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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Predicting mesoscale spectral thermal conductivity using advanced deterministic phonon transport techniques

We present a review, demonstration and simulation of phonon transport for the purposes of predicting materials performance at the mesoscale. We focus primarily on the development and implementation of a unified methodology to enable predictive heat transport. We report on the current state of the art as it pertains to deterministic phonon transport methodologies, discussing various topics concerning phonons. In application, we focus on the Self-Adjoint Angular Flux (SAAF) formulation of the Boltzmann transport equation for phonons, and develop the spatial, angular, and material property discretization required to accurately simulate the predictive physics of heat transport in dielectrics. We discuss thermal interfacial resistance and present our formulation of the diffuse mismatch model for simulating phonon interactions at internal boundaries. We have recently developed a deterministic, spectral phonon transport method for predicting effective thermal conductivity ($\kappa_{\textrm{eff}}$), using Bose-Einstein source terms coupled through an average material temperature. In this method, we introduce a closure term to the phonon transport system which acts as a redistribution function for the total energy of the system, and serves as a guide for the amount of non-equilibrium behavior occurring in the system. This method predicts thermal conductivity and equilibrium temperature distributions in homogeneous and heterogeneous materials using data generated by ab initio density functional theory methods. We employ polarization, density of states and full dispersion spectra to resolve thermal conductivity with numerous angular and spatial discretizations. Our implementation utilizes a Richardson iteration on a modified version of the phonon scattering source. The equations associated with this method are solved via a modification of traditional source iteration. We compare the performance of source iteration applied to an existing uncoupled, traditional SAAF method to our new method and comment on the iterative performance of each. We observe ballistic and diffusive phonon scattering as acoustic thickness of the domain changes, and are able to make comparisons between the accuracy and efficiency of both methods.

36 MATERIALS SCIENCE↗
DOE OSTI2021

A Systematic Way to Extend the Debye–Hückel Theory beyond Dilute Electrolyte Solutions

An extended Debye–Hückel theory with fourth order gradient term is developed for electrolyte solutions; namely, the electric potential φ(r) of the bulk electrolyte solution can be described by ∇ 2 φ(r) = κ 2 φ(r) + L Q 2 ∇ 4 φ(r), where the parameters κ and L Q are chosen to reproduce the first two roots of the dielectric response function of the bulk solution. Three boundary conditions for solving the electric potential problem are proposed based upon the continuity conditions of involving functions at the dielectric boundary, with which a boundary element method for the electric potential of a solute with a general geometrical shape and charge distribution is derived. Solutions for the electric potential of a spherical ion and a diatomic molecule are found and used to calculate their electrostatic solvation energies. In this work, the validity of the theory is successfully demonstrated when applied to binary as well as multicomponent primitive models of electrolyte solutions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Determining the Structure-Property Relationships of Quasi-Two-Dimensional Semiconductor Nanoplatelets.

We report a theoretical study of CdSe nanoplatelets aimed at identifying the main factors determining their photophysical properties. Using atomic configurations optimized with density functional theory calculations, we computed quasiparticle and exciton binding energies of nanoplatelets with two to seven monolayers. We employed many body perturbation theory at the GW level and solved the Bethe-Salpeter equation to obtain absorption spectra and excitonic properties. Our results, which agree well with recent experiments, were then used to design a model that allows us to disentangle the effects of quantum confinement, strain induced by passivating ligands, and dielectric environment on the electronic properties of nanoplatelets. We found that, for the model to accurately reproduce our first principle results, it is critical to account for surface stress and consider a finite potential barrier and energy-dependent effective masses when describing quantum confinement. Our findings call into question previous assumptions on the validity of an infinite barrier to describe carrier confinement in nanoplatelets, suggesting that it may be possible to optimize interfacial charge transfer and extraction by appropriately choosing passivating ligands. The model developed here is generalizable to core-shell platelets and enables the description of system sizes not yet directly treatable by first-principles calculations.

Greenwood, Arin R.↗
NASA NTRS1991

Derivation of mid-infrared (5-25 microns) optical constraints of some silicates and palagonite

This study was initially conceived in order to aid in the interpretation of Martian surface and atmospheric aerosol mineralogy. As a result, the minerals included are biased toward samples which represent hydrated and hydroxylated silicates. Due to their physical particle size, clays and other materials, such as palagonite, cannot be prepared using typical preparation techniques. Yet in some cases, such as for Mars, these are the materials of perhaps the greatest interest. In order to obtain a suitable sample of these less cohesive materials for the laboratory measurements, a KBr pellet die was used and a pellet of the pure sample was prepared. For all clays and the palagonite, a pellet with highly reflective surfaces at visible wavelengths was produced. The reflectivities of all samples were determined, and to derive the optical constants of a materials as a function of wavelength, dispersion analysis was used which describes the real and imaginary indices of refraction as the contributions due to a sum of classical oscillators and relates them via Frensel's equations for non-normal incidence, the the measured near-normal reflectivity. The final values that were determined represent averages of several model fits to each data set using the same number of oscillators by varying the high frequency dielectric constant.

Roush, T. L.↗
DOE OSTI2023

Uniqueness of relaxation times determined by dielectric spectroscopy

Dielectric spectroscopy is extremely powerful to study molecular dynamics, because of the very broad frequency range. Often multiple processes superimpose resulting in spectra that expand over several orders of magnitude, with some of the contributions partially hidden. For illustration, we selected two examples, (i) normal mode of high molar mass polymers partially hidden by conductivity and polarization and (ii) contour length fluctuations partially hidden by reptation using the well-studied polyisoprene melts as example. The intuitive approach to describe experimental spectra and to extract relaxation times is the addition of two or more model functions. Here, we use the empirical Havriliak-Negami function to illustrate the ambiguity of the extracted relaxation time, despite an excellent agreement of the fit with experimental data. We show that there are an infinite number of solutions for which a perfect description of experimental data can be achieved. However, a simple mathematical relationship indicates uniqueness of the pairs of the relaxation strength and relaxation time. Sacrificing the absolute value of the relaxation time enables to find the temperature dependence of the parameters with a high accuracy. For the specific cases studied here, the time temperature superposition (TTS) is very useful to confirm the principle. However, the derivation is not based on a specific temperature dependence, hence, independent from the TTS. We compare new and traditional approaches and find the same trend for the temperature dependence. The important advantage of the new technology is the knowledge of the accuracy of the relaxation times. Relaxation times determined from data for which the peak is clearly visible are the same within the experimental accuracy for traditional and new technology. However, for data where a dominant process hides the peak, substantial deviations can be observed. Finally, we conclude that the new approach is particularly helpful for cases in which relaxation times need to be determined without having access to the associated peak position.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Atomistic models of In and Ga diffusion in Cu(In,Ga)Se 2

To improve the performance of Cu(In,Ga)Se 2 thin-film photovoltaic devices, a robust understanding of the dominant diffusion pathways of the alloy species In and Ga is needed. Here, the most probable defect complexes and mechanisms for In and Ga diffusion are identified with the aid of density functional theory. The binding energies and migration barriers for these complexes are calculated in bulk CuInSe 2 and CuGaSe 2 . Analytic models and kinetic lattice Monte Carlo simulations are employed to predict the diffusivity of In and Ga under variations in composition and temperature. Here, we find that a model based on coulombic interactions between group III antisites and vacancies on the Cu-sublattice produces results that match well with experiment.

14 SOLAR ENERGY↗
NASA NTRS1983

Electromagnetic backscattering from a layer of vegetation - A discrete approach

Electromagnetic backscattering from a layer of vegetation over a flat lossy ground is studied. The vegetated region is composed of leaves which are modeled by lossy circular dielectric discs with prescribed orientation statistics. The mean field in the layer is computed by using the Foldy approximation and a two-variable technique which is valid for small fractional volume. Simple expressions are given for the skin depth of the mean wave. Following this, the distorted Born approximation is used to calculate the co-polarized and cross polarized backscattering coefficients. These are then computed as a function of angle of incidence for different layer depths and leaf configurations.

Lang, R. H.↗
NASA NTRS1995

An experimental study of light scattering by large, irregular particles

The intensity and polarization of light scattered by a variety of types of artificial partices large compared to the wavelength were measured as a function of phase angle. Shape, surface roughness, absorption coefficient, and internal scattering coefficient were varied systematically and their effects studied. Scattering by clear, smooth-surfaced spheres is in quantitative agreement with the predictions of the geometrical optics (ray theory) approximation to physical optics (Mie theory). The phase functions of almost all of the particles measured have both forward and backward scattering lobes. A two-parameter, double Henyey-Greenstein function generally provides reasonably good descriptions of the data, while keeping the number of free parameters to the minimum necessary. On a double Henyey- Greenstein parameter plot all of the particles fall into an L-shaped area of restricted size in which the location is characteristic of the particle type. Formalisms based on the equivalent slab model are also given for estimating the scattering efficiency of a large, irregular particle. For most dielectric particles the transmitted, forward scattered light is partially negatively polarized. It is this component that is respopnsible for the well-known maximum in the polarization curves of planetary regoliths at phase angles around 100 deg. For phase angles between about 30 deg and 70 deg the internally scattered light is found to be randomly polarized in the particles studied here, so that the only contribution to the second component of the Stokes vector is by Fresnel reflection from the particle surface. If this empirical result is general, measurement of the second Stokes vector of the light scattered from a regolith at these angles may provide a method of remotely measuring the mean refractive index.

Mcguire, Audrey F.↗
DOE OSTI2020

Accelerated Modeling of Lithium Diffusion in Solid State Electrolytes using Artificial Neural Networks

Abstract Previous efforts to understand structure‐function relationships in high ionic conductivity materials for solid state batteries have predominantly relied on density functional theory (DFT‐) based ab initio molecular dynamics (MD). Such simulations, however, are computationally demanding and cannot be reasonably applied to large systems containing more than a hundred atoms. Here, an artificial neural network (ANN) is trained to accelerate the calculation of high accuracy atomic forces and energies used during such MD simulations. After carefully training a robust ANN for four and five element systems, nearly identical lithium ion diffusivities are obtained for Li 10 GeP 2 S 12 (LGPS) when benchmarking the ANN‐MD results with DFT‐MD. Applying the ANN‐MD approach, the effect of chlorine doping on the lithium diffusivity is calculated in an LGPS‐like structure and it is found that a dopant concentration of 1.3% maximizes ionic conductivity. The optimal concentration balances the competing consequences of effective atomic radii and dielectric constants on lithium diffusion and agrees with the experimental composition. Performing simulations at the resolution necessary to model experimentally relevant and optimal concentrations would be infeasible with traditional DFT‐MD. Systems that require a large number of simulated atoms can be studied more efficiently while maintaining high accuracy with the proposed ANN‐MD framework.

Rao, Karun K.↗
DOE OSTI2022

Active learning of polarizable nanoparticle phase diagrams for the guided design of triggerable self-assembling superlattices

Polarizable nanoparticles are of interest in materials science because of their rich and complex phase behavior that can be used to engineer nanostructured materials with long-range crystalline order. To understand and rationally navigate the design space of polarizable nanoparticles for self-assembling highly ordered superlattices, we developed a coarse-grained computational model to describe the nanoparticle-nanoparticle interactions in implicit solvent and employ the computationally efficient image method to model many-body polarization interactions. We conducted high-throughput virtual screening over a five-dimensional particle design space spanned by temperature, particle size, particle charge, particle dielectric, and solvent dielectric using enhanced sampling molecular dynamics calculations within an active learning framework to efficiently map out the regions of thermodynamic stability of the self-assembled aggregates. We validate our predictions in comparisons against small angle x-ray scattering measurements of gold nanoparticles surface functionalized with metal chalcogenide ligands. Lastly, we use our validated phase maps to computationally design switchable nanostructured materials capable of triggered assembly and disassembly as a function of temperature and solvent dielectric with potential applications as sensors, smart windows, optoelectronic devices, and in medical diagnostics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Epitaxial SrTiO 3 films with dielectric constants exceeding 25,000

Significance Semiconductor interfaces are among the most important in use in modern technology. The properties they exhibit can either enable or disable the characteristics of the materials they connect for functional performance. While much is known about important junctions involving conventional semiconductors such as Si and GaAs, there are several unsolved mysteries surrounding interfaces between oxide semiconductors. Here we resolve a long-standing issue concerning the measurement of anomalously low dielectric constants in SrTiO 3 films with record high electron mobilities. We show that the junction between doped and undoped SrTiO 3 required to make dielectric constant measurements masks the dielectric properties of the undoped film. Through modeling, we extract the latter and show that it is much higher than previously measured.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Screened Range-Separated Hybrid Functional with Polarizable Continuum Model Overcomes Challenges in Describing Triplet Excitations in the Condensed Phase Using TDDFT

Long range-corrected (LRC) or range-separated hybrid (RSH) functionals where the long-range (LR) limit of electronic interactions is set to the exact exchange have been shown to correct the tendency of traditional density functional theory (DFT) to underestimate the frontier orbital gap. Consequently, the use of such functionals in calculating electronic excited states using linear response based time-dependent DFT (TDDFT) has been successful in correcting the tendency for underestimating the energies of charge transfer states by DFT-based calculations. More recently formulations of functionals that attenuate the LR limit to address condensed-phase effects to polarize the electronic density have been reported. In particular screened RSH (SRSH) combined with polarizable continuum model (PCM) was benchmarked successfully in reproducing the fundamental gap and charge transfer state energies of molecular systems in the condensed phase. Here we use SRSH-PCM to address triplet excited states, and show its success in obtaining correspondence of the low-lying triplet states to the singlet–triplet gap in a similar way that the fundamental orbital gap corresponds to electron removal and addition energies. Importantly, the accuracy of the SRSH-PCM in calculating triplet excitations stands on the polarization consistent framework in addressing the scalar dielectric constant and without affecting the optimal tuning by triplet energies. Finally, the prospect of even further improving the SRSH-PCM accuracy in calculating triplet states can be achieved by optimal tuning on the basis of the spin multiplicity gap.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1984

Remote Sensing of Earth Terrain

Theoretical models that are useful and practical in relating remote sensing data to the important physical parameters characterizing Earth terrain are developed. The development of models that are useful in data analysis and interpretation, scene simulation, and developing new remote sensing approaches and techniques is discussed. Numerous theoretical models that are applicable to the active and passive remote sensing of plowed fields, atmospheric precipitation, vegetation, and snow fields were developed. The radiative transfer theory is used to interpret the active and passive data as a function of rain rate. Both the random medium model and the discrete scatterer model is used to study the remote sensing of vegetation fields. Due to the non-spherical geometry of the scatterers there is strong azimuthal dependence in the observed data. Thus, the anisotropic random medium model and the discrete scatterer model with nonspherical particles was developed. In order to relate the remote sensing data to the actual physical parameters, the scattering of electromagnetic waves from randomly distributed dielectric scatterers was studied. Both the rigorous random discrete scatterer theory and the strong fluctuation theory are used to derive the backscattering cross section in terms of the actual physical parameters and the results agree well with the data obtained from the snow fields.

Kong, J. A.↗
NASA NTRS1985

Water permeation and dielectric breakdown. Water permeability in Pub Tedlar. Pub/Tedlar as a function of temperature and humidity

Moisture transport and dielectric breakdown of polyvinyl butyral (PVB), Tedlar, and PVB/Tedlar composites were addressed. Data for the temperature range between 20 and 80 C showed that the moisture flux through the composite is governed by the slower material; and that the composite permeability is intermediate to those of the component material, as predicted by theory. Data for Tedlar at 71 C, showing the dependence of moisture flux on relative humidity, was also presented. Dielectric breakdown data were less precise and less conclusive. The generally applied theoretical model does not match the experimental data. The PVB/Tedlar composite exhibited greater voltage breakdown resistance than either component. Testing of EVA and EVA/Tedlar composites is underway.

Orehotsky, J.↗
NASA NTRS1984

Microwave dielectric properties of plant materials

Three waveguide transmission systems covering the 1-2, 3.5-6.5, and 7.5-8.5 GHZ bands were used to measure the dielectric properties of vegetation material as a function of moisture content and microwave frequency. The materials measured included, primarily, the leaves and stalks of corn and wheat. Dielectric measurements also were made of the liquid included in the vegetation material after it was extracted from the vegetation by mechanical means. The extracted liquids were found to have an equivalent NaCl salinity of about 10 per mil, which can have a significant effect on the dielectric loss at frequencies below 5 GHz. The results of attempts to model the dielectric constant of the vegetatioon-water mixture in terms of the dielectric constants and volume fractions of its constituent parts (i.e., bulk vegetation, air, bound water, and free water) are discussed. Additionally, measurements of the temporal variations in the total attenuation at 10.2 GHz are presented for a corn canopy and a soybean canopy.

Ulaby, F. T.↗
NASA NTRS1974

The effect of droplets in the air-sea transition zone on the sea brightness temperature

A model is presented which shows that, for a fully developed sea driven by the wind with speeds above 5 m/sec the air in the transition zone immediately above the air-sea interface is mixed with sea water droplets from bursting air bubbles. The absorptive droplet concentration in the zone is assumed to have a profile tapering off from the interface to zero at a certain height. The dielectric constant of the absorptive inhomogeneous droplet profile is thus both a function of the wind speed and the height above the interface. Both the inhomogeneity effect and the absorption-emission effect of the droplet concentration have been considered. Theoretical calculations show that the presence of the absorptive inhomogeneous droplet transition zone significantly increases the sea brightness temperature as wind speed rises. Combined effects of both the droplet areas and the foam areas on sea surface have also been considered.

Tang, C. C. H.↗
DOE OSTI2022

Optical and magneto-optical properties of ferromagnetic monolayer CrBr 3 : A first-principles G W and G W plus Bethe-Salpeter equation study

The discovery of atomically thin two-dimensional (2D) magnetic semiconductors has triggered enormous research interest recently. In this paper, we use first-principles many-body perturbation theory to study a prototypical 2D ferromagnetic semiconductor, monolayer chromium tribromide (CrBr 3 ). With broken time-reversal symmetry, spin-orbit coupling, and excitonic effects included through the full-spinor GW and GW plus Bethe-Salpeter equation (GW-BSE) methods, we compute the frequency-dependent layer polarizability tensor and dielectric function tensor that govern the optical and magneto-optical (MO) properties. In addition, we provide a detailed theoretical formalism for simulating magnetic circular dichroism, MO Kerr effect, and Faraday effect, demonstrating the approach with monolayer CrBr 3 . Due to reduced dielectric screening in 2D and the localized nature of the Cr d orbitals, we find strong self-energy effects on the quasiparticle band structure of monolayer CrBr 3 that give a 3.8 eV indirect bandgap. Also, excitonic effects dominate the low-energy optical and MO responses in monolayer CrBr 3 where a large exciton binding energy of 2.3 eV is found for the lowest bright exciton state with excitation energy at 1.5 eV. We further find that the MO signals demonstrate strong dependence on the excitation frequency and substrate refractive index. Furthermore, our theoretical framework for modeling optical and MO effects could serve as a powerful theoretical tool for future study of optoelectronic and spintronics devices consisting of van der Waals 2D magnets.

36 MATERIALS SCIENCE↗