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At least 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Thermodynamic and Kinetic Transitions of Liquids in Nanoconfinement

Core principles of chemistry are ubiquitously invoked to shed light on the nature of molecular level interactions in nanoconfined fluids, which play a pivotal role in a wide range of processes in geochemistry, biology, and engineering. A detailed understanding of the physicochemical processes involved in the flow, structural transitions, and freezing or melting behavior of fluids confined within nanometer-sized pores of solid materials is thus of enormous importance for both basic research and technological applications. This Account provides a perspective on new insights into the thermodynamic and kinetic transitions of nanoconfined fluids in their stable and metastable forms. After briefly introducing the unique properties of mesoporous silicas from the SBA, MCM, and FDU families that serve as the confinement matrices, combining highly ordered single and bimodal mesopore architectures with tunable pore sizes in the ~2-15 nm range and narrow size distributions, recent studies on melting/freezing behavior of water confined in these host matrices are reviewed. While differential scanning calorimetry (DSC) reveals a linear relationship between melting point depression and pore size (independent of the pore shape), as predicted by the Gibbs-Thomson relation, variable temperature 2 H wide-line nuclear magnetic resonance (NMR) spectroscopy studies confirm the core-shell model of water and give evidence for a layer-by-layer freezing mechanism, which gives rise to an apparent fragile-to-strong transition in the solidification dynamics. In contrast to the freezing/melting behavior of water, the effect of nanoconfinement on the glass transition of supercooled liquids is nonuniversal and the glass transition temperature T g can either increase or decrease with the dimensionality and extent of confinement. This nonuniversal behavior is exemplified by the two glass-forming molecular liquids, glycerol and ortho-terphenyl (OTP). While glycerol shows an increase in T g and a pronounced slowdown of the rotational dynamics of the constituent molecules due to a change in the molecular packing between the bulk and the confined liquid, OTP displays a linear and confining-media-dependent depression of T g with increased confinement that is strongly influenced by the pore-liquid interface characteristics. This Account concludes with a focus on recent experimental evidence of extreme spatial and dynamical heterogeneity in both freezing and glass transition processes. This discovery was enabled by the unique mesoporous structures of SBA-16 and FDU-5, possessing bimodal architectures with two interconnected pore types of different size and shape (spherical and cylindrical). For the very first time, two melting points for water and two glass transitions for supercooled OTP, corresponding to a specific pore type, were observed. Collectively, these observations strongly suggest a close mechanistic connection between the local fluctuations in the structure and dynamics of nanoconfined liquids. Finally, while the findings reviewed in this Account provide new insights into thermodynamic and kinetic transitions of fluids, there remain many unanswered questions regarding the effects of nanoconfinement on the fundamental properties of fluids, which offer exciting future opportunities in chemical research.

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

Photodissociation Dynamics of CH 2 OO on Multiple Potential Energy Surfaces: Experiment and Theory

UV excitation of the CH 2 OO Criegee intermediate across most of the broad span of the (B 1A') – (X 1A') spectrum results in prompt dissociation to two energetically accessible asymptotes: O ( 1 D) + H 2 CO (X 1 A 1 ) and O ( 3 P) + H 2 CO (a 3A"). Dissociation proceeds on multiple singlet potential energy surfaces that are coupled by two regions of conical intersection (CoIn). Velocity map imaging (VMI) studies reveal a bimodal total kinetic energy (TKER) distribution for the O ( 1 D) + H 2 CO (X 1 A 1 ) products with the major and minor components accounting for ca. 40% and ca. 20% on average of the available energy (E avl ), respectively. The unexpected low TKER component corresponds to highly internally excited H 2 CO (X 1 A 1 ) products accommodating ca. 80% of E avl . Full dimensional trajectory calculations suggest that the bimodal TKER distribution of the O ( 1 D) + H 2 CO (X 1 A 1 ) products originates from two different dynamical pathways: a primary pathway (69%) evolving through one CoIn region to products and a smaller component (20%) sampling both CoIn regions enroute to products. Those that access both CoIn regions likely give rise to the more highly internally excited H 2 CO (X 1 A 1 ) products. The remaining trajectories (11%) dissociate to O ( 3 P) + H 2 CO (a 3 A") products after traversing through both CoIn regions. Here, the complementary experimental and theoretical investigation provides insight on the photodissociation of CH 2 OO via multiple dissociation pathways through two regions of CoIn that control the branching and energy distributions of products.

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

The distribution of [α/Fe] in the Milky Way disc

ABSTRACT Using a sample of red giant stars from the Apache Point Observatory Galactic Evolution Experiment (APOGEE) Data Release 16, we infer the conditional distribution $p([\alpha /{\rm Fe}]\, |\, [{\rm Fe}/{\rm H}])$ in the Milky Way disk for the α-elements Mg, O, Si, S, and Ca. In each bin of [Fe/H] and Galactocentric radius R, we model p([α/Fe]) as a sum of two Gaussians, representing ‘low-α’ and ‘high-α’ populations with scale heights $z_1=0.45\, {\rm kpc}$ and $z_2=0.95\, {\rm kpc}$, respectively. By accounting for age-dependent and z-dependent selection effects in APOGEE, we infer the [α/Fe] distributions that would be found for a fair sample of long-lived stars covering all z. Near the Solar circle, this distribution is bimodal at sub-solar [Fe/H], with the low-α and high-α peaks clearly separated by a minimum at intermediate [α/Fe]. In agreement with previous results, we find that the high-α population is more prominent at smaller R, lower [Fe/H], and larger |z|, and that the sequence separation is smaller for Si and Ca than for Mg, O, and S. We find significant intrinsic scatter in [α/Fe] at fixed [Fe/H] for both the low-α and high-α populations, typically ∼0.04-dex. The means, dispersions, and relative amplitudes of this two-Gaussian description, and the dependence of these parameters on R, [Fe/H], and α-element, provide a quantitative target for chemical evolution models and a test for hydrodynamic simulations of disk galaxy formation. We argue that explaining the observed bimodality will probably require one or more sharp transitions in the disk’s gas accretion, star formation, or outflow history in addition to radial mixing of stellar populations.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Characterization of Radiation Induced Defects Across Scales

The Whole Powder Pattern Modelling (WPPM) approach of diffraction line profile analysis (LPA) was applied for the first time on PuO 2 in order to understand the evolution of the microstructural properties as a function of process conditions. Crystallite size distributions and defect concentrations were determined by WPPM on three different PuO 2 samples - including one with a bimodal distribution and compared to the result of more common LPA analyses used in PuO 2 literature studies (e.g. Scherrer equation, double Voigt method). The conclusion was that a lognormal distribution of spherical crystallites with dislocations most closely represent the microstructure of PuO 2 produced by heating Pu 2 (C 2 O 4 ) 3 (H 2 O) 6 •3H 2 O between 650°C and 850°C. The volume-weighted mean column length (Lvol) parameter obtained from the double Voigt method for the monomodal samples were the same as the Lvol obtained from the WPPM within uncertainty. The two LPA methods did not agree on the Lvol parameters of the bimodal distribution sample with only the WPPM getting values that were consistent with the individual components. The WPPM can potentially provide more insight into future studies of the influences on the microstructure properties of PuO 2 .

36 MATERIALS SCIENCE↗
DOE OSTI2023

Development of Binder Jet Compatible Silicon Carbide Mixtures for Increased Sintered Density

Binder jet additive manufacturing can process a variety of ceramic powder feedstocks to manufacture near net shape green parts that are subsequently sintered to achieve densification. In particular, silicon carbide (SiC) is a promising ceramic material for heat exchangers in energy storage applications and binder jet is a well-suited process for manufacturing these heat exchangers due to the often geometrically complex designs. However, the need for good powder flowability in binder jet printing often limits the feedstock powder to be larger particles rather than that of ultra fine submicron powders used in conventional ceramic processing, which are more readily densified during sintering. The present work explores the use of various powder mixtures and sintering settings to identify strategies for achieving high density sintered parts in binder jet compatible systems without the use of infiltration. Liquid-phase sintering additives and bimodal powder mixtures are explored alongside different sintering temperatures, rates, atmospheres, and hold times. Two mixtures were found to be good candidates for further exploration: 1) 90 wt% 0.6 µm SiC + 6.25 wt% Al 2 O 3 + 3.75 wt% Y 2 O 3 mixture achieved the highest sintered relative density of 91.2%; and 2) a bimodal mixture comprised of 45 wt% 10 µm SiC + 45 wt% 0.6 µm SiC + 6.25 wt% Al 2 O 3 + 3.75 wt% Y 2 O 3 had the best powder flowability of the powders measured and a 75.1% sintered relative density.

25 ENERGY STORAGE↗
DOE OSTI2021

Wide Dust Gaps in Protoplanetary Disks Induced by Eccentric Planets: A Mass-eccentricity Degeneracy

The tidal perturbation of embedded protoplanets on their natal disks has been widely attributed to be the cause of gap-ring structures in submillimeter images of protoplanetary disks around T Tauri stars. Numerical simulations of this process have been used to propose scaling of characteristic dust-gap width/gap-ring distance with respect to planet mass. Applying such scaling to analyze observed gap samples yields a continuous mass distribution for a rich population of hypothetical planets in the range of several Earth to Jupiter masses. In contrast, the conventional core-accretion scenario of planet formation predicts a bimodal mass function due to (1) the onset of runaway gas accretion above ~20 Earth masses and (2) suppression of accretion induced by gap opening. Here, we examine the dust disk response to the tidal perturbation of eccentric planets as a possible resolution of this paradox. Based on simulated gas and dust distributions, we show the gap-ring separation of Neptune-mass planets with small eccentricities might become comparable to that induced by Saturn-mass planets on circular orbits. Furthermore, this degeneracy may obliterate the discrepancy between the theoretical bimodal mass distribution and the observed continuous gap width distribution. Despite damping due to planet–disk interaction, modest eccentricity may be sustained either in the outer regions of relatively thick disks or through resonant excitation among multiple super Earths. Moreover, the ring-like dust distribution induced by planets with small eccentricities is axisymmetric even in low viscosity environments, consistent with the paucity of vortices in Atacama Large Millimeter/submillimeter Array images.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2023

A Tale of Two Disks: Mapping the Milky Way with the Final Data Release of APOGEE

We present new maps of the Milky Way disk showing the distribution of metallicity ([Fe/H]), α-element abundances ([Mg/Fe]), and stellar age, using a sample of 66,496 red giant stars from the final data release (DR17) of the Apache Point Observatory Galactic Evolution Experiment survey. We measure radial and vertical gradients, quantify the distribution functions for age and metallicity, and explore chemical clock relations across the Milky Way for the low-α disk, high-α disk, and total population independently. The low-α disk exhibits a negative radial metallicity gradient of -0.06 ± 0.001 dex kpc -1 , which flattens with distance from the midplane. The high-α disk shows a flat radial gradient in metallicity and age across nearly all locations of the disk. The age and metallicity distribution functions shift from negatively skewed in the inner Galaxy to positively skewed at large radius. Significant bimodality in the [Mg/Fe]–[Fe/H] plane and in the [Mg/Fe]–age relation persist across the entire disk. The age estimates have typical uncertainties of ~0.15 in log(age) and may be subject to additional systematic errors, which impose limitations on conclusions drawn from this sample. Nevertheless, these results act as critical constraints on galactic evolution models, constraining which physical processes played a dominant role in the formation of the Milky Way disk. We discuss how radial migration predicts many of the observed trends near the solar neighborhood and in the outer disk, but an additional more dramatic evolution history, such as the multi-infall model or a merger event, is needed to explain the chemical and age bimodality elsewhere in the Galaxy.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS1972

Oil-film-parameter investigation

A counter rotating fixture was designed and built to measure starved EHD film thicknesses. Some good geometry glass races were obtained. A theoretical analysis of starvation was made. Measurements of retainer stability during bimode torque disturbances were made. The most common form of bimode was related to stability of retainer cock.

Kingsbury, E. P.↗
NASA NTRS1973

Tensile properties to 650 C and deformation structures in a precipitation strengthened titanium-aluminum alloy

Appreciable strength levels were retained to 650 C in a Ti-10Al-1Si alloy aged in the (alpha + alpha sub 2) phase field to yield optimum room temperature strength and ductility. The aging treatment precipitated a uniform distribution of alpha sub 2-particles such that, at room temperature, dislocations bypassed instead of shearing the particles at low strains. Specimens fractured at room temperature exhibited fine uniform dimples even for those aging conditions that imparted no macroscopic ductility. The main crack appeared to propagate through the planar slip bands that had cut through the alpha sub 2-particles. A two-step aging process produced a higher volume fraction of bimodally distributed alpha sub 2-particles that led to higher strength levels at elevated temperatures. Both for the single size and the bimodal alpha sub 2-particle distributions, elevated-temperature deformation structures consisted mainly of planar slip bands that sheared through the alpha sub 2-particles.

Mendiratta, M. G.↗
NASA NTRS1976

Response of deep and shallow tropical maritime cumuli to large-scale processes

The bulk diagnostic method of Yanai et al. (1973) and a simplified version of the spectral diagnostic method of Nitta (1975) are used for a more quantitative evaluation of the response of various types of cumuliform clouds to large-scale processes, using the same data set in the Marshall Islands area for a 100-day period in 1956. The dependence of the cloud mass flux distribution on radiative cooling, large-scale vertical motion, and evaporation from the sea is examined. It is shown that typical radiative cooling rates in the tropics tend to produce a bimodal distribution of mass spectrum exhibiting deep and shallow clouds. The bimodal distribution is further enhanced when the large-scale vertical motion is upward, and a nearly unimodal distribution of shallow clouds prevails when the relative cooling is compensated by the heating due to the large-scale subsidence. Both deep and shallow clouds are modulated by large-scale disturbances. The primary role of surface evaporation is to maintain the moisture flux at the cloud base.

Yanai, M.↗
NASA NTRS1978

CTS-type variable conductance heat pipes for SEP FM/PPU

The development effort for, and the fabrication and testing of, six CTS-type variable conductance heat pipes is described. The heat pipes are constructed of stainless steel, use methanol as a working fluid, and a nitrogen/helium mixture as the control gas. The wicking structure consists of interior wall grooves, a metal-felt diametral slab wick, and two wire-mesh arteries. The heat pipes are used to cool two Functional Model/Power Processing Units in a Solar Electric Propulsion prototype BIMOD thruster subsystem assembly. The Power Processing Units convert the electric power from a spacecraft solar array system to the voltages required to operate the electric thrusters which are part of the BIMOD assembly.

Antoniuk, D.↗
NASA NTRS1981

The electric rail gun for space propulsion

An analytic feasibility investigation of an electric propulsion concept for space application is described. In this concept, quasistatic thrust due to inertial reaction to repetitively accelerated pellets by an electric rail gun is used to propel a spacecraft. The study encompasses the major subsystems required in an electric rail gun propulsion system. The mass, performance, and configuration of each subsystem are described. Based on an analytic model of the system mass and performance, the electric rail gun mission performance as a reusable orbital transfer vehicle (OTV) is analyzed and compared to a 30 cm ion thruster system (BIMOD) and a chemical propulsion system (IUS) for payloads with masses of 1150 kg and 2300 kg. For system power levels in the range from 25 kW(e) to 100 kW(e) an electric rail gun OTV is more attractive than a BIMOD system for low Earth orbit to geosynchronous orbit transfer durations in the range from 20 to 120 days.

Bauer, D. P.↗
NASA NTRS1985

The Geology of Mt. Hope, a Silicic Volcanic Center in West Central Arizona

The purpose was to establish a detailed history of the sequence of geologic events which occurred at Mt. Hope and an area 6.8 miles in diameter surrounding it. The final result will be comprised of information collected during field mapping, with data from petrographic studies and wet chemical analyses. From this it should be possible to suggest relationships to other volcanic regions, particularly bimodal suites in the transition zone, and gain a clearer picture of the petrologic nature of this area. Field work conducted this past summer confirmed the bimodal nature of volcanism at Mt. Hope. The symmetrical, radial cone is comprised of several rhyolites with numerous intrusions of intermediate-composition dikes and two breccia pipes near the summit.

Simmons, A. M.↗
NASA NTRS1985

Radio phase characteristics of terrain from multipolarized synthetic aperture radar data

Recent advances in digital data acquisition and signal processing technology permit simultaneous measurement of the complex (amplitude and phase) radar backscatter from several polarization-diverse antennas. While absolute phase mesurements remain to be analyzed in detail. The differential phase of signals polarized parallel and perpendicular to the plane of incidence provide information on the scattering mechanisms that dominate the interaction of the radio waves with the terrain. Analysis of phase backscatter maps from a typical urban area yields a bimodal distribution with the two peaks separated by approximately 180 degrees, highly indicative of a dominant simple geometric one bounce-two bounce mechanism. Some maps of agricultural areas exhibit a similar distribution, however, other agricultural areas yield a distribution that, while still bimodal, consists of two peaks separated by about 110 deg. Still other agricultural areas exhibit a more complex distribution. All of the observed phase shifts appear to be independent of incidence angle from at least 20 deg to 55 deg, therefore the 110 degree shifts are inconsistent with both the geometric model used for the urban area and with common dielectric slab models.

Zebker, H. A.↗
NASA NTRS1987

Correlation between spectral state and quasi-periodic oscillation parameters in GX 5-1

In a series of seven Exosat observations, the bimodal spectral behavior and the quasi-periodic oscillation (QPO)/red noise properties of GX 5-1 show a strict correlation. In one of the two spectral states (characterized by a 'horizontal branch' in the hardness-intensity diagram), strong 20-40 Hz QPO and red noise below about 60 Hz were always present. In the other ('normal branch'), no QPO between 6 and 60 Hz or red noise above 1 Hz were detected, but there was an indication for weak QPO near 5 Hz. In both states 'very low frequency noise' (VLFN) is detected below 0.1 Hz which has a power-law shape and and which extends down to the lowest observed frequencies (0.0001 Hz). The VLFN is probably not directly related to the QPO. The results are compared to those on Sco X-1 and Cyg X-2 and it is concluded that, although all three sources show bimodal spectral and QPO/red noise behavior, there is a qualitative difference between GX 5-1 and Cyg X-2 on one hand and Sco X-1 on the other.

Van Der Klis, M.↗
NASA NTRS1986

The over-the-limb hard X-ray events

Over-the-limb hard X-ray events offer a uniquely direct view of the hard X-ray emission from the solar corona during a major flare. Limb occultation at angles greater than about 10 deg (an arbitrary definition of this class of events) excludes any confusion with brighter chromospheric sources. Published observations of seven over-the-limb events, beginning with the prototype flare of March 30, 1969, are reviewed. The hard X-ray spectra appear to fall into two classes: hard events, with power-law index of about 2.0; and soft events, with power-law index about 5.4. This tendency towards bimodality is only significant at the 90-percent confidence level due to the smallness of the number of events observed to date. If borne out by future data, the bimodality would suggest the existence of two different acceleration mechanisms.

Hudson, H. S.↗
NASA NTRS1988

Random Process Simulation for stochastic fatigue analysis

A simulation technique is described which directly synthesizes the extrema of a random process and is more efficient than the Gaussian simulation method. Such a technique is particularly useful in stochastic fatigue analysis because the required stress range moment E(R sup m), is a function only of the extrema of the random stress process. The family of autoregressive moving average (ARMA) models is reviewed and an autoregressive model is presented for modeling the extrema of any random process which has a unimodal power spectral density (psd). The proposed autoregressive technique is found to produce rainflow stress range moments which compare favorably with those computed by the Gaussian technique and to average 11.7 times faster than the Gaussian technique. The autoregressive technique is also adapted for processes having bimodal psd's. The adaptation involves using two autoregressive processes to simulate the extrema due to each mode and the superposition of these two extrema sequences. The proposed autoregressive superposition technique is 9 to 13 times faster than the Gaussian technique and produces comparable values for E(R sup m) for bimodal psd's having the frequency of one mode at least 2.5 times that of the other mode.

Larsen, Curtis E.↗
NASA NTRS1989

Denitrification in the Antarctic stratosphere

Rapid loss of ozone over Antarctica in spring requires that the abundance of gaseous nitric acid be very low. Precipitation of particulate nitric acid has been assumed to occur in association with large ice crystals, requiring significant removal of H2O and temperatures well below the frost point. However, stratospheric clouds exhibit a bimodal size distribution in the Antarctic atmosphere, with most of the nitrate concentrated in particles with radii of 1 micron or greater. It is argued here that the bimodal size distribution sets the stage for efficient denitrification, with nitrate particles either falling on their own or serving as nuclei for the condensation of ice. Denitrification can therefore occur without significant dehydration, and it is unnecessary for temperatures to drop significantly below the frost point.

Salawitch, R. J.↗