 2 wt% CNT hybrid fillers, the thermal conductivity of PA12 composites could reach 1.09 W/mK. It could be attributed to the synergistic effect of multi‐dimensional fillers to form dense and continuous thermal conduction paths. The factors influencing the performance of PA12 composites such as melting and crystallization behaviors, dielectric properties, and mechanical properties were also discussed. The results show that these composites have favorable dielectric and mechanical properties. Overall, the PA12 composites fabricated by SLS technology in this study exhibit excellent thermal management ability.

Yuan, Yue↗

DOE OSTI2020

Ion Pairing and Redissociaton in Low-Permittivity Electrolytes for Multivalent Battery Applications

Detailed speciation of electrolytes as a function of chemical system and concentration provides the foundation for understanding bulk transport as well as possible decomposition mechanisms. In particular, multivalent electrolytes have shown a strong coupling between anodic stability and solvation structure. Furthermore, solvents that are found to exhibit reasonable stability against alkaline-earth metals generally exhibit low permittivity, which typically increases the complexity of the electrolyte species. To improve our understanding of ionic population and associated transport in these important classes of electrolytes, the speciation of Mg(TFSI)2 in monoglyme and diglyme systems is studied via a multiscale thermodynamic model using first-principles calculations for ion association and molecular dynamics simulations for dielectric properties. The results are then compared to Raman and dielectric relaxation spectroscopies, which independently confirm the modeling insights. We find that the significant presence of free ions in the low-permittivity glymes in the concentration range from 0.02 to 0.6 M is well-explained by the low-permittivity redissociation hypothesis. Here, salt speciation is largely dictated by long-range electrostatics, which includes permittivity increases due to polar contact ion pairs. The present results suggest that other low-permittivity multivalent electrolytes may also reach high conductivities as a result of redissociation.

25 ENERGY STORAGE↗

DOE OSTI2022

Molecular-scale mechanisms of CO 2 mineralization in nanoscale interfacial water films

The calamitous impacts of untethered carbon emission from fossil-fuel-burning energy infrastructure calls for accelerated development of large-scale CO 2 capture, utilization, and storage technologies that are underpinned by fundamental understanding of molecular-level chemical processes. In the subsurface, rocks rich in divalent metals can react with CO 2 , permanently sequestering it in the form of stable metal carbonate minerals, with the CO 2 -H 2 O composition of the post-injection pore fluid acting as a primary control variable. Herein, we compare mechanistic reaction pathways for aqueous-mediated carbonation with carbon mineralization occurring in nanoscale adsorbed water films. In the extreme of pores filled with a CO 2 -dominant fluid, carbonation reactions are confined to nanometer-thick water films coating mineral surfaces, which enable metal cation release, transport, nucleation, and crystallization of metal carbonate minerals. Though seemingly counterintuitive, laboratory studies have demonstrated facile carbonation rates in these low water environments, which in recent years has begun to be better understood in mechanistic detail. The overarching objective of this review is to delineate the unique underlying molecular-scale reaction mechanisms that govern CO 2 mineralization in these reactive and dynamic quasi-2D interfaces. Here. we highlight the importance of understanding unique properties in thin water films, such as how water dielectric properties, and consequently ion solvation/hydration behavior, can change under nanoconfinement. We conclude by identifying important frontiers for future work and opportunities to exploit these fundamental chemical insights for decarbonization technologies in the 21st century.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2011

Dust removal from solar cells

A solar panel cleaning device includes a solar panel having a plurality of photovoltaic cells arranged in rows and embedded in the solar panel with space between the rows. A transparent dielectric overlay is affixed to the solar panel. A plurality of electrode pairs each of which includes an upper and a lower electrode are arranged on opposite sides of the transparent dielectric and are affixed thereto. The electrodes may be transparent electrodes which may be arranged without concern for blocking sunlight to the solar panel. The solar panel may be a dielectric and its dielectric properties may be continuously and spatially variable. Alternatively the dielectric used may have dielectric segments which produce different electrical field and which affects the wind "generated."

Ashpis, David E.↗

NASA NTRS2015

Dust Removal from Solar Cells

Ashpis, David E.↗

NASA NTRS1973

Electrical properties of dry rocks

The mechanism by which atmospheric moisture affects the conductivity and dielectric constant of rock specimens was studied in time and frequency domains. It is suggested that adsorbed water molecules alter the surface conductivity in a manner similar to that observed in semiconductors and insulators. Powdered basalts show a low-frequency dispersion produced by the atmospheric moisture remaining in the pore system of the sample in a high vacuum; this effect is attributed to isolated adsorption centers. Simulated lunar permafrost at 100 K and a vacuum of 10 to the -8th power torr together with data on lunar samples contaminated with atmospheric moisture and the dielectric properties of ice at various temperatures indicate that, if permafrost exists in the moon it should present a relaxation peak at approximately 300 Hz; for temperatures up to 263 K it may go up to 20 KHz. It is concluded that in order to have electrical steady state conditions in rock samples it is necessary to have volume charge accumulations at interfaces within the sample and at the electrode sample interface. A method for measuring heterogeneous dielectrics with non-negligible ohmic and dielectric conductivities is proposed and experimentally verified.

Morrison, H.↗

NASA NTRS1988

Modelling changes in the dielectric and scattering properties of young snow-covered sea ice at GHz frequencies

Observations of the physical properties of the snow cover and underlying young fast ice in Resolute Passage, Canada, were made during the winter of 1982. Detailed measurements of snow density and ice and snow temperatures, salinities, and brine volumes were made over a period of 46 d, beginning when the ice was 0.4 m thick and about 9 d old. The recorded values are used in a theoretical mixture model to predict the dielectric properties of the snow cover over the microwave frequency range. The results of this analysis are then used to investigate the effects of the snow properties on the radar backscatter signatures of young sea ice. The results show that backscatter is a function of the incidence angle and can change significantly over short periods of time during the early evolutionary phase of ice and snow-cover development. This has important consequences for the identification of young ice forms from SAR or SLAR images.

Drinkwater, Mark R.↗

NASA NTRS2013

Victim Simulator for Victim Detection Radar

Testing of victim detection radars has traditionally used human subjects who volunteer to be buried in, or climb into a space within, a rubble pile. This is not only uncomfortable, but can be hazardous or impractical when typical disaster scenarios are considered, including fire, mud, or liquid waste. Human subjects are also inconsistent from day to day (i.e., they do not have the same radar properties), so quantitative performance testing is difficult. Finally, testing a multiple-victim scenario is difficult and expensive because of the need for multiple human subjects who must all be coordinated. The solution is an anthropomorphic dummy with dielectric properties that replicate those of a human, and that has motions comparable to human motions for breathing and heartbeat. Two airfilled bladders filled and drained by solenoid valves provide the underlying motion for vinyl bags filled with a dielectric gel with realistic properties. The entire assembly is contained within a neoprene wetsuit serving as a "skin." The solenoids are controlled by a microcontroller, which can generate a variety of heart and breathing patterns, as well as being reprogrammable for more complex activities. Previous electromagnetic simulators or RF phantoms have been oriented towards assessing RF safety, e.g., the measurement of specific absorption rate (SAR) from a cell phone signal, or to provide a calibration target for diagnostic techniques (e.g., MRI). They are optimized for precise dielectric performance, and are typically rigid and immovable. This device is movable and "positionable," and has motion that replicates the small-scale motion of humans. It is soft (much as human tissue is) and has programmable motions.

Lux, James P.↗

NASA NTRS2020

Far-Infrared Properties of Cyclic Olefin Copolymer

Cyclic olefin copolymer (COC) is an amorphous thermoplastic with desirable dielectric and mechanical characteristics for optical applications. In particular, its low refractive index, overall mechanical strength, and absence of strong absorption features make it a promising substrate material for far-infrared applications, which include frequency-selective surfaces, scattering filters, and windows. The dielectric properties of selected COC formulations are surveyed from ≈10−700 per.cm (1000−14µm), and representative usage as a thin film membrane structure in optical filters is presented.

Wollack, Edward J.↗

NASA NTRS1998

Seasonally Frozen Soil Monitoring Using Passive Microwave Satellite Data and Simulation Modeling

Satellite data and simulation modeling were used to assess seasonally frozen soils in the central US - Canada borders area (46-53 degrees N and 96-108 degrees). We used Scanning Multichannel Microwave Radiometer (SMMR) satellite data to delineate the top layer of frozen soils. SMMR is a passive microwave sensor having five channels (6.6, 10, 18, 21 and 37 GHz) with a horizontal and vertical polarization. SMRR data are available between 1978-1987 with noon and midnight overpass and footprint sizes between 25 km and 150 km. SMMR data were processed from resampled 1/4 degree grid cells during fall freeze-up and spring thaw (fall 1985 - spring 1987). The dielectric properties of a target may directly affect the satellite signal. The dielectric value is an order of magnitude smaller for frozen soil water. There are other significant changes to the emitted microwave signal from changes to the surface physical temperature, attenuation of the soil signal from plant water and soil moisture. We further characterized the temporal and spatial dynamic of frozen soils using the FroST (Frozen Soil Temperature) simulation model. The FroST model was used to further predict soil water and ice content, and soil temperature. SMMR results were compared versus 5-cm soil temperature data from available weather stations (14 in Canada and 11 for available months in the US). SMMR data were analyzed as a function of frequency, polarization, polarization difference, and "frequency gradient". In addition, vegetation density, physical temperature and snow depth were also considered. Preliminary analysis of SMMR derived frozen soil/thaw classification using a simple threshold classification indicates a mean overall classification accuracy by season of 85 percent. A sensitivity analysis for different soils with varying amounts of snow was conducted with FroST, which showed that the amount of snow, and the time of snow fall and melt affected the ice and water content, and depth of thaw. These results indicate a potential source of flooding and erosion under conditions when melting snow and spring rains provide a source of infiltrating water.

Toll, D. L.↗

NASA NTRS2000

A Melting Layer Model for Passive/Active Microwave Remote Sensing Applications: Model Formulation and Comparison with Observations - Part 1

In this study, a 1-D steady-state microphysical model which describes the vertical distribution of melting precipitation particles is developed. The model is driven by the ice-phase precipitation distributions just above the freezing level at applicable gridpoints of "parent" 3-D cloud-resolving model (CRM) simulations. It extends these simulations by providing the number density and meltwater fraction of each particle in finely separated size categories through the melting layer. The depth of the modeled melting layer is primarily determined by the initial material density of the ice-phase precipitation. The radiative properties of melting precipitation at microwave frequencies are calculated based upon different methods for describing the dielectric properties of mixed phase particles. Particle absorption and scattering efficiencies at the Tropical Rainfall Measuring Mission Microwave Imager frequencies (10.65 to 85.5 GHz) are enhanced greatly for relatively small (approx. 0.1) meltwater fractions. The relatively large number of partially-melted particles just below the freezing level in stratiform regions leads to significant microwave absorption, well-exceeding the absorption by rain at the base of the melting layer. Calculated precipitation backscatter efficiencies at the Precipitation Radar frequency (13.8 GHz) increase in proportion to the particle meltwater fraction, leading to a "bright-band" of enhanced radar reflectivities in agreement with previous studies. The radiative properties of the melting layer are determined by the choice of dielectric models and the initial water contents and material densities of the "seeding" ice-phase precipitation particles. Simulated melting layer profiles based upon snow described by the Fabry-Szyrmer core-shell dielectric model and graupel described by the Maxwell-Garnett water matrix dielectric model lead to reasonable agreement with radar-derived melting layer optical depth distributions. Moreover, control profiles that do not contain mixed-phase precipitation particles yield optical depths that are systematically lower than those observed. Therefore, the use of the melting layer model to extend 3-D CRM simulations appears justified, at least until more realistic spectral methods for describing melting precipitation in high-resolution, 3-D CRM's are implemented.

Olson, William S.↗

DOE OSTI2024

Machine learning the electric field response of condensed phase systems using perturbed neural network potentials

Abstract The interaction of condensed phase systems with external electric fields is of major importance in a myriad of processes in nature and technology, ranging from the field-directed motion of cells (galvanotaxis), to geochemistry and the formation of ice phases on planets, to field-directed chemical catalysis and energy storage and conversion systems including supercapacitors, batteries and solar cells. Molecular simulation in the presence of electric fields would give important atomistic insight into these processes but applications of the most accurate methods such as ab-initio molecular dynamics (AIMD) are limited in scope by their computational expense. Here we introduce Perturbed Neural Network Potential Molecular Dynamics (PNNP MD) to push back the accessible time and length scales of such simulations. We demonstrate that important dielectric properties of liquid water including the field-induced relaxation dynamics, the dielectric constant and the field-dependent IR spectrum can be machine learned up to surprisingly high field strengths of about 0.2 V Å −1 without loss in accuracy when compared to ab-initio molecular dynamics. This is remarkable because, in contrast to most previous approaches, the two neural networks on which PNNP MD is based are exclusively trained on molecular configurations sampled from zero-field MD simulations, demonstrating that the networks not only interpolate but also reliably extrapolate the field response. PNNP MD is based on rigorous theory yet it is simple, general, modular, and systematically improvable allowing us to obtain atomistic insight into the interaction of a wide range of condensed phase systems with external electric fields.

Science & Technology - Other Topics↗

NASA NTRS1982

Measuring the Electrical Properties of Epoxies

Two techniques rapidly determine low-frequency resistivity of conductive epoxies and high-frequency dielectric properties of insulating epoxies. Conductive epoxy is molded in channels in plastic block. Four-point ohmmeter is used to apply current and sense voltage; it reads out resistance. Because mold has precise and stable dimensions, it produces accurate consistent measurements.

Sergent, J. E.↗

DOE OSTI2021

On the molecular correlations that result in field-dependent conductivities in electrolyte solutions

Employing recent advances in response theory and nonequilibrium ensemble reweighting, we study the dynamic and static correlations that give rise to an electric field-dependent ionic conductivity in electrolyte solutions. We consider solutions modeled with both implicit and explicit solvents, with different dielectric properties, and at multiple concentrations. Implicit solvent models at low concentrations and small dielectric constants exhibit strongly field-dependent conductivities. We compare these results to Onsager-Wilson theory of the Wien effect, which provides a qualitatively consistent prediction at low concentrations and high static dielectric constants but is inconsistent away from these regimes. The origin of the discrepancy is found to be increased ion correlations under these conditions. Explicit solvent effects act to suppress nonlinear responses, yielding a weakly field-dependent conductivity over the range of physically realizable field strengths. By decomposing the relevant time correlation functions, we find that the insensitivity of the conductivity to the field results from the persistent frictional forces on the ions from the solvent. Our findings illustrate the utility of nonequilibrium response theory in rationalizing nonlinear transport behavior.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗