SEARCH · Search NASA
Results for “principles”
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.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
First-Principles Analysis of Potential-Dependent Proton Coupled Electron Transfer between Polypyridyl–Ruthenium Complexes and Oxygen-Modified Graphene Electrodes
Explore the source record for details and available documents.
First-Principles Analysis of Defect-Mediated Li Adsorption on Graphene
To evaluate the possible utility of single layer graphene for applications in Li ion batteries, an extensive series of periodic density functional theory (DFT) calculations are performed on graphene sheets with both point and extended defects for a wide range of lithium coverages. Consistent with recent reports, it is found that Li adsorption on defect-free single layer graphene is not thermodynamically favorable compared to bulk metallic Li. However, graphene surfaces activated by defects are generally found to bind Li more strongly, and the interaction strength is sensitive to both the nature of the defects and their densities. Double vacancy defects are found to have much stronger interactions with Li as compared to Stone–Wales defects, and increasing defect density also enhances the interaction of the Stone–Wales defects with Li. Li interaction with one-dimensional extended defects on graphene is additionally found to be strong and leads to increased Li adsorption. A rigorous thermodynamic analysis of these data establishes the theoretical Li storage capacities of the defected graphene structures. In some cases, these capacities are found to approach, although not exceed, those of graphite. The results provide new insights into the fundamental physics of adsorbate interactions with graphene defects and suggest that careful defect engineering of graphene might, ultimately, provide anode electrodes of suitable capacity for lithium ion battery applications.
First-Principles Modeling of the Initial Stages of Organic Solvent Decomposition on LixMn2O4(100) Surfaces
Explore the source record for details and available documents.
Prediction of A 2 BX 4 metal-chalcogenide compounds via first-principles thermodynamics
Not Available
Grain growth in U–7Mo alloy: A combined first-principles and phase field study
Grain size is an important factor in controlling the swelling behavior in irradiated U-Mo dispersion fuels. Increasing the grain size in U-Mo fuel particles by heat treatment is believed to delay the fuel swelling at high fission density. In this work, a multiscale simulation approach combining first-principles calculation and phase field modeling is used to investigate the grain growth behavior in U-7Mo alloy. The density functional theory based first-principles calculations were used to predict the material properties of U-7Mo alloy. The obtained grain boundary energies were then adopted as an input parameter for mesoscale phase field simulations. The effects of annealing temperature, annealing time and initial grain structures of fuel particles on the grain growth in U-7Mo alloy were examined. The predicted grain growth rate was compared well with the empirical correlation derived from experiments.
Rigorous force field optimization principles based on statistical distance minimization
We use the concept of statistical distance to define a measure of distinguishability between a pair of statistical mechanical systems, i.e., a model and its target, and show that its minimization leads to general convergence of the model’s static measurable properties to those of the target. We exploit this feature to define a rigorous basis for the development of accurate and robust effective molecular force fields that are inherently compatible with coarse-grained experimental data. The new model optimization principles and their efficient implementation are illustrated through selected examples, whose outcome demonstrates the higher robustness and predictive accuracy of the approach compared to other currently used methods, such as force matching and relative entropy minimization. We also discuss relations between the newly developed principles and established thermodynamic concepts, which include the Gibbs-Bogoliubov inequality and the thermodynamic length.
Lattice Anharmonicity and Thermal Conductivity from Compressive Sensing of First-Principles Calculations
First-principles prediction of lattice thermal conductivity K L of strongly anharmonic crystals is a long-standing challenge in solid state physics. Using recent advances in information science, we propose a systematic and rigorous approach to this problem, compressive sensing lattice dynamics (CSLD). Compressive sensing is used to select the physically important terms in the lattice dynamics model and determine their values in one shot. Non-intuitively, high accuracy is achieved when the model is trained on first-principles forces in quasi-random atomic configurations. The method is demonstrated for Si, NaCl, and Cu 12 Sb 4 S 13 , an earth-abundant thermoelectric with strong phononphonon interactions that limit the room-temperature K L to values near the amorphous limit.
Thermodynamic properties of Ce x Th 1-x O2 solid solution from first-principles calculations
Explore the source record for details and available documents.
Finite temperature effects on the X-ray absorption spectra of lithium compounds: First-principles interpretation of X-ray Raman measurements
We elucidate the role of room-temperature-induced instantaneous structural distortions in the Li K-edge X-ray absorption spectra (XAS) of crystalline LiF, Li{sub 2}SO{sub 4}, Li{sub 2}O, Li{sub 3}N, and Li{sub 2}CO{sub 3} using high resolution X-ray Raman spectroscopy (XRS) measurements and first-principles density functional theory calculations within the eXcited electron and Core Hole approach. Based on thermodynamic sampling via ab initio molecular dynamics simulations, we find calculated XAS in much better agreement with experiment than those computed using the rigid crystal structure alone. We show that local instantaneous distortion of the atomic lattice perturbs the symmetry of the Li 1s core-excited-state electronic structure, broadening spectral line-shapes and, in some cases, producing additional spectral features. The excellent agreement with high-resolution XRS measurements validates the accuracy of our first-principles approach to simulating XAS, and provides both accurate benchmarks for model compounds and a predictive theoretical capability for identification and characterization of multi-component systems, such as lithium-ion batteries, under working conditions.
First-principles study of roles of Cu and Cl in polycrystalline CdTe
Cu and Cl treatments are important processes to achieve high efficiency polycrystalline cadmium telluride (CdTe) solar cells, thus it will be beneficial to understand the roles they play in both bulk CdTe and CdTe grain boundaries (GBs). Using first-principles calculations, we systematically study Cu and Cl-related defects in bulk CdTe. We find that Cl has only a limited effect on improving p-type doping and too much Cl can induce deep traps in bulk CdTe, whereas Cu can enhance p-type doping of bulk CdTe. In the presence of GBs, we find that, in general, Cl and Cu will prefer to stay at GBs, especially for those with Te-Te wrong bonds, in agreement with experimental observations.
Lithium Ion Solvation and Diffusion in Bulk Organic Electrolytes from First-Principles and Classical Reactive Molecular Dynamics
Explore the source record for details and available documents.
Connecting thermoelectric performance and topological-insulator behavior: Bi 2 Te 3 and Bi 2 Te 2 Se from first principles
Thermoelectric performance is of interest for numerous applications such as waste-heat recovery and solid-state energy conversion and will be seen to be closely connected to topological-insulator behavior. In this paper, we here report first-principles transport and defect calculations for Bi 2 Te 2 Se in relation to Bi 2 Te 3 . The two compounds are found to contain remarkably different electronic structures in spite of being isostructural and isoelectronic. We also discuss these results in terms of the topological-insulator characteristics of these compounds.
Impact of first-principles properties of deuterium–tritium on inertial confinement fusion target designs
A comprehensive knowledge of the properties of high-energy-density plasmas is crucial to understanding and designing low-adiabat, inertial confinement fusion (ICF) implosions through hydrodynamic simulations. Warm-dense-matter (WDM) conditions are routinely accessed by low-adiabat ICF implosions, in which strong coupling and electron degeneracy often play an important role in determining the properties of warm dense plasmas. The WDM properties of deuterium–tritium (DT) mixtures and ablator materials, such as the equation of state, thermal conductivity, opacity, and stopping power, were usually estimated by models in hydro-codes used for ICF simulations. In these models, many-body and quantum effects were only approximately taken into account in the WMD regime. Moreover, the self-consistency among these models was often missing. To examine the accuracy of these models, we have systematically calculated the static, transport, and optical properties of warm dense DT plasmas, using first-principles (FP) methods over a wide range of densities and temperatures that cover the ICF “path” to ignition. These FP methods include the path-integral Monte Carlo (PIMC) and quantum-molecular dynamics (QMD) simulations, which treat electrons with many-body quantum theory. The first-principles equation-of-state table, thermal conductivities (κ{sub QMD}), and first principles opacity table of DT have been self-consistently derived from the combined PIMC and QMD calculations. They have been compared with the typical models, and their effects to ICF simulations have been separately examined in previous publications. In this paper, we focus on their combined effects to ICF implosions through hydro-simulations using these FP-based properties of DT in comparison with the usual model simulations. We found that the predictions of ICF neutron yield could change by up to a factor of ∼2.5; the lower the adiabat of DT capsules, the more variations in hydro-simulations. The FP-based properties of DT are essential for designing ICF ignition targets. Future work on first-principles studies of ICF ablator materials is also discussed.
VARIATIONAL PRINCIPLE FOR PLANETARY INTERIORS
In the past few years, the number of confirmed planets has grown above 2000. It is clear that they represent a diversity of structures not seen in our own solar system. In addition to very detailed interior modeling, it is valuable to have a simple analytical framework for describing planetary structures. The variational principle is a fundamental principle in physics, entailing that a physical system follows the trajectory, which minimizes its action. It is alternative to the differential equation formulation of a physical system. Applying the variational principle to the planetary interior can beautifully summarize the set of differential equations into one, which provides us some insight into the problem. From this principle, a universal mass–radius relation, an estimate of the error propagation from the equation of state to the mass–radius relation, and a form of the virial theorem applicable to planetary interiors are derived.
From the Sabatier principle to a predictive theory of transition-metal heterogeneous catalysis
Explore the source record for details and available documents.