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DOE OSTI2017

Holey two-dimensional transition metal oxide nanosheets for efficient energy storage

Transition metal oxide nanomaterials are promising electrodes for alkali-ion batteries owing to their distinct reaction mechanism, abundant active sites and shortened ion diffusion distance. However, detailed conversion reaction processes in terms of the oxidation state evolution and chemical/mechanical stability of the electrodes are still poorly understood. Herein we explore a general synthetic strategy for versatile synthesis of various holey transition metal oxide nanosheets with adjustable hole sizes that enable greatly enhanced alkali-ion storage properties. We employ in-situ transmission electron microscopy and operando X-ray absorption structures to study the mechanical properties, morphology evolution and oxidation state changes during electrochemical processes. We find that these holey oxide nanosheets exhibit strong mechanical stability inherited from graphene oxide, displaying minimal structural changes during lithiation/delithiation processes. Furthermore, these holey oxide nanosheets represent a promising material platform for in-situ probing the electrochemical processes, and could open up opportunities in many energy storage and conversion systems.

25 ENERGY STORAGE↗

DOE OSTI2016

Exceptional energy and new insight with a sodium–selenium battery based on a carbon nanosheet cathode and a pseudographite anode

We created a unique sodium ion battery (NIB, SIB) cathode based on selenium in cellulose-derived carbon nanosheets (CCNs), termed Se-CCN. The elastically compliant two-dimensional CCN host incorporates a high mass loading of amorphous Se (53 wt%), which is primarily impregnated into 1 cm 3 g -1 nanopores. The results in facile sodiation kinetics due to short solid-state diffusion distances and a large charge transfer area of the nanosheets were established. The architecture also leads to an intrinsic resistance to polyselenide shuttle and to disintegration/coarsening. As a Na half-cell, the Se-CCN cathode delivers a reversible capacity of 613 mA h g -1 with 88% retention over 500 cycles. The exceptional stability is achieved by using a standard electrolyte (1 M NaClO4 EC-DMC) without secondary additives or high salt concentrations. The rate capability is also superb, achieving 300 mA h g -1 at 10C. Compared to recent state-of-the-art literature, the Se-CCN is the most cyclically stable and offers the highest rate performance. As a Se–Na battery, the system achieves 992 W h kg -1 at 68 W kg -1 and 384 W h kg -1 at 10144 W kg -1 (by active mass in a cathode). We are the first to fabricate and test a Se-based full NIB, which is based on Se-CCN coupled to a Na intercalating pseudographitic carbon (PGC) anode. It is demonstrated that the PGC anode increases its structural order in addition to dilating as a result of Na intercalation at voltages below 0.2 V vs. Na/Na+. The {110} Na reflections are distinctly absent from the XRD patterns of PGC sodiated down to 0.001 V, indicating that the Na metal pore filling is not significant for pseudographitic carbons. Lastly, the battery delivers highly promising Ragone chart characteristics, for example yielding 203 and 50 W h kg -1 at 70 and 14 000 W kg -1 (via total material mass in the anode and cathode).

25 ENERGY STORAGE↗

DOE OSTI2017

Water dynamics in hydrated amorphous materials: a molecular dynamics study of the effects of dehydration in amorphous calcium carbonate

Amorphous calcium carbonate (ACC) is often a critical transient phase in the formation of crystalline phases of CaCO 3 via dehydration of hydrated ACC. The behavior of the water molecules plays a pivotal role in this transformation. We report here the dynamics of water molecules in ACC at hydration levels from CaCO 3 ·1H 2 O to CaCO 3 ·0.25H 2 O using molecular dynamics (MD) simulations. Due to the presence of highly hydrophilic Ca 2+ and the strong H-bond acceptor CO 3 2- , most of the water molecules in our simulations have restricted translational and orientational dynamics. These are referred here as ‘slow water’. However, a small fraction of them show high diffusivity at all hydration states and are referred here as ‘fast water’. The computed diffusion coefficients of the slow waters, as extrapolated from simulation results, yield diffusion distances of the order of μm on the 1 hour time scale, consistent with rapid dehydration of ACC nano-particles in the laboratory. We correlate our fast waters with the water molecules in the percolating water-rich, Ca 2+ -deficient nano-pores in the structure of Goodwin et al. [Chem. Mater., 2010, 22, 3197], obtained by analysis of X-ray scattering data, and our slow waters with those in the Ca 2+ -rich volumes with less water in their model. The fast waters can be considered to be free rotors on the ns time scale and have orders of magnitude shorter rotational relaxation times than the slow waters.

Saharay, Moumita↗

DOE OSTI2020

A 3D nm-thin biomimetic membrane for ultimate molecular separation

Multi-functional membranes with high permeance and selectivity that can mimic nature's designs have tremendous industrial and bio-medical applications. In this paper, we report a novel concept of a 3D nanometer (nm)-thin membrane that can overcome the shortcomings of conventional membrane structures. Our 3D membrane is composed of two three-dimensionally interwoven channels that are separated by a continuous nm-thin amorphous TiO 2 layer. This 3D architecture dramatically increases the surface area by 6000 times, coupled with an ultra-short diffusion distance through the 2–4 nm-thin selective layer that allows for ultrafast gas and water transport, ~900 l m –2 h –1 bar –1 . The 3D membrane also exhibits a very high ion rejection (R ~ 100% for potassium ferricyanide) due to the combined size- and charge-based exclusion mechanisms. The combination of high ion rejection and ultrafast permeation makes our 3DM superior to the state-of-the-art high-flux membranes whose performances are limited by the flux-rejection tradeoff. Furthermore, its ultimate Li+ selectivity over polysulfide or gas can potentially solve major technical challenges in energy storage applications, such as lithium–sulfur or lithium–O 2 batteries.

36 MATERIALS SCIENCE↗

DOE OSTI2013

Self-propagating reactions in Al/Zr multilayers: Anomalous dependence of reaction velocity on bilayer thickness

High temperature, self-propagating reactions are observed in vapor-deposited Al/Zr multilayered foils of overall atomic ratios 3 Al:1 Zr and 2 Al:1 Zr and nanoscale layer thicknesses; however, the reaction velocities do not exhibit the inverse dependence on bilayer thickness that is expected based on changes in the average diffusion distance. Instead, for bilayer thicknesses of 20-30 nm, the velocity is essentially constant at ∼7.7 m/s. We explore several possible explanations for this anomalous behavior, including microstructural factors, changes in the phase evolution, and phase transformations in the reactant layers, but find no conclusive explanations. We determine that the phase evolution during self-propagating reactions in foils with a 3 Al:1 Zr stoichiometry is a rapid transformation from Al/Zr multilayers to the equilibrium intermetallic Al{sub 3}Zr compound with no intermediate crystalline phases. This phase evolution is the same for foils of 90 nm bilayer thicknesses and foils of bilayer thicknesses in the range of 27 nm to 35 nm. Further, for foils with a bilayer thickness of 90 nm and a 3 Al:1 Zr overall chemistry, the propagation front is planar and steady, in contrast to unsteady reaction fronts in foils with 1 Al:1 Zr overall chemistry and similar bilayer thicknesses.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Ab-initio calculation study on the formation mechanism of boron-oxygen complexes in c-Si

Boron-oxygen (B-O) complex in crystalline silicon (c-Si) solar cells is responsible for the light-induced efficiency degradation of solar cell. However, the formation mechanism of B-O complex is not clear yet. By Ab-initio calculation, it is found that the stagger-type oxygen dimer (O{sub 2i}{sup st}) should be the component of B-O complex, whose movement occurs through its structure reconfiguration at low temperature, instead of its long-distance diffusion. The O{sub 2i}{sup st} can form two stable “latent centers” with the B{sub s}, which are recombination-inactive. The latent centers can be evolved into the metastable recombination centers via their structure transformation in the presence of excess carriers. These results can well explain the formation behaviors of B-O complexes in c-Si.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Photogenerated carriers transport behaviors in L-cysteine capped ZnSe core-shell quantum dots

The photoexcited carrier transport behavior of zinc selenide (ZnSe) quantum dots (QDs) with core–shell structure is studied because of their unique photoelectronic characteristics. The surface photovoltaic (SPV) properties of self-assembled ZnSe/ZnS/L-Cys core–shell QDs were probed via electric field induced surface photovoltage and transient photovoltage (TPV) measurements supplemented by Fourier transform infrared, laser Raman, absorption, and photoluminescence spectroscopies. The ZnSe QDs displayed p-type SPV characteristics with a broader stronger SPV response over the whole ultraviolet-to-near-infrared range compared with those of other core–shell QDs in the same group. The relationship between the SPV phase value of the QDs and external bias was revealed in their SPV phase spectrum. The wide transient photovoltage response region from 3.3 × 10{sup −8} to 2 × 10{sup −3} s was closely related to the long diffusion distance of photoexcited free charge carriers in the interfacial space–charge region of the QDs. The strong SPV response corresponding to the ZnSe core mainly originated from an obvious quantum tunneling effect in the QDs.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2015

Characterization of extended channel bioreactors for continuous-flow protein production

In this paper, protein based therapeutics are an important class of drugs, used to treat a variety of medical conditions including cancer and autoimmune diseases. Requiring continuous cold storage, and having a limited shelf life, the ability to produce such therapeutics at the point-of-care would open up new opportunities in distributing medicines and treating patients in more remote locations. Here, the authors describe the first steps in the development of a microfluidic platform that can be used for point-of-care protein synthesis. While biologic medicines, including therapeutic proteins, are commonly produced using recombinant deoxyribonucleic acid (DNA) technology in large batch cell cultures, the system developed here utilizes cell-free protein synthesis (CFPS) technology. CFPS is a scalable technology that uses cell extracts containing the biological machinery required for transcription and translation and combines those extracts with DNA, encoding a specific gene, and the additional metabolites required to produce proteins in vitro. While CFPS reactions are typically performed in batch or fed-batch reactions, a well-engineered reaction scheme may improve both the rate of protein production and the economic efficiency of protein synthesis reactions, as well as enable a more streamlined method for subsequent purification of the protein product—all necessary requirements for point-of-care protein synthesis. In this work, the authors describe a new bioreactor design capable of continuous production of protein using cell-free protein synthesis. The bioreactors were designed with three inlets to separate reactive components prior to on-chip mixing, which lead into a long, narrow, serpentine channel. These multiscale, serpentine channel bioreactors were designed to take advantage of microscale diffusion distances across narrow channels in reactors containing enough volume to produce a therapeutic dose of protein, and open the possibility of performing these reactions continuously and in line with downstream purification modules. Here, the authors demonstrate the capability to produce protein over time with continuous-flow reactions and examine basic design features and operation specifications fundamental to continuous microfluidic protein synthesis.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2017

Catalytic and Transport Behaviors of Model and Porous and Composite Nanostructures

As stressed in the Basic Energy Sciences Advisory Committee (BESAC) Report “New Science for a Secure and Sustainable Energy Future” (December 2008), solving our Nation’s energy challenges will entail more than incremental changes in present materials-related technologies; new, advanced routes to nanostructured materials with transformational properties will be required. Herein we describe the design and fabrication of a hybrid biotic/abiotic membrane reactor that, mimicking natural systems, employs the metalloenzyme, carbonic anhydrase, to separate CO 2 from N 2 with unprecedented purity and rate. The membrane design, synthesis, and operation are based on multiple biomimetic and nanoscale fabrication strategies, nanoscale dimensional features, and nanoscale physical phenomena, for example: 1) Bottom-up self-assembly of a membrane comprising a periodic, aligned, cylindrical nanopore array with 8 nm diameter pores designed to accommodate carbonic anhydrase (CA) enzymes 2) Top-down Atomic Layer Deposition (ALD) and plasma processing of the nanopore array to create 18nm deep (by 8nm in diameter) superhydrophilic pores bounded by hydrophobic/superhydrophobic interfaces 3) Formation of a continuous, defect free, ultra-thin (~18-nm thick) but strong water membrane by capillary condensation within the uniformly-sized, superhydrophilic nanopore array 4) Accommodation of CA within the water filled nanopore array (~2 CAs per hydrophilic pore channel) to achieve an effective CA concentration within the 18-nm thick water membrane over 10X greater than achievable in solution Exposed to a mixture of CO 2 and N 2 this biomimetic membrane rapidly and selectively dissolves CO 2 within the CA filled water nano-channels on the ‘upstream side’ and regenerates CO 2 at the superhydrophobic interface on the ‘downstream’ side. In combination, the high CA concentration and exceptionally short diffusion distances enable rapid and highly selective CO 2 separation from N 2 and H 2 . Our membrane has a combined CO 2 flux and selectivity that exceed by orders of magnitude all existing CO 2 membranes and for the first time meet the US Department of Energy guidelines for CO 2 sequestration technologies. (The performance of our membrane was recognized by an R&D100 Award and the first R&D100 Green Technology Award in 2015 and an issued US Patent in 2017). We believe this membrane could be employed in combination with sequestration to help reduce greenhouse gas emissions and provide a viable, economically feasible pathway to achieve the goals of the 2016 Paris Accord, which aims to maintain a global temperature rise this century less than 2°C above pre-industrial levels. Further this membrane concept could be adapted to other enzymes to accomplish other separations of interest, e.g. H 2 . We also have established processing-structure-property relationships of ultrathin membrane-like monolayer materials that are intrinsically catalytic. Establishing processing-structure-property relationships for monolayer materials is crucial for a vast range of applications spanning optics, catalysis, electronics, and energy. Presently, for MoS 2 , a promising catalyst for artificial photosynthesis, considerable debate surrounds the structure/property relationships of its various allotropes. Using high-resolution transmission electron microscopy supported by density functional theory, we unambiguously solved the structure of MoS 2 monolayers and showed lithium intercalation to direct a preferential transformation of the basal plane from 2H (trigonal prismatic) to 1T’ (clustered Mo). These changes alter the energetics of MoS 2 interactions with hydrogen ((GH), and, with respect to catalysis, the 1T’ transformation renders the normally inert basal plane amenable towards hydrogen adsorption and H 2 evolution achieving Hydrogen Evolution Reaction (HER) catalytic activity comparable to 2H MoS 2 edges on Au(111), one of the most active HER catalysts known.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2018

Thermally and chemically responsive nanoporous materials for efficient capture of fission product gases.

The objective of this project was to develop robust, high-efficiency materials for capture of fission product gases such as He, Xe and Kr in scenarios relevant for both reactor fuels and reprocessing operations. The relevant environments are extremely harsh, encompassing temperatures up to 1500 °C, high levels of radiation, as well as potential exposures to highly-reactive chemicals such as nitric acid and organic solvents such as kerosene. The requirement for nanostructured capture materials is driven in part by the very short (few micron) diffusion distances for product gases in nuclear fuel. We achieved synthesis, characterization and detailed modeling of the materials. Although not all materials reviewed in this report will be feasible for the ultimate goal of integration in nuclear fuel, nevertheless each material studied has particular properties which will enable an optimized material to be efficiently developed and characterized.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Limiting Retained Austenite Decomposition in Quenched and Tempered Steels: Influences of Rapid Tempering and Silicon

Tempering reactions are critical to microstructure and property control in martensitic steels. Here, retained austenite decomposition and cementite precipitation are monitored using Mössbauer spectroscopy in 4340 and 300-M steel under conventional and rapid tempering conditions. Tempering times are compared at a constant tempered hardness by increasing tempering temperatures associated with short time conditions to achieve equivalent matrix softening to that of longer tempering times. Time-temperature combinations that provide equivalent tempered hardness generated microstructures with similar dislocation densities and cementite precipitation fractions; these mechanisms are controlled by self-diffusion. However, systematic differences in retained austenite content were observed at a given degree of softening, where shorter tempering times exhibited higher levels of retained austenite compared to more conventional conditions. At low temperatures, the differences in retained austenite preservation between explored time-temperature conditions are attributed to corresponding differences in carbon diffusion distance (in austenite), the controlling diffusional process of retained austenite decomposition. At higher temperatures, retained austenite decomposition exhibits C-curve kinetic behavior in 4340. Thus, reduced thermodynamic driving force for cementite and ferrite formation at higher temperature is believed to play a role in restricting retained austenite decomposition within some short-time, high temperature tempering regimes. The addition of silicon pushes cementite precipitation and retained austenite decomposition to higher temperatures, although retained austenite decomposition is suppressed to a greater extent than cementite precipitation. Potential is illustrated for coupling rapid tempering with silicon alloying to produce appreciably tempered martensite (~490 HV) with relatively less retained austenite decomposition compared to conventional tempering conditions.

36 MATERIALS SCIENCE↗

DOE OSTI2018

The Ability of Soil Pore Network Metrics to Predict Redox Dynamics Is Scale Dependent

Variations in microbial community structure and metabolic efficiency are governed in part by oxygen availability, which is a function of water content, diffusion distance, and oxygen demand; for this reason, the volume, connectivity, and geometry of soil pores may exert primary controls on spatial metabolic diversity in soil. Here, we combine quantitative pore network metrics derived from X-ray computed tomography (XCT) with measurements of electromotive potentials to assess how the metabolic status of soil depends on variations of the overall pore network architecture. Contrasting pore network architectures were generated using a Mollisol—A horizon, and compared to intact control samples from the same soil. Mesocosms from each structural treatment were instrumented with Pt-electrodes to record available energy dynamics during a regimen of varying moisture conditions. We found that volume-based XCT-metrics were more frequently correlated with metrics describing changes in available energy than medial-axis XCT-metrics. An abundance of significant correlations between pore network metrics and available energy parameters was not only a function of pore architecture, but also of the dimensions of the sub-sample chosen for XCT analysis. Pore network metrics had the greatest power to statistically explain changes in available energy in the smallest volumes analyzed. Our work underscores the importance of scale in observations of natural systems.

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS1985

Dendritic solidification. III - Some further refinements to the model for dendritic growth under an imposed thermal gradient

Some further refinements to a simple model for dendritic solidification in a binary alloy melt under an imposed positive thermal gradient are presented. Two new expressions for the dendrite tip undercooling have been obtained and shown to yield a limiting value of Delta T sub 0 and very small growth rates. Here Delta T sub 0 is the equilibrium solidification range of the alloy. At very large growth rates, all three tip undercooling expressions reach the same limiting value depending on the value of a dimensionless parameter lambda which is related to the effective diffusion distance ahead of the dendrite tip. The predicted tip undercoolings are, however, somewhat lower at intermediate growth rates. An improved calculation for the solute buildup at the dendrite tip due to curvature effects is also included.

Laxmanan, V.↗

NASA NTRS1994

Changes in intervertebral disc cross-sectional area with bed rest and space flight

STUDY DESIGN. We measured the cross-sectional area of the intervertebral discs of normal volunteers after an overnight rest; before, during, and after 5 or 17 weeks of bed rest; and before and after 8 days of weightlessness. OBJECTIVES. This study sought to determine the degree of expansion of the lumbar discs resulting from bed rest and space flight. SUMMARY OF BACKGROUND DATA. Weightlessness and bed rest, an analog for weightlessness, reduce the mechanical loading on the musculoskeletal system. When unloaded, intervertebral discs will expand, increasing the nutritional diffusion distance and altering the mechanical properties of the spine. METHODS. Magnetic resonance imaging was used to measure the cross-sectional area and transverse relaxation time (T2) of the intervertebral discs. RESULTS. Overnight or longer bed rest causes expansion of the disc area, which reaches an equilibrium value of about 22% (range 10-40%) above baseline within 4 days. Increases in disc area were associated with modest increases in disc T2. During bed rest, disc height increased approximately 1 mm, about one-half of previous estimates based on body height measurements. After 5 weeks of bed rest, disc area returned to baseline within a few days of ambulation, whereas after 17 weeks, disc area remained above baseline 6 weeks after reambulation. After 8 days of weightlessness, T2, disc area, and lumbar length were not significantly different from baseline values 24 hours after landing. CONCLUSIONS. Significant adaptive changes in the intervertebral discs can be expected during weightlessness. These changes, which are rapidly reversible after short-duration flights, may be an important factor during and after long-duration missions.

Non-NASA Center↗

DOE OSTI2016

On the averaging of cardiac diffusion tensor MRI data: the effect of distance function selection

Diffusion tensor magnetic resonance imaging (DT-MRI) allows a unique insight into the microstructure of highly-directional tissues. The selection of the most proper distance function for the space of diffusion tensors is crucial in enhancing the clinical application of this imaging modality. Both linear and nonlinear metrics have been proposed in the literature over the years. The debate on the most appropriate DT-MRI distance function is still ongoing. Here, in this paper, we presented a framework to compare the Euclidean, affine-invariant Riemannian and log-Euclidean metrics using actual high-resolution DT-MRI rat heart data. We employed temporal averaging at the diffusion tensor level of three consecutive and identically-acquired DT-MRI datasets from each of five rat hearts as a means to rectify the background noise-induced loss of myocyte directional regularity. This procedure is applied here for the first time in the context of tensor distance function selection. When compared with previous studies that used a different concrete application to juxtapose the various DT-MRI distance functions, this work is unique in that it combined the following: (i) metrics were judged by quantitative—rather than qualitative—criteria, (ii) the comparison tools were non-biased, (iii) a longitudinal comparison operation was used on a same-voxel basis. The statistical analyses of the comparison showed that the three DT-MRI distance functions tend to provide equivalent results. Hence, we came to the conclusion that the tensor manifold for cardiac DT-MRI studies is a curved space of almost zero curvature. The signal to noise ratio dependence of the operations was investigated through simulations. Finally, the 'swelling effect' occurrence following Euclidean averaging was found to be too unimportant to be worth consideration.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2014

Fluorescence-Correlation Spectroscopy Study of Molecular Transport within Reversed-Phase Chromatographic Particles Compared to Planar Model Surfaces

Reversed-phase liquid chromatography (RPLC) is a widely used technique for molecular separations. Stationary-phase materials for RPLC generally consist of porous silica-gel particles functionalized with n-alkane ligands. Understanding motions of molecules within the interior of these particles is important for developing efficient chromatographic materials and separations. To characterize these dynamics, time-resolved spectroscopic methods (photobleach recovery, fluorescence correlation, single-molecule imaging) have been adapted to measure molecular diffusion rates, typically at n-alkane-modified planar silica surfaces, which serve as models of chromatographic interfaces. A question arising from these studies is how dynamics of molecules on a planar surface relate to motions of molecules within the interior of a porous chromatographic particle. In this paper, imaging-fluorescence-correlation spectroscopy is used to measure diffusion rates of a fluorescent probe molecule 1,1'-dioctadecyl-3,3,3'3'-tetramethylindocarbocyanine perchlorate (DiI) within authentic RPLC porous silica particles and compared with its diffusion at a planar C18-modified surface. The results show that surface diffusion on the planar C18 substrate is much faster than the diffusion rate of the probe molecule through a chromatographic particle. Surface diffusion within porous particles, however, is governed by molecular trajectories along the tortuous contours of the interior surface of the particles. By accounting for the greater surface area that a molecule must explore to diffuse macroscopic distances through the particle, the molecular-scale diffusion rates on the two surfaces can be compared, and they are virtually identical. Furthermore, these results provide support for the relevance of surface-diffusion measurements made on planar model surfaces to the dynamic behavior of molecules on the internal surfaces of porous chromatographic particles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Release history and transport parameters of relativistic solar electrons inferred from near-the-sun in situ observations

We study four consecutive 300–800 keV electron events observed on 1980 May 28 by Helios-1, when the spacecraft was located at 0.31 au from the Sun. We use two different techniques to extract the release time history of electrons at the Sun: (1) a data-driven method based on the assumption that particles conserve their magnetic moment as they propagate between the Sun and the spacecraft and (2) an inversion method that utilizes particle transport simulation results. Both methods make use of the particle angular distributions measured relative to the local direction of the magnetic field. The general characteristics of the release time profiles obtained by these two techniques are similar, especially during their rising phases. We find indications that the strength of the interplanetary scattering varies with the size of the solar parent event, suggesting that scattering processes are not necessarily an inherent property of the medium but are related to the amount of released particles at the Sun. We use the inferred release profiles to compute the expected intensities at 1 au. In contrast to simultaneous near-Earth observations by the Interplanetary Monitoring Platform (IMP-8), our simulations predict the observation of four separate events at 1 au. Processes that could contribute to the observation of one single time-extended event at 1 au include (1) distinct magnetic connections of the spacecraft to the particle sources, (2) the spatio-temporal evolution of the particle sources, and (3) different particle transport conditions, including a variation of λ{sub r} with radial distance and/or heliolongitude, as well as the possibility that electrons reached IMP-8 by diffusion perpendicular to the interplanetary magnetic field.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS1992

Estimation of the viscosities of silicate liquids at high pressure from measurements of oxygen diffusivity

The dynamics and evolution of a magma ocean depend significantly on the structure and physical properties of silicate liquids at high pressure. Viscosity is particularly important because of its effect on the dynamics of convection and crystal setting. Traditionally, the viscosities of silicate liquids have been measured at high pressure by falling sphere viscometry but, due to some limitations of this technique, few measurements have been made at pressures exceeding 2.5 GPa. An alternative approach, which has previously been proven up to 2 GPa, is to use high pressure measurements of oxygen self-diffusivity (D) to estimate viscosity (eta) from the Eyring relationship eta = kT/D lambda (where k is the Boltzmann constant, T is absolute temperature, and lambda is the diffusive jump distance). We have performed preliminary experiments on Na2Si4O9 liquid in order to explore the feasibility of this method up to pressures in excess of 10 GPa. Diffusion couples were prepared from glass starting materials with one half of the sample enriched in O-18 and the other half containing the natural abundance (0.2 wt percent). Diffusion experiments were performed at 1600 to 1800 C at pressures in the range of 2.5 to 10 GPa for times up to 6 minutes using a 1200 ton multianvil apparatus. Oxygen diffusivities were derived from the resulting O-18 concentration profiles, which were analyzed using an ion microprobe. At 1800 C, oxygen diffusivities increase continuously from 1 x 10(exp -10) m(exp -2) s(exp -1) at 2.5 Gpa to 5 x 10(exp -10) m(exp -2) s(exp -1) at 10 GPa. From the Eyring relationship, the viscosity of Na2SiO9 liquid is predicted to decrease by approx. 0.7 log units over this pressure range at 1800 C. These trends, which can be related to changes in the structure of the liquid at high pressure, are in agreement with results of molecular dynamics calculations. These results suggest that it should be possible to estimate the viscosities of silicate liquids up to at least 15 GPa and 2200 C by this method.

Rubie, D. C.↗