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DOE OSTI2019

Energy barriers for Pb adatom diffusion on stepped ultrathin Pb(111) quantum nanofilms: First-principles calculations

Various properties of Pb(111) nanofilms, prototypical quantum films, have been studied extensively. However, key ab initio -level energy barriers for Pb adatom diffusion on stepped Pb(111) nanofilm surfaces are still not available. Using first-principles density functional theory, we calculate these barriers for films with thicknesses of few monolayers (ML). We find that two-atom exchange is always much more favorable than direct hopping to cross A- or B-type steps. Ehrlich-Schwoebel (ES) barriers for downward transport to a higher-coordination step-edge site depend strongly on the film thickness. For such transport from 2- to 1-ML terraces, or from 4- to 3-ML terraces, there is no an ES barrier, but large ES barriers of more than 100 meV are found from 3- to 2-ML terraces. We also obtain the barriers for diffusion along the step edges and find that these step-edge barriers are significantly larger than terrace diffusion barriers. In addition, we analyze energetics for diffusion on the top flat surface of a nanofilm supported on a vicinal surface, and thus having underlying buried or ghost steps. We quantify the tilted potential energy surface in both ghost A- and B-step regions separating 2- and 3-ML (as well as 3- and 4-ML) terraces. Finally, consequences are discussed for the growth kinetics of supported Pb nanofilms, where the support does not strongly affect electronic states within the film.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS1999

Material Science Experiments on Mir

This paper describes the microgravity materials experiments carried out on the Shuttle/Mir program. There were six experiments, all of which investigated some aspect of diffusivity in liquid melts. The Liquid Metal Diffusion (LMD) experiment investigated the diffusivity of molten Indium samples at 185 C using a radioactive tracer, In-114m. By monitoring two different gamma ray energies (190 keV and 24 keV) emitted by the samples it was possible to measure independently the diffusion rates in the bulk and at the surface of the samples. The Queens University Experiment in Liquid Diffusion (QUELD) was the furnace facility used to process 213 samples for the five other experiments. These experiments investigated the diffusion, ripening, crystal growth, and glass formation in metal, semiconductor, and glass samples. This facility had the capability to process samples in an isothermal or gradient configuration for varying periods of time at temperatures up to 900 C. Both the LMD and the QUELD furnaces were mounted on the Microgravity Isolation Mount (MIM) which provided isolation from g-jitter. All the microgravity experiments were supported by the Space Acceleration Measurement System (SAMS); a three head three axes acceleration monitoring system which measured and recorded the acceleration environment.

Kroes, Roger L.↗

DOE OSTI2020

Pulsed power accelerator surface Joule heating models

Understanding the effects of contaminant plasmas generated within the Z machine at Sandia is critical to understanding current loss mechanisms. The plasmas are generated at the accelerator electrode surfaces and include desorbed species found in the surface and substrate of the walls. These desorbed species can become ionized. The timing and location of contaminant species desorbed from the wall surface depend non-linearly on the local surface temperature. For accurate modeling, it is necessary to utilize wall heating models to estimate the amount and timing of material desorption. One of these heating mechanisms is Joule heating. In this paper, we propose several extended semi-analytic magnetic diffusion heating models for computing surface Joule heating and demonstrate their effects for several representative current histories. We quantitatively assess under what circumstances these extensions to classical formulas may provide a validatable improvement to the understanding of contaminant desorption timing.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS2005

Application of Glow Discharge Plasma to Alter Surface Properties of Materials

Some polymer materials that are considered important for spaceport operations are rendered noncompliant when subjected to the Kennedy Space Center (KSC) Standard electrostatic testing. These materials operate in stringent environmental conditions, such as high humidity. Treating materials that fail electrostatic testing and altering their surface properties so that they become compliant would result in considerable cost savings. Significant improvement in electrostatic dissipation of Saf-T-Vu PVC after treatment with air Atmospheric Plasma Glow Discharge (APGD) was observed and the material now passed the KSC electrostatic test. The O:C ratio on the surface, as monitored by X-ray Photoelectron Spectroscopy, increased from 0.165 tO 0.275 indicating enhanced oxidation, and surface contact angle measurements decreased from 107.5 to 72.6 showing increased hydrophilicity that accounted for the increased conductivity. Monitoring of the aging showed that the materials hydrophobic recovery resulted in it failing the electrostatic test 30 hours after treatment. This was probably due to the out-diffusion of the added Zn, Ba, and Cd salt stabilizers detected on the surface and/or diffusion of low molecular weight oligomers. On going work includes improving the long term hydrophilicity by optimizing the APGD process with different gas mixtures. Treatment of other spaceport materials is also presented.

Trigwell, Steve↗

NASA NTRS1989

Characterization of Venera 15/16 Geologic Units from Pioneer Venus Reflectivity and Roughness Data

Geologic units have been defined for the surface of Venus from Venera 15/16 image data. A characterization of these geologic units is carried out using information on surface properties derived from Pioneer Venus (PV) reflectivity and rms slope data. The geologic context provided by Venera 15/16 units allows additional, more specific interpretations of surface radar properties to be made. Characterization of Venera units results in the definition of four groups of Venera units: (1) smooth rocky units, 2) rough rocky units, (3) rough high dielectric units, and (4) diffusely scattering units. On the basis of correlations of surface morphology to spatial and statistical distributions in rms slope and reflectivity data, we test models for the origin of the surface properties of some units. We conclude that plains and tectonic units can be contrasted in terms of the average roughness of the surface and that tectonic deformation appears to roughen the surface at 0.5- to 10-m and 5- to 50-cm scales. This tectonic weathering process appears to dominate the erosional regime of Venus. Unlike Earth or Mars, production and transport of soils dominates only a small portion (less than or equal to 5%) of the surface. Some of the Venera units display distinctive spatial and statistical distributions of PV radar data. In particular, apparent low reflectivity in the tesserae appears to be caused by small (5-50 cm) rock fragments on the surface which cause diffuse scattering at Pioneer Venus wavelengths. Analysis of models for the formation of these fragments suggests that they are due to the pervasive deformation undergone by the tesserae. Finally, aspects of this study have been used to extend results of Venera image data analysis southward of 30 deg. N lat, resulting in it prediction of the distribution of tessera. Such results can aid in Magellan investigations.

Bindschadler, D. L.↗

DOE OSTI2024

Tracking surface charge dynamics on single nanoparticles

Surface charges play a fundamental role in physics and chemistry, in particular in shaping the catalytic properties of nanomaterials. However, tracking nanoscale surface charge dynamics remains challenging due to the involved length and time scales. Here, we demonstrate time-resolved access to the nanoscale charge dynamics on dielectric nanoparticles using reaction nanoscopy. We present a four-dimensional visualization of the spatiotemporal evolution of the charge density on individual SiO 2 nanoparticles under strong-field irradiation with femtosecond-nanometer resolution. The initially localized surface charges exhibit a biexponential redistribution over time. Our findings reveal the influence of surface charges on surface molecular bonding through quantum dynamical simulations. We performed semi-classical simulations to uncover the roles of diffusion and charge loss in the surface charge redistribution process. Understanding nanoscale surface charge dynamics and its influence on chemical bonding on a single-nanoparticle level unlocks an increased ability to address global needs in renewable energy and advanced health care.

74 ATOMIC AND MOLECULAR PHYSICS↗

NASA NTRS1984

An improved thermal model for cometary nuclei

A thermal model for cometary nuclei is presented and used in comparisons of predictions with data on Halley's comet. The model considers the surface boundary conditions and heat diffusion equations, the sublimation rate of ice, the energy balance, and the dust production rate. Projections were made for the Halley nucleus over 18 latitudes from -85 to +85 deg, from 185 d before to 110 d after perihelion, and in 20 layers of its surface in 1.3 cm increments. Sublimation is predicted to increase by a factor of 2.2 every orbit, thereby allowing 320 returns for a nucleus with a coma, 710 returns with a bare ice nucleus. The gas production during the Giotto intercept at 0.9 AU will be 4.4 x 10 to the 29th molecules/sec, close to an estimate made during the 1910 return.

Weissman, P. R.↗

NASA NTRS1979

Volcanic features of Io

The various volcanic landforms observed on Io by Voyager 1 are described and compared with similar features on earth. Ionian calderas, observed to cover 5% of the surface, are generally found to be of low relief, similar to certain terrestrial calderas. Flow patterns observed include dark, linear markings with lobate margins resembling terrestrial lava flows, bright lobate markings originating at calderas, and a bright flow feature surrounding the calderas. Positive relief features associated with volcanic structures include pancake-like constructions similar to low volcanic cones, sheet-like structures, rugged mountains, and a type of surface upheaval. Bright and dark diffuse markings have also been found. The implications of the high rates of volcanic activity and the apparent abundance of sulfur on Io for the type of volcanism observed are discussed, and it is concluded that while there are strong arguments for sulfur flows on the surface of Io, silicate volcanism of the type observed on earth may also occur.

Carr, M. H.↗

NASA NTRS1984

Surface-slip equations for low-Reynolds-number multicomponent gas flows

Equations have been obtained for jump (or slip) in the wall values of species concentration, pressure, velocity, and temperature for the low-Reynolds-number high-altitude flight regime of a space vehicle. The analysis, based on the Chapman-Enskog method as applied by Shidlovskiy for a single-species gas, includes multicomponent diffusion with finite-rate surface catalytic recombination. A consistent set of equations is provided for multicomponent, binary, and single species mixtures.

Gupta, R. N.↗

NASA NTRS1984

Surface-slip equations for low-Reynolds-number multicomponent gas flows

Gupta, R. N.↗

NASA NTRS1972

Roughness effects on radiant heat transfer between interacting surfaces.

The radiative transfer between interacting plates with rough surfaces is analyzed on the basis of Beckman's (1963) rough-surface bidirectional reflectance model and, for comparison, on the basis of a direction-dependent specular reflection property model and an approximate rough surface model which assumes a diffuse distribution of the scattered energy. It is found that the overall heat transfer obtained with the Beckman model is only slightly (1.5%) less than that obtained with the direction-dependent specular reflection model. Furthermore, constant property specular reflection analysis gave results within 3% of the rough surface values. The region of uncertainty for the rough surface flux increases, however, as optical roughness increases.

Houchens, A. F.↗

NASA NTRS1980

Fabrication and evaluation of brazed titanium-clad Borsic/aluminum compression panels

Processes for brazing Borsic/aluminum composite materials that eliminate diffusion of braze alloy constituents into the aluminum matrix developed. One brazing study led to the development of a hybrid composite which combines high strength Borsic/aluminum and ductile titanium to form a material identified as titanium clad Borsic/aluminum. The titanium foil provides the Borsic/aluminum with a durable outer surface and serves as a diffusion barrier which alleviates fiber and matrix degradation during brazing. Titanium clad Borsic/aluminum skin panels were joined to titanium clad Borsic/aluminum stringers by brazing and were tested in end compression at room and elevated temperatures. The data include failure strength, buckling strength, and the effects of brazing on the material properties. Predicted buckling loads are compared with experimental data.

Royster, D. M.↗

NASA NTRS1982

Effective temperatures and luminosities of very hot o-type subdwarfs

Twelve very hot O-type subdwarfs were observed with the IUE-satellite in the low dispersion mode. Temperatures were derived from the slopes of the UV continua and distances were estimated from the color excesses. Most of them are hotter than 60,000 K, i.e., they are the hottest known subdwarfs. From their spectral appearance and location in a H.R.-diagram they form a rather inhomogeneous group. Three of them turned out to be central stars or nearly central stars, and four are definitely near the white dwarf stage. The surface helium to hydrogen ratio varies from about normal to the extreme case. Most of them appear to be post EHB objectives of 0.5 solar mass with a helium burning shell as their energy source, and their peculiar helium-to-hydrogen ratios are most likely the result of diffusion and convective mixing in surface layers.

Schoenberner, D.↗

NASA NTRS1984

Effective temperatures and luminosities of very hot O type subdwarfs

Twelve very hot O-type subdwarfs were observed with the IUE-satellite in the low dispersion mode. Temperatures were derived from the slopes of the UV continua and distances were estimated from the color excesses. Most of them are hotter than 60,000 K, i.e., they are the hottest known subdwarfs. From their spectral appearance and location in a H.R.-diagram, they form a rather inhomogeneous group. Three of them turned out to be central stars or nearly central stars, and four are definitely near the white dwarf stage. The surface helium to hydrogen ratio varies from about normal to the extreme case. Most of them appear to be post EHB objectives of 0.5 solar mass with a helium burning shell as their energy source, and their peculiar helium-to-hydrogen ratios are most likely the result of diffusion and convective mixing in surface layers. Previously announced in STAR as N83-23254

Schonberner, D.↗

DOE OSTI2018

Theory of Carbon Dioxide Absorption by Hanford Waste - 18208

Hanford nuclear waste has a very high pH, and Hanford tanks are ventilated with air. Air has CO{sub 2(g)} in it, which is an acid, so it has some affinity for the waste. The absorption of CO{sub 2} by the waste is important because CO{sub 2} absorption consumes hydroxide at the liquid-air interface, and the hydroxide is important for inhibiting tank corrosion. NaOH is periodically added to some tanks in order to mitigate the surface acidification. The NaOH added then becomes part of the waste and must be treated as waste, increasing the cost of the mission. The Hobbs Equation, developed at the Savannah River site, is used at Hanford to predict CO{sub 2} absorption from the tank ventilation system. In this study, the Hobbs Equation functional form is theoretically evaluated from thermodynamic calculations of CO{sub 2} absorption, and diffusion rates in the waste surface. This study theoretically justifies the empirical equation reported by Hobbs. Thermodynamic calculations performed using the Environmental Simulation Program (ESP) software on a typical double-shell tank waste composition indicate that essentially 100 % of CO{sub 2} that contacts the waste will react with the waste whenever the pH is above 10. In the 1990's, a substantial amount of data was collected on the concentration of CO{sub 2} in the off-gas of ventilated double-shell tanks at Hanford. This historic data was mined in order to determine the quantity of CO{sub 2} absorbed by the waste. The results of this data mining activity determined that tanks below approximately pH 10 (i.e., tank 241-AN-107) will show limited CO{sub 2} absorption, consistent with both the Hobbs model and the theory developed here. Two other tank with higher pH showed contrasting CO{sub 2} absorption. One showed substantial CO{sub 2} absorption, and the other showed minimal CO{sub 2} absorption despite the high waste pH in one tank, presumably because there was minimal contact between the waste surface and most of the air flow. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Environmental Protection Coating System for Refractory Metal Alloys (EPCS for RMAs)

As part of ARPA-E’s Ultra High Temperature Impervious Materials Advancing Turbine Efficiency (UITIMATE) program, this project aims to develop an environmental protection coating system (EPCS) for refractory metal alloys (RMAs) – which will provide radical improvement in long term protection for ultra-high temperature refractory metal components in harsh gas-turbine environments. The drive for higher fuel efficiency and higher core power of gas turbines used in electric power generation and in aircraft propulsion requires higher peak operation temperatures. The temperature capability of state-of-the-art materials cannot meet the new requirements. Refractory metal alloys have desirable capabilities for achieving the required peak temperatures, but most of them are subject to oxidation in the gas turbine environment. Thus, there is a strong need to develop novel environmental protective coatings that enable the refractory metals to operate in an ultra-high temperature engine environment. This project is composed of four major technical innovations that can provide a potentially transformational solution in providing environmental protection for refractory metal alloys over a wide range of temperature. 1) Multi-layer self-healing environmental barrier coating (EBC) that provides protection against combustion gas environment. 2) Oxidation resistant diffusion barrier (DB) on the alloy surface to enhance coating stability. 3) Synergistic integration of the multi-layer self-healing EBC with the diffusion barrier to extend coating life. 4) Guidance of physics-based modeling to accelerate coating development and optimization. Our team has successfully developed a multi-layer self-healing environmental protection coating system (EPCS) that can provide oxidation protection for commercially available molybdenum based refractory metal alloys over a wide temperature range of up to 1600 °C for fuel-efficient gas turbine applications. The team also developed a multi-layer high temperature coating design tool to accelerate coating development and optimization based on physics-based modeling. The team also engaged RTX business unite, notable Pratt and Whitney, for future commercialization of this technology. The successful completion of this Phase I effort led to the selection of performing Phase II of the program. In Phase II, the team plans to apply the EPCS in the protection of a newly discovered molybdenum-based metal alloy which has the potential of superior high temperature properties to the commercial products. Th coating will be evaluated under test conditions and environment that mimic gas turbine operation.

36 MATERIALS SCIENCE↗

NASA NTRS1996

Observing large-scale solar surface flows with GONG: Investigation of a key element in solar activity buildup

The Global Oscillation Network Group (GONG) solar telescope network has begun regular operations, and will provide continuous Doppler images of large-scale nearly-steady motions at the solar surface, primarily those due to supergranulation. Not only the Sun's well-known magnetic network, but also flux diffusion, dispersal, and concentration at the surface appear to be controlled by supergranulation. Through such magnetoconvective interactions, magnetic stresses develop, leading to solar activity. We show a Doppler movie made from a 45.5 hr time series obtained 1995 May 9-10 using data from three of the six GONG sites (Learmonth, Tenerife, Tucson), to demonstrate the capability of this system.

Beck, John G.↗

DOE OSTI2020

Exploring the Role of Inorganic and Organic Interfaces on CO 2 and CH 4 Partitioning: Case Study of Silica, Illite, Calcite, and Kerogen Nanopores on Gas Adsorption and Nanoscale Transport Behaviors

The adsorption, partitioning, and diffusion of CO 2 and CH 4 in organic–inorganic pores composed of kerogen with silica, illite, or calcite are studied using density functional theory and classical molecular dynamics simulations. The adsorption and partitioning behavior of CO 2 and CH 4 molecules is found to be a function of chemistry of the solid interface, pore size, and surface area. CO 2 molecules are preferentially adsorbed compared to CH 4 molecules on silica, illite, calcite, and kerogen surfaces due to significant contributions of electrostatic interactions with the atoms of the associated surfaces. CO 2 and CH 4 molecules display higher adsorption energy on calcite and silica compared to those on illite and kerogen because of enhanced interactions with the positively charged calcium ions on the calcite surface and the hydroxyl group (-OH) on the silica surface. Enhanced internal nanopores and the availability of adsorption active sites in illite and kerogen matrices aid in higher partitioning of the gas molecules into these pores. CO 2 has a significant influence on the clustering and swelling of kerogen fragments compared to CH 4 . Higher CO 2 adsorption on inorganic and kerogen surfaces results in lower overall self-diffusivities compared to CH 4 . This study illustrates surface and pore size controls on the adsorption, partitioning, and self-diffusivities of CO 2 and CH 4 at conditions relevant for subsurface energy applications. The chemistry of the surfaces along with the availability of internal pores and active adsorption sites influences the adsorption behavior of gases. Our results suggest that CO 2 stored in depleted gas reservoirs may preferentially inhabit nanoconfined pores.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗