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At least 1,135 records · Page 63
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

The grain-size effect on thermal conductivity of uranium dioxide

We have investigated the grain-boundary scattering effect on the thermal transport behavior of uranium dioxide (UO 2 ). The polycrystalline samples having different grain-sizes (0.125, 1.8, and 7:2 µm) have been prepared by a spark plasma sintering technique and characterized by x-ray powder diffraction, scanning electron microscope, and Raman spectroscopy. The thermal transport properties (the thermal conductivity and thermoelectric power) have been measured in the temperature range of 2–300 K, and the results were analyzed in terms of various physical parameters contributing to thermal conductivity in these materials in relation to grain-size. We show that thermal conductivity decreases systematically with lowering grain-size in the temperatures below 30 K, where the boundary scattering dominates the thermal transport. At higher temperatures, more scattering processes are involved in the heat transport in these materials, making the analysis difficult. We determined the grain-boundary Kapitza resistance that would result in the observed increase in thermal conductivity with grain-size and compared the value with Kapitza resistances calculated for UO 2 using molecular dynamics from the literature.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Palladium oxidation leads to methane combustion activity: Effects of particle size and alloying with platinum

Pd- and Pt-based catalysts are highly studied materials due to their widespread use in emissions control catalysis. However, claims continue to vary regarding the active phase and oxidation state of the metals. Different conclusions have likely been reached due to the heterogeneous nature of such materials containing various metal nanoparticle sizes and compositions, which may each possess unique redox features. In this work, using uniform nanocrystal catalysts, we study the effect of particle size and alloying on redox properties of Pd-based catalysts and show their contribution to methane combustion activity using operando quick extended x-ray absorption fine structure measurements. Results demonstrate that for all studied Pd sizes (3 nm–16 nm), Pd oxidation directly precedes CH 4 combustion to CO 2 , suggesting Pd oxidation as a prerequisite step to methane combustion, and an oxidation pretreatment shows equal or better catalysis than a reduction pretreatment. Results are then extended herein to uniform alloyed Pt x Pd 1–x nanoparticles, where oxidative pretreatments are shown to enhance low-temperature combustion. In these uniform alloys, we observe a composition-dependent effect with Pt-rich alloys showing the maximum difference between oxidative and reductive pretreatments. In Pt-rich alloys, we initially observe that the presence of Pt maintains Pd in a lower-activity reduced state. However, with time on stream, PdO eventually segregates under oxidizing combustion conditions, leading to a slowly increasing activity. Overall, across particle sizes and alloy compositions, we relate increased catalytic activity to Pd oxidation, thus shedding light on previous contrasting results related to the methane combustion activity of these catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

The influence of particle size on the fluid dynamics of a laser-induced plasma

The interaction of a laser-induced shock wave with nanoparticles and microparticles of aluminum oxide is investigated through experiments and modeling. The chemistry and physics of the interaction between the particles and plasma generated from laser ablation shows similarities and discrete differences for the two particle sizes. For both particle sizes, early stage (< 10 μs) ionization was dominant and evidenced by higher concentrations of Al II. While both sizes exhibit ionization over the same duration, the intensity of emission was greater for nanoparticles indicating greater concentrations of ionized species. Moreover, the dispersion of species was notably more elongated for microparticles while radial dispersion was more pronounced for nanoparticles with elevated drag forces. At later stages (i.e., > 10 μs), oxidation reactions were dominant for both particle sizes, but the same distinctions in flow field were observed and attributed to particle drag. In all stages of interaction, microparticles expand axially with less drag that suppresses their radial expansion. As a result, the dispersion of reactive species was mapped over an up to 80% larger area for nanoparticles relative to microparticles. Results shown here can be applied toward advancing experimental diagnostics and particle-shock wave modeling and simulation efforts for energetic materials.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Repartitioned Brillouin-Wigner perturbation theory with a size-consistent second-order correlation energy

Second-order Møller-Plesset perturbation theory (MP2) often breaks down catastrophically in small-gap systems, leaving much to be desired in its performance for myriad chemical applications such as noncovalent interactions, thermochemistry, and dative bonding in transition metal complexes. This divergence problem has reignited interest in Brillouin-Wigner perturbation theory (BWPT), which is regular at all orders but lacks size consistency and extensivity, severely limiting its application to chemistry. In this work, we propose an alternative partitioning of the Hamiltonian that leads to a regular BWPT perturbation series that, through the second order, is size-extensive, size-consistent (provided its Hartree–Fock reference is also), and orbital invariant. Here, our second-order size-consistent Brillouin-Wigner (BW-s2) approach can describe the exact dissociation limit of H 2 in a minimal basis set, regardless of the spin polarization of the reference orbitals. More broadly, we find that BW-s2 offers improvements relative to MP2 for covalent bond breaking, noncovalent interaction energies, and metal/organic reaction energies, although rivaling coupled-cluster with single and double substitutions for thermochemical properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Size-dependent second-order-like phase transitions in Fe nanocluster melting from low-temperature structural isomerization

Here, in this work, the melting phase transitions of Fe n nanoclusters with 10 ≤ n ≤ 100 atoms are investigated using classical many-body molecular dynamics simulations. For many cluster sizes, surface melting occurs at much lower temperatures than core melting. Surface and core melting points and energetic melting points (temperatures of maximum heat capacity, C v ) are calculated for all cluster sizes. Melting properties are found to be strong functions of cluster structure. Cluster sizes with closed-shell structures always have first-order-like phase transitions. Almost one-third of cluster sizes in the analyzed range exhibit second-order-like phase transitions due to the presence of multiple structural configurations close in energy. 1-shell clusters with one to a few more atoms than a neighboring closed-shell structure have very low surface melting points and very high energetic melting points compared to their closed-shell counterparts. In clusters above 50 atoms with certain core structures, melting of the surface before the core was observed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Size-dependent dynamic structures of supported gold nanoparticles in CO oxidation reaction condition

Significance Gold is the noblest metal. However, when the size decreases to nanoscale and is supported on reducible oxides, the gold nanoparticle shows exceptionally high catalytic performance even at low temperatures. Here, through state-of-the-art in situ aberration-corrected environmental transmission electron microscopy and ab initio molecular-dynamic simulations, we discovered that, upon exposing to reactant gas (carbon monoxide and oxygen), ultrasmall gold clusters on ceria show a size-dependent order-to-disorder transformation with generation of dynamic low-coordinated atoms, which presumably can effectively boost the oxidation reaction of carbon monoxide. The findings provide much-needed insights on the origin of size-dependent catalytic properties of supported gold and demonstrate a size effect in absorbent–particle interactions that may widely exist and play an essential role in heterogeneous catalysts.

He, Yang↗
DOE OSTI2025

Multiphasic size-dependent growth dynamics of nanoparticle ensembles

Colloidal nanoparticles are of great interest in modern science and industry. However, the thermodynamic mechanism and dynamics of nanoparticle growth have yet to be understood. Addressing these issues, we tracked hundreds of in-situ growth trajectories of a nanoparticle ensemble using liquid-phase TEM and found that the nanoparticle growth, including coalescence, exhibits nanoparticle size-dependent multiphasic dynamics, unexplainable by current theories. Motivated by this finding, we developed a model and theory for an ensemble of growing nanoparticles, providing a unified, quantitative understanding of the time-dependent mean and fluctuation of nanoparticle size and size-dependent growth rate profiles across various nanoparticle systems and experimental conditions. Our work reveals that the chemical potential in a small nanoparticle strongly deviates from the Gibbs-Thomson equation, shedding light on how it governs the size-dependent growth dynamics of nanoparticles.

Kim, Ji-Hyun↗
DOE OSTI2014

On the validity of the Poisson assumption in sampling nanometer-sized aerosols

A Poisson process is traditionally believed to apply to the sampling of aerosols. For a constant aerosol concentration, it is assumed that a Poisson process describes the fluctuation in the measured concentration because aerosols are stochastically distributed in space. Recent studies, however, have shown that sampling of micrometer-sized aerosols has non-Poissonian behavior with positive correlations. The validity of the Poisson assumption for nanometer-sized aerosols has not been examined and thus was tested in this study. Its validity was tested for four particle sizes - 10 nm, 25 nm, 50 nm and 100 nm - by sampling from indoor air with a DMA- CPC setup to obtain a time series of particle counts. Five metrics were calculated from the data: pair-correlation function (PCF), time-averaged PCF, coefficient of variation, probability of measuring a concentration at least 25% greater than average, and posterior distributions from Bayesian inference. To identify departures from Poissonian behavior, these metrics were also calculated for 1,000 computer-generated Poisson time series with the same mean as the experimental data. For nearly all comparisons, the experimental data fell within the range of 80% of the Poisson-simulation values. Essentially, the metrics for the experimental data were indistinguishable from a simulated Poisson process. The greater influence of Brownian motion for nanometer-sized aerosols may explain the Poissonian behavior observed for smaller aerosols. Although the Poisson assumption was found to be valid in this study, it must be carefully applied as the results here do not definitively prove applicability in all sampling situations.

concentration measurement↗
DOE OSTI2013

Suppression of Cannibalism during Larviculture of Burbot through Size Grading

Abstract The survival and percentage of North American Burbot Lota lota maculosa larvae and metamorphosing larvae presumed to have been cannibalized during a 15-d period immediately following a size-grading event were compared with those of fish in nongraded control groups. In larvae (mean TL, 11.8 mm), grading immediately produced a size distinction, as the group that passed the grader was significantly narrower and shorter than the group retained by the grader. The mean coefficient of variation of the length of larvae in the retained group was significantly lower than that of the control group, indicating that grading reduced size heterogeneity. Grading significantly increased larval survival, which averaged 74.3% and 93.3% for the passed and retained fish, respectively, compared with 59.3% in the control. Increased survival was linked to a reduction in the percentage of larvae presumed cannibalized in the graded groups. In metamorphosing larvae (mean TL, 21.0 mm), grading did not significantly change TL, width, or the coefficient of variation of length, nor did it improve survival or reduce presumed cannibalism. This study provides initial empirical evidence that size grading can be an effective way to significantly reduce cannibalism when done at the onset of cannibalism in larval-stage Burbot.

Barron, James M.↗
DOE OSTI2012

THE SIZE SCALE OF STAR CLUSTERS

Direct N-body simulations of star clusters in a realistic Milky-Way-like potential are carried out using the code NBODY6. Based on these simulations, a new relationship between scale size and galactocentric distance is derived: the scale size of star clusters is proportional to the hyperbolic tangent of the galactocentric distance. The half-mass radius of star clusters increases systematically with galactocentric distance but levels off when star clusters orbit the galaxy beyond {approx}40 kpc. These simulations show that the half-mass radius of individual star clusters varies significantly as they evolve over a Hubble time, more so for clusters with shorter relaxation times, and remains constant through several relaxation times only in certain situations when expansion driven by the internal dynamics of the star cluster and the influence of the host galaxy tidal field balance each other. Indeed, the radius of a star cluster evolving within the inner 20 kpc of a realistic galactic gravitational potential is severely truncated by tidal interactions and does not remain constant over a Hubble time. Furthermore, the half-mass radius of star clusters measured with present-day observations bears no memory of the original cluster size. Stellar evolution and tidal stripping are the two competing physical mechanisms that determine the present-day size of globular clusters. These simulations also show that extended star clusters can form at large galactocentric distances while remaining fully bound to the host galaxy. There is thus no need to invoke accretion from an external galaxy to explain the presence of extended clusters at large galactocentric distances in a Milky-Way-type galaxy.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2013

INITIAL SIZE DISTRIBUTION OF THE GALACTIC GLOBULAR CLUSTER SYSTEM

Despite the importance of their size evolution in understanding the dynamical evolution of globular clusters (GCs) of the Milky Way, studies that focus specifically on this issue are rare. Based on the advanced, realistic Fokker-Planck (FP) approach, we theoretically predict the initial size distribution (SD) of the Galactic GCs along with their initial mass function and radial distribution. Over one thousand FP calculations in a wide parameter space have pinpointed the best-fit initial conditions for the SD, mass function, and radial distribution. Our best-fit model shows that the initial SD of the Galactic GCs is of larger dispersion than today's SD, and that the typical projected half-light radius of the initial GCs is {approx}4.6 pc, which is 1.8 times larger than that of the present-day GCs ({approx}2.5 pc). Their large size signifies greater susceptibility to the Galactic tides: the total mass of destroyed GCs reaches 3-5 Multiplication-Sign 10{sup 8} M {sub Sun }, several times larger than previous estimates. Our result challenges a recent view that the Milky Way GCs were born compact on the sub-pc scale, and rather implies that (1) the initial GCs were generally larger than the typical size of the present-day GCs, (2) the initially large GCs mostly shrank and/or disrupted as a result of the galactic tides, and (3) the initially small GCs expanded by two-body relaxation, and later shrank by the galactic tides.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2013

A PLATEAU IN THE PLANET POPULATION BELOW TWICE THE SIZE OF EARTH

We carry out an independent search of Kepler photometry for small transiting planets with sizes 0.5-8.0 times that of Earth and orbital periods between 5 and 50 days, with the goal of measuring the fraction of stars harboring such planets. We use a new transit search algorithm, TERRA, optimized to detect small planets around photometrically quiet stars. We restrict our stellar sample to include the 12,000 stars having the lowest photometric noise in the Kepler survey, thereby maximizing the detectability of Earth-size planets. We report 129 planet candidates having radii less than 6 R{sub E} found in three years of Kepler photometry (quarters 1-12). Forty-seven of these candidates are not in Batalha et al., which only analyzed photometry from quarters 1-6. We gather Keck HIRES spectra for the majority of these targets leading to precise stellar radii and hence precise planet radii. We make a detailed measurement of the completeness of our planet search. We inject synthetic dimmings from mock transiting planets into the actual Kepler photometry. We then analyze that injected photometry with our TERRA pipeline to assess our detection completeness for planets of different sizes and orbital periods. We compute the occurrence of planets as a function of planet radius and period, correcting for the detection completeness as well as the geometric probability of transit, R{sub *}/a. The resulting distribution of planet sizes exhibits a power law rise in occurrence from 5.7 R{sub E} down to 2 R{sub E} , as found in Howard et al. That rise clearly ends at 2 R{sub E} . The occurrence of planets is consistent with constant from 2 R{sub E} toward 1 R{sub E} . This unexpected plateau in planet occurrence at 2 R{sub E} suggests distinct planet formation processes for planets above and below 2 R{sub E} . We find that 15.1{sup +1.8}{sub -2.7}% of solar type stars-roughly one in six-has a 1-2 R{sub E} planet with P = 5-50 days.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2013

EVOLUTION OF THE SIZES OF GALAXIES OVER 7 < z < 12 REVEALED BY THE 2012 HUBBLE ULTRA DEEP FIELD CAMPAIGN

We analyze the redshift- and luminosity-dependent sizes of dropout galaxy candidates in the redshift range z ∼ 7-12 using deep images from the 2012 Hubble Ultra Deep Field (UDF12) campaign, which offers two advantages over that used in earlier work. First, we utilize the increased signal-to-noise ratio offered by the UDF12 imaging to provide improved measurements for known galaxies at z ≅ 6.5-8 in the HUDF. Second, because the UDF12 data have allowed the construction of the first robust galaxy sample in the HUDF at z > 8, we have been able to extend the measurement of average galaxy size out to higher redshifts. Restricting our measurements to sources detected at >15σ, we confirm earlier indications that the average half-light radii of z ∼ 7-12 galaxies are extremely small, 0.3-0.4 kpc, comparable to the sizes of giant molecular associations in local star-forming galaxies. We also confirm that there is a clear trend of decreasing half-light radius with increasing redshift, and provide the first evidence that this trend continues beyond z ≅ 8. Modeling the evolution of the average half-light radius as a power law, ∝(1 + z) {sup s}, we obtain a best-fit index of s=-1.30{sup +0.12}{sub -0.14} over z ∼ 4-12. A clear size-luminosity relation is evident in our dropout samples. This relation can be interpreted in terms of a constant surface density of star formation over a range in luminosity of 0.05-1.0 L{sub z=3}. The average star formation surface density in dropout galaxies is 2-3 orders of magnitude lower than that found in extreme starburst galaxies, but is comparable to that seen today in the centers of normal disk galaxies.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2013

A bayesian approach to estimate the size and structure of the broad-line region in active galactic nuclei using reverberation mapping data

This is the first paper in a series devoted to the systematic study of the size and structure of the broad-line region (BLR) in active galactic nuclei (AGNs) using reverberation mapping (RM) data. We employ a recently developed Bayesian approach that statistically describes the variability as a damped random walk process and delineates the BLR structure using a flexible disk geometry that can account for a variety of shapes, including disks, rings, shells, and spheres. We allow for the possibility that the line emission may respond non-linearly to the continuum, and we detrend the light curves when there is clear evidence for secular variation. We use a Markov Chain Monte Carlo implementation based on Bayesian statistics to recover the parameters and uncertainties for the BLR model. The corresponding transfer function is obtained self-consistently. We tentatively constrain the virial factor used to estimate black hole masses; more accurate determinations will have to await velocity-resolved RM data. Application of our method to RM data with Hβ monitoring for about 40 objects shows that the assumed BLR geometry can reproduce quite well the observed emission-line fluxes from the continuum light curves. We find that the Hβ BLR sizes obtained from our method are on average ∼20% larger than those derived from the traditional cross-correlation method. Nevertheless, we still find a tight BLR size-luminosity relation with a slope of α = 0.55 ± 0.03 and an intrinsic scatter of ∼0.18 dex. In particular, we demonstrate that our approach yields appropriate BLR sizes for some objects (such as Mrk 142 and PG 2130+099) where traditional methods previously encountered difficulties.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2014

Size distribution of possible dust carriers for the extended red emission

Power-law size distributions expected to be applicable to possible carriers of extended red emission (ERE) have been examined using Monte Carlo (MC) simulations. Si nanoparticles and some polycyclic aromatic hydrocarbon complexes such as oligoacene and oligorylenes with energy gaps close to 2 eV have been considered. In the simplest case of unit quantum efficiency, the MC-generated size distributions are used to obtain photoluminescence (PL) spectra that are then corrected for dust extinction and reddening effects for comparison with observed ERE spectra. It is shown that a power-law size distribution with a decay exponent of α = 7/2, which closely agrees with starlight extinction data, fails to produce an ERE-like spectrum. However, size distributions with decay exponents of α = 19/12 and 3/2 are found to lead to acceptable spectra. Results indicate that energetic photon-induced breakup and competing aggregation effects dominate collisional effects in producing the observed steady-state mass distribution. It is shown that the peak wavelength of emission critically depends on the band gap, rather than cluster mass, which for oligoacenes and oligorylenes is widely different. The peak wavelength is also shown to be insensitive to dust attenuation.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

EVIDENCE FOR (AND AGAINST) PROGENITOR BIAS IN THE SIZE GROWTH OF COMPACT RED GALAXIES

Most massive, passive galaxies are compact at high redshifts, but similarly compact massive galaxies are rare in the local universe. The most common interpretation of this phenomenon is that massive galaxies have grown in size by a factor of about five since redshift z = 2. An alternative explanation is that recently quenched massive galaxies are larger (a {sup p}rogenitor bias{sup )}. In this paper, we explore the importance of progenitor bias by looking for systematic differences in the stellar populations of compact early-type galaxies in the DEEP2 survey as a function of size. Our analysis is based on applying the statistical technique of bootstrap resampling to constrain differences in the median ages of our samples and to begin to characterize the distribution of stellar populations in our co-added spectra. The light-weighted ages of compact early-type galaxies at redshifts 0.5 < z < 1.4 are compared to those of a control sample of larger galaxies at similar redshifts. We find that massive compact early-type galaxies selected on the basis of red color and high bulge-to-total ratio are younger than similarly selected larger galaxies, suggesting that size growth in these objects is not driven mainly by progenitor bias, and that individual galaxies grow as their stellar populations age. However, compact early-type galaxies selected on the basis of image smoothness and high bulge-to-total ratio are older than a control sample of larger galaxies. Progenitor bias will play a significant role in defining the apparent size changes of early-type galaxies if they are selected on the basis of the smoothness of their light distributions.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

THE STICKINESS OF MICROMETER-SIZED WATER-ICE PARTICLES

Water ice is one of the most abundant materials in dense molecular clouds and in the outer reaches of protoplanetary disks. In contrast to other materials (e.g., silicates), water ice is assumed to be stickier due to its higher specific surface energy, leading to faster or more efficient growth in mutual collisions. However, experiments investigating the stickiness of water ice have been scarce, particularly in the astrophysically relevant micrometer-sized region and at low temperatures. In this work, we present an experimental setup to grow aggregates composed of μm-sized water-ice particles, which we used to measure the sticking and erosion thresholds of the ice particles at different temperatures between 114 K and 260 K. We show with our experiments that for low temperatures (below ∼210 K), μm-sized water-ice particles stick below a threshold velocity of 9.6 m s{sup –1}, which is approximately 10 times higher than the sticking threshold of μm-sized silica particles. Furthermore, erosion of the grown ice aggregates is observed for velocities above 15.3 m s{sup –1}. A comparison of the experimentally derived sticking threshold with model predictions is performed to determine important material properties of water ice, i.e., the specific surface energy and the viscous relaxation time. Our experimental results indicate that the presence of water ice in the outer reaches of protoplanetary disks can enhance the growth of planetesimals by direct sticking of particles.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

AN ANCIENT EXTRASOLAR SYSTEM WITH FIVE SUB-EARTH-SIZE PLANETS

The chemical composition of stars hosting small exoplanets (with radii less than four Earth radii) appears to be more diverse than that of gas-giant hosts, which tend to be metal-rich. This implies that small, including Earth-size, planets may have readily formed at earlier epochs in the universe's history when metals were more scarce. We report Kepler spacecraft observations of Kepler-444, a metal-poor Sun-like star from the old population of the Galactic thick disk and the host to a compact system of five transiting planets with sizes between those of Mercury and Venus. We validate this system as a true five-planet system orbiting the target star and provide a detailed characterization of its planetary and orbital parameters based on an analysis of the transit photometry. Kepler-444 is the densest star with detected solar-like oscillations. We use asteroseismology to directly measure a precise age of 11.2 ± 1.0 Gyr for the host star, indicating that Kepler-444 formed when the universe was less than 20% of its current age and making it the oldest known system of terrestrial-size planets. We thus show that Earth-size planets have formed throughout most of the universe's 13.8 billion year history, leaving open the possibility for the existence of ancient life in the Galaxy. The age of Kepler-444 not only suggests that thick-disk stars were among the hosts to the first Galactic planets, but may also help to pinpoint the beginning of the era of planet formation.

79 ASTRONOMY AND ASTROPHYSICS↗