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At least 721 records · Page 40

Investigation of Low-Energy Lattice Dynamics and Their Role in Superionic Na Diffusion and Ultralow Thermal Conductivity of Na 3 PSe 4 as a Solid-State Electrolyte

The atomic dynamics of Na 3 PSe 4 were investigated using a combination of neutron scattering experiments and ab initio and machine-learned molecular dynamics simulations to probe the interplay of fast ionic diffusion with atomic vibrations (phonons) of the host lattice. Our results reveal the existence of low-energy vibrational modes, simultaneously involving motions of Na + ions and framework polyanion subunits, and show that these modes become strongly overdamped in the superionic regime as they couple with the Na + hopping process. In particular, the Na+ migration energy landscape is strongly impacted by low-energy phonons derived from a soft acoustic branch of the host lattice, which modulates the diameter of the Na + diffusion channel at the bottleneck. We find that an additional factor for the enhanced Na + conductivity in Na 3 PSe 4 is the presence of Na-vacancies, which also affect the low-frequency dynamics and thermal vibration amplitudes, pointing to an interplay between Na + vacancies and host dynamics, jointly enhancing ionic diffusivity. Finally, we investigate the origin of ultralow thermal conductivities in Na 3 PSe 4 and Na 3 PS 4 using Green–Kubo simulations and find that low-energy acoustic phonon modes of the overall crystal framework provide a dominant contribution to the thermal conductivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Alignment Charts for Transport Properties Viscosity, Thermal Conductivity, and Diffusion Coefficients for Nonpolar Gases and Gas Mixtures at Low Density

Alignment charts (nomographs) designed to permit rapid calculations of the low-pressure transport properties of nonpolar gases and gas mixtures are presented. Calculations for pure gases are based on the rigorous kinetic theory of gases as applied to a realistic intermolecular force law. Mixture viscosities and conductivities are calculated from good approximations derived from rigorous theory. The properties are calculable with a precision of 2 percent or better. Accuracy depends on how well the constants characterizing the Intermolecular force law are known; if constants are derived from experimental data, results should be accurate to 5 percent or better. Force constants are tabulated for 65 gases.

Brokaw, Richard S.↗

Status Report on Photothermal Radiometry Development

Thermal transport properties such as thermal conductivity and diffusivity, are critical parameters in the development of improved nuclear fuels and components. It is well known that thermal transport properties change temporally and spatially due to dynamic microstructural evolution as a result of neutron irradiation. Laser based photothermal techniques are an ideal candidate for thermal properties measurement of irradiated materials because they are non contact, non destructive and can be performed remotely. In this report, we present the progress in the development of a photothermal radiometry (PTR) system to measure the thermal diffusivity of solid samples. The PTR technique measures the local temperature response from a modulated heat source by detecting the sample radiation heat flux. Initially, a well developed thermal wave analytical model was fit to the data to obtain the thermal diffusivity. However, systematic errors from the diffraction effect and non linearity issues resulted in thermal diffusivity measurements higher than literature values. These effects have been studied, an improved analytical model has been developed, and the physics behind the phenomena are still under investigation. A procedure for optimizing measurements from the benchtop system has been provided.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The subsurface hydrologic response of Mars to the thermal evolution of its early crust

The Martian valley networks and outflow channels provide persuasive evidence that large bodies of groundwater were present on Mars throughout much of its early geologic history. However, little attention was focused on how these volatile reservoirs may have responded to the thermal evolution of the early Martian crust. In this regard, one process that has likely been of critical importance to the subsurface hydrologic evolution of Mars is thermal vapor diffusion. Various aspects of the thermal vapor diffusion process on Mars are discussed.

Clifford, S. M.↗

Highly Effective GeNi Alloy Contact Diffusion Barrier for BiSbTe Long-Term Thermal Exposure

A GeNi alloy diffusion barrier for contacts on bismuth antimony telluride is proposed. Multiple gold contact diffusion barriers were tested at different thermal aging conditions in air and reducing atmospheres. Among all diffusion barriers, the GeNi alloy barrier shows the best performance for bulk samples with no substantial degradation of the contact resistance, no contact color change, and no change of thermoelectric properties. We observed D Au–GeNi = (9.8 ± 2.7) × 10 –20 m 2 /s within the GeNi alloy barrier, which is 4 times smaller than D Au–BiSbTe . The presence of the initial Ge layer also proves to be effective in reducing nickel diffusion yielding D Ni–BiSbTe = (8.57 ± 0.49) × 10 –19 m 2 /s. During GeNi alloy formation, Ge diffusion into BiSbTe produces GeTe, which apparently blocks the van der Waals gaps eliminating Au and Ni fast diffusion pathways. Thermal aging of BiSbTe nanowires shows that Au and Ni diffusion degrades the thermoelectric power factor, whereas the GeNi alloy barrier sample is mostly preserved. The GeNi alloy barrier is a reliable solution to long-term thermal applications of BiTe-based materials.

36 MATERIALS SCIENCE↗

Characterization of Grain‐Size Distribution, Thermal Conductivity, and Gas Diffusivity in Variably Saturated Binary Sand Mixtures

Core Ideas Parameterized models are relevant to applications where different porous media mixtures are used. Models include a grain‐size distribution function to describe bimodal behavior for binary mixtures. Improved model describes observed thermal conductivity–saturation relations for binary mixtures. Combined Buckingham–Penman model used to describe observed gas diffusivity–air content relations. This work is relevant for proper simulation of mixed porous media. Characterization of differently textured porous materials, as well as different volumetric porous media mixtures, in relation to mass and heat transport is vital for many engineering and research applications. Functional relations describing physical (e.g., grain‐size distribution, total porosity), thermal, and gas diffusion properties of porous media and mixtures are necessary to optimize the design of porous systems that involve heat and gas transport processes. However, only a limited number of studies provide characterization of soil physical, thermal, and gas diffusion properties and the functional relationships of these properties under varying soil water contents, especially for soil mixtures, complicating optimization efforts. To better understand how mixing controls the physical, thermal, and gas diffusion properties of porous media, a set of laboratory experiments was performed using five volumetric mixtures of coarse‐ and fine‐grained sand particles. For each mixture, the grain‐size distribution (GSD), thermal conductivity, and gas diffusivity were obtained and parameterized using existing and suggested parametric models. Results show that the extended, two‐region Rosin–Rammler particle‐size distribution model proposed in this study could successfully describe the bimodal behavior of the GSD of binary mixtures. Further, the modified Côté and Konrad thermal conductivity model adequately described the thermal conductivity–water saturation relations observed in different mixtures. The proposed simple soil‐gas diffusivity descriptive model parameterized the upper limit, average, and lower limit behavior in gas diffusivity–air content relations in apparently texture‐invariant gas diffusivity data. Results further show a close analogy between gas diffusivity and thermal conductivity and their variation with saturation across different binary mixtures. Overall, the results of the study provide useful numerical insight into the physical, thermal, and gas transport characteristics of binary mixtures, with wide implications for future engineering and research applications that involve multicomponent porous systems.

Deepagoda, T. K. K. Chamindu↗

Studies of the role of metastables and doubly ionized species in the chemical and thermal structure of the Venusian and Martian ionospheres

Models of the upper atmospheres of Mars and Venus were constructed using Viking and Pioneer Venus data. The neutral densities, with the exception of NO, N(4S), N(2D) and N(2P) were taken from the measured values, along with the neutral, ion, and electron temperatures. Using solar fluxes and relevant cross sections, the production rates of ions and neutral fragments by photo and electron impact processes were computed. These production rates were combined with chemical production rates and loss along with one dimensional transport eddy diffusion, molecular and ambi polar diffusion, and thermal diffusion, to determine the densities of ions and odd nitrogen species. Preliminary calculations show that the chemistry of metastables and doubly ionized species is important in the ionospheres of Mars and Venus. Production of N(+) in metastable reactions is particularly important, and it explains the discrepancy between the measurements of earlier models. Production of CO(+) is also affected. Reactions of O(++) and O(+)(2D) with N2 have important consequences for the escape rate of atomic nitrogen from the Martian atmosphere.

Fox, J. L.↗

Structural and chemical disorder enhance point defect diffusion and atomic transport in Ni 3 Al-based γ' phase

The ordered L1 2 γ' Ni 3 Al intermetallic inclusions are routinely used as strengthening constituents in Ni-based superalloys and recent high-entropy alloys. As there are different metallic elements relative to the alloy matrix, the composition of γ' phase inclusions usually suffers some variations. In this work, we studied the elemental partition and its influence on atomic transport properties in a model (NiCo) 3 Al γ' phase with chemical and structural disorder. Combining the Monte Carlo and molecular static techniques, we first determined the elemental distribution in such compositionally-complexed γ' phase. The results suggest that Co tends to segregate, which profoundly influences defect energetics and diffusion properties. By modeling thermally activated diffusion by molecular dynamics, we found that chemical disorder induced by Co can enhance vacancy diffusion while significantly suppress diffusion via interstitial atom migration, as compared to the stoichiometric γ' Ni 3 Al. We further reveal that these observations are closely related to the defect energetics in these systems. Furthermore, our results explain the effects of disorder, long- and short-range orders on the diffusion properties in multicomponent intermetallic alloys, which helps to understand the stability and, thus, γ'-phase-assisted strengthening at different conditions including annealing and irradiation.

36 MATERIALS SCIENCE↗

High-Pressure Transport Properties Of Fluids: Theory And Data From Levitated Drops At Combustion-Relevant Temperatures

Although the high pressure multicomponent fluid conservation equations have already been derived and approximately validated for binary mixtures by this PI, the validation of the multicomponent theory is hampered by the lack of existing mixing rules for property calculations. Classical gas dynamics theory can provide property mixing-rules at low pressures exclusively. While thermal conductivity and viscosity high-pressure mixing rules have been documented in the literature, there is no such equivalent for the diffusion coefficients and the thermal diffusion factors. The primary goal of this investigation is to extend the low pressure mixing rule theory to high pressures and validate the new theory with experimental data from levitated single drops. The two properties that will be addressed are the diffusion coefficients and the thermal diffusion factors. To validate/determine the property calculations, ground-based experiments from levitated drops are being conducted.

Bellan, Josette↗

Ice nucleating particle concentrations measured by the CSU-CFDC during the AGINSGP field experiment

Real-time, immersion mode ambient ice nucleating particle (INP) concentrations were measured at ARM&rsquo;s Southern Great Plains (SGP) site during the AGINSGP field experiment using a continuous flow diffusion chamber (CFDC) from Colorado State University (CSU). The CSU-CFDC is an ice-thermal gradient diffusion chamber that optically detects the freezing of single aerosol particles (Rogers 1988; Rogers et al. 2001; and Eidhammer et al. 2010). The instrument was located in the guest instrument facility (GIF) and measured INP concentrations from April 8th to April 29th. Air was drawn into the GIF through custom aluminum stack inlets (6&rdquo; inner diameter) attached vertically to the outer GIF wall and the GIF outside platform. A blower pulled air through the stacks at a velocity of 1 m/s. Aerosol instruments subsampled via wall ports, through either 3/8&rdquo; or 1/4" copper lines, depending on sample flow of the instrument. Rogers, D. C., Development of a continuous flow thermal gradient diffusion chamber for ice nucleation studies, Atmospheric Research, 22(2), 149-181, doi:10.1016/0169-8095(88)90005-1, 1988. Rogers, D. C., P. J. DeMott, S. M. Kreidenweis and Y. Chen, A continuous flow diffusion chamber for airborne measurements of ice nuclei, J. Atmos. Oceanic Technol., 18, 725-741, doi:10.1175/1520-0426(2001)018<0725:ACFDCF>2.0.CO;2, 2001. Eidhammer, T., DeMott, P. J., Prenni, A. J., Petters, M. D., Twohy, C. H., Rogers, D. C., Stith, J., Heymsfield, A., Wang, Z., Haimov, S., French, J., Pratt, K., Prather, K., Murphy, S., Seinfeld, J., Subramanian, R., and Kreidenweis, S. M., Ice initiation by aerosol particles: Measured and predicted ice nuclei concentrations versus measured ice crystal concentrations in an orographic wave cloud, J. Atmos. Sci., 67, 2417-2436, doi:10.1175/2010JAS3266.1, 2010

54 ENVIRONMENTAL SCIENCES↗

Thermal fluctuations and the diffuse electrostatic emissions

The suggestion that the weak-banded electrostatic emissions observed in the magnetosphere at frequencies between the electron gyrofrequency and upper hybrid frequency are thermal fluctuations is quantitatively explored, by means of a hot-cold model for dayside electron distributions with density and temperature ratios much greater than unity. It is determined that, for typical dayside conditions, the observed waves are weakly damper Bernstein-Harris modes whose spectral density and polarization, perpendicular to the ambient magnetic field, can be accounted for by the theory. It is suggested that the formalism developed may be applicable to weak electron cyclotron emissions at Jupiter and Saturn, and can be extended to lower-frequency ion cyclotron fluctuations by modifying the theory to include ion contributions.

Sentman, D. D.↗

Diffusion wave phenomena

Thermal and bleaching waves as diffusion phenomena in opposite limits, discussing laser heating

Ahlstrom, H. G.↗

Detection of diffusion limited oxidation in thermally aged ethylene propylene rubber cable insulation material

The lifetime prediction of electrical cable insulation in nuclear power plants (NPPs) is primarily based on accelerated aging. Polymeric insulation exposed to accelerated aging at high temperatures may demonstrate diffusion limited oxidation (DLO) where oxygen within the material is consumed faster than can be supplied by diffusion from the surrounding air. This situation leads to equilibrium oxidation at the exposed surfaces and limited oxidation away from the surfaces. Therefore, DLO results in a heterogeneously aged material which can lead to underestimation of lifetime for in-service cable insulation. In this study, the presence of inhomogeneous aging caused by DLO was evaluated on cross-sectioned cable insulation specimens made of ethylene propylene rubber (EPR). The studies were performed on thermally aged specimens (165 °C, 1 day and 165 °C, 16 days) using local measurement techniques including nanoindentation, micro-Fourier transform infrared spectroscopy (FTIR), and scanning electron microscopy (SEM) - energy dispersive spectroscopy (EDS). All the results indicate some degree of heterogenous aging, with 165 °C, 16 days, aging demonstrating highest degree of oxidative degradation on the inside edges presumably caused due to copper catalyzed oxidation.

Pallaka, Madhusudhan Reddy↗

A Monte Carlo Thermal Radiative Transfer Solver with Nonlinear Elimination

Here in this paper, we present a new Monte Carlo method for solving the thermal radiative transfer (TRT) equations via the method of nonlinear elimination (NLEM). This method is inspired by the previous application of NLEM to thermal radiation diffusion. Our approach, called diffusion accelerated Implicit Monte Carlo (DAIMC), is a hybrid technique which combines a Monte Carlo method for solving a purely-absorbing transport equation and a diffusion solution that accounts for effective scattering, or absorption–reemission. The method aims to improve the implicitness of the traditional implicit Monte Carlo (IMC) method. We derive DAIMC generally for 3D Cartesian geometries, but in this paper, we present results and analysis in 1D slab geometry. These preliminary results indicate that DAIMC implementations may provide more accurate and robust TRT solutions than IMC in certain test problems.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗