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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 37 records · Page 2

Origin of Rapid Delithiation In Secondary Particles Of LiNi 0.8 Co 0.15 Al 0.05 O 2 and LiNi y Mn z Co 1− y − z O 2 Cathodes

Abstract Most research on the electrochemical dynamics in materials for high‐energy Li‐ion batteries has focused on the global behavior of the electrode. This approach is susceptible to misleading analyses resulting from idiosyncratic kinetic conditions, such as surface impurities inducing an apparent two‐phase transformation within LiNi 0.8 Co 0.15 Al 0.05 O 2 . Here, nano‐focused X‐ray probes are used to measure delithiation operando at the scale of secondary particle agglomerates in layered cathode materials during charge. After an initial latent phase, individual secondary particles undergo rapid, stochastic, and largely uniform delithiation, which is in contrast with the gradual increase in cell potential. This behavior reproduces across several layered oxides. Operando X‐ray microdiffraction (‐XRD) leverages the relationship between Li content and lattice parameter to further reveal that rate acceleration occurs between Li‐site fraction ( x Li ) ≈0.9 and ≈0.5 for LiNi 0.8 Co 0.15 Al 0.05 O 2 . Physics‐based modeling shows that, to reproduce the experimental results, the exchange current density ( i 0 ) must depend on x Li , and that i 0 should increase rapidly over three orders of magnitude at the transition point. The specifics and implications of this jump in i 0 are crucial to understanding the charge‐storage reaction of Li‐ion battery cathodes.

25 ENERGY STORAGE↗

Resonance-stabilized hydrocarbon-radical chain reactions may explain soot inception and growth

Mystery surrounds the transition from gas-phase hydrocarbon precursors to terrestrial soot and interstellar dust, which are carbonaceous particles formed under similar conditions. Although polycyclic aromatic hydrocarbons (PAHs) are known precursors to high-temperature carbonaceous-particle formation, the molecular pathways that initiate particle formation are unknown. We present experimental and theoretical evidence for rapid molecular clustering–reaction pathways involving radicals with extended conjugation. These radicals react with other hydrocarbon species to form covalently bound complexes that promote further growth and clustering by regenerating resonance-stabilized radicals through low-barrier hydrogen-abstraction and hydrogen-ejection reactions. Such radical–chain reaction pathways may lead to covalently bound clusters of PAHs and other hydrocarbons that would otherwise be too small to condense at high temperatures, thus providing the key mechanistic steps for rapid particle formation and surface growth by hydrocarbon chemisorption.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Evaporation of a Reactive Nanofluid Sessile Drop: Capturing Rapid Emergence of Surface Crystals with In Situ Synchrotron X-ray Diffraction

Mechanisms for surface pattern formation from evaporation of a reactive nanofluid sessile drop are not well understood. In contrast to the coffee-ring effect from inert particles, rapid chemical and morphological transformation of reactive nanoparticles upon rapid evaporative drying are challenging to probe experimentally. Here, using grazing-incidence X-ray surface scattering, the nanostructure of nascent surface patterns has been probed as a ZnO nanofluid sessile drop rapidly dries. The high temporal resolution enabled by the high flux of synchrotron X-rays allows the observation of the emergence of Zn(OH) 2 surface crystals from the onset of evaporation and their rapid evolution into the final residual surface pattern, via transient layered complexes evident from the temporary appearance of X-ray diffraction peaks preceding Zn(OH) 2 formation. The results offer mechanistic insights of morphogenesis of surface patterns from evaporation-induced self-assembly and self-organization of reactive nanofluids, previously untenable using other experimental methods.

36 MATERIALS SCIENCE↗

Hydrodynamic irreversibility of non-Brownian suspensions in highly confined duct flow

The irreversible behaviour of a highly confined non-Brownian suspension of spherical particles at low Reynolds number in a Newtonian fluid is studied experimentally and numerically. In the experiment, the suspension is confined in a thin rectangular channel that prevents complete particle overlap in the narrow dimension and is subjected to an oscillatory pressure-driven flow. In the small cross-sectional dimension, particles rapidly separate to the walls, whereas in the large dimension, features reminiscent of shear-induced migration in bulk suspensions are recovered. Furthermore, as a consequence of the channel geometry and the development and application of a single-camera particle tracking method, three-dimensional particle trajectories are obtained that allow us to directly associate relative particle proximity with the observed migration. Companion simulations of a steadily flowing suspension highly confined between parallel plates are conducted using the force coupling method, which also show rapid migration to the walls as well as other salient features observed in the experiment. While we consider relatively low volume fractions compared to most prior work in the area, we nevertheless observe significant and rapid migration, which we attribute to the high degree of confinement.

42 ENGINEERING↗

System-size dependence of the charged-particle pseudorapidity density at $\sqrt{s_{NN}}$ = 5.02 TeV for pp, p–Pb, and Pb–Pb collisions

We present the first systematic comparison of the charged-particle pseudorapidity densities for three widely different collision systems, pp, p–Pb, and Pb–Pb, at the top energy of the Large Hadron Collider ($\sqrt{s_{NN}}$ = 5.02 TeV) measured over a wide pseudorapidity range (-3.5 < η < 5), the widest possible among the four experiments at that facility. The systematic uncertainties are minimised since the measurements are recorded by the same experimental apparatus (ALICE). The distributions for p–Pb and Pb–Pb collisions are determined as a function of the centrality of the collisions, while results from pp collisions are reported for inelastic events with at least one charged particle at midrapidity. The charged-particle pseudorapidity densities are, under simple and robust assumptions, transformed to charged-particle rapidity densities. This allows for the calculation and the presentation of the evolution of the width of the rapidity distributions and of a lower bound on the Bjorken energy density, as a function of the number of participants in all three collision systems. We find a decreasing width of the particle production, and roughly a smooth ten fold increase in the energy density, as the system size grows, which is consistent with a gradually higher dense phase of matter

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

PARTICLE ACCELERATION AT LOW CORONAL COMPRESSION REGIONS AND SHOCKS

We present a study on particle acceleration in the low corona associated with the expansion and acceleration of coronal mass ejections (CMEs). Because CME expansion regions low in the corona are effective accelerators over a finite spatial region, we show that there is a rigidity regime where particles effectively diffuse away and escape from the acceleration sites using analytic solutions to the Parker transport equation. This leads to the formation of broken power-law distributions. Based on our analytic solutions, we find a natural ordering of the break energy and second power-law slope (above the break energy) as a function of the scattering characteristics. These relations provide testable predictions for the particle acceleration from low in the corona. Our initial analysis of solar energetic particle observations suggests a range of shock compression ratios and rigidity dependencies that give rise to the solar energetic particle (SEP) events studied. The wide range of characteristics inferred suggests competing mechanisms at work in SEP acceleration. Thus, CME expansion and acceleration in the low corona may naturally give rise to rapid particle acceleration and broken power-law distributions in large SEP events.

79 ASTRONOMY AND ASTROPHYSICS↗

Emergent Properties from Three-Dimensional Assemblies of (Nano)particles in Confined Spaces

The assembly of (nano)particles into compact hierarchical structures yields emergent properties not found in the individual constituents. The formation of these structures relies on a profound knowledge of the nanoscale interactions between (nano)particles, which are often designed by researchers aided by computational studies. These interactions have an effect when the (nano)particles are brought into close proximity, yet relying only on diffusion to reach these closer distances may be inefficient. Recently, physical confinement has emerged as an efficient methodology to increase the volume fraction of (nano)particles, rapidly accelerating the time scale of assembly. Specifically, the high surface area of droplets of one immiscible fluid into another facilitates the controlled removal of the dispersed phase, resulting in spherical, often ordered, (nano)particle assemblies. In this review, we discuss the design strategies, computational approaches, and assembly methods for (nano)particles in confined spaces and the emergent properties therein, such as trigger-directed assembly, lasing behavior, and structural photonic color. Finally, we provide a brief outlook on the current challenges, both experimental and computational, and farther afield application possibilities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Synthesis and characterisation of magnetic iron sulfide nanocrystals

Fe{sub 1-x}S and Fe{sub 3}S{sub 4} nanocrystals with a variety of morphologies and average sizes were synthesised by the reaction of iron(II) acetylacetonate (Fe(acac){sub 2}) and elemental sulfur in oleylamine. Reaction at 200 Degree-Sign C for 240 min produced extremely thin Fe{sub 3}S{sub 4} sheets, which displayed low coercivities (14 kA m{sup -1}) suggestive of pseudosingle-domain or multidomain particles. Reaction temperatures {>=}300 Degree-Sign C for 30 min produced 70 nm Fe{sub 1-x}S nanocrystals with hexagonal plate and hexagonal prism morphologies, which displayed high magnetic coercivities (110 kA m{sup -1}) characteristic of single magnetic domain particles. Rapid injection of sulfur solution at 280 Degree-Sign C followed by immediate cooling produced a mixture of Fe{sub 1-x}S nanocrystals and spherical, polydisperse {approx}5 nm Fe{sub 3}S{sub 4} nanocrystals, which displayed superparamagnetism above an average blocking temperature of 55 K. - Graphical abstract: Reaction of Fe(acac){sub 2} and sulfur in oleylamine produces Fe{sub 3}S{sub 4} nanocrystals at 200 Degree-Sign C and Fe{sub 1-x}S nanocrystals at 310 Degree-Sign C. Highlights: Black-Right-Pointing-Pointer Synthesis of Fe{sub 1-x}S and Fe{sub 3}S{sub 4} nanocrystals from Fe(acac){sub 2} and sulfur. Black-Right-Pointing-Pointer Fe{sub 3}S{sub 4} sheets formed after 4 h at 200 Degree-Sign C. Black-Right-Pointing-Pointer Fe{sub 1-x}S nanocrystals formed above 200 Degree-Sign C. Black-Right-Pointing-Pointer Five nanometre Fe{sub 3}S{sub 4} formed by rapid injection. Black-Right-Pointing-Pointer Five nanometre Fe{sub 3}S{sub 4} nanocrystals superparamagnetic above blocking temperature of 55 K.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Chain Dynamics in Magnetorheological Suspensions

Magnetorheological (MR) suspensions are composed of colloidal particles which acquire dipole moments when subjected to an external magnetic field. At sufficient field strengths and concentrations, the dipolar particles rapidly aggregate to form long chains. Subsequent lateral cross-linking of the dipolar chains is responsible for a rapid liquid-to-solid-like rheological transition. The unique, magnetically-activated rheological properties of MR suspensions make them ideal for interfacing mechanical systems to electronic controls. Additionally, the ability to experimentally probe colloidal suspensions interacting through tunable anisotropic potentials is of fundamental interest. Our current experimental work has focused on understanding the fluctuations of dipolar chains. It has been proposed by Halsey and Toor (HT) that the strong Landau-Peierls thermal fluctuations of dipolar chains could be responsible for long-range attractions between chains. Such interactions will govern the long-time relaxation of MR suspensions. We have synthesized monodisperse neutrally buoyant MR suspensions by density matching stabilized ferrofluid emulsion droplets with D2O. This allows us to probe the dynamics of the dipolar chains using light scattering without gravitational, interfacial, and polydispersity effects to resolve the short-wavelength dynamics of the dipolar chains. We used diffusing wave spectroscopy to measure these dynamics. The particle displacements at short times that show an independence to the field strength, but at long times exhibit a constrained, sub-diffusive motion that slows as the dipole strength is increased. The experiments are in good qualitative agreement with Brownian dynamics simulations of dipolar chains. Although there have been several important and detailed studies of the structure and interactions in MR suspensions, there has not been conclusive evidence that supports or contradicts the HT model prediction that long-range interactions exist between fluctuating chains of dipolar particles. Resolving this issue would contribute greatly to the understanding of these interesting and important materials. We have begun to test the predictions of the HT model by both examining the dynamics of individual chains and by measuring the forces between dipolar chains directly to accurately and quantitatively assess the interactions that they experience. To do so, we employ optical trapping techniques and video-microscopy to manipulate and observe our samples on the microscopic level. With these techniques, it is possible to observe chains that are fluctuating freely in three-dimensions, independent of interfacial effects. More importantly, we are able to controllably observe the interactions of two chains at various separations to measure the force-distance profile. The techniques also allow us to study the mechanical properties of individual chains and chain clusters. Our work to this point has focused on reversibly-formed dipolar chains due to field induced dipoles where the combination of this chaining, the dipolar forces, and the hydrodynamic interactions that dictate the rheology of the suspensions. One can envision, however, many situations where optical, electronic, or rheological behavior may be optimized with magneto-responsive anisotropic particles. Chains of polarizable particles may have the best properties as they can coil and flex in the absence of a field and stiffen and orient when a field is applied. We have recently demonstrated a synthesis of stable, permanent paramagnetic chains by both covalently and physically linking paramagnetic colloidal particles. The method employed allows us to create monodisperse chains of controlled length. We observed the stability, field-alignment, and rigidity of this new class of materials. The chains may exhibit unique rheological properties in an applied magnetic field over isotropic suspensions of paramagnetic particles. They are also useful rheological models as bead-spring systems. These chains form the basis for our current experiments with optical traps.

Gast, A. P.↗

Cell migration is another player of the minute virus of mice infection

The parvovirus minute virus of mice, prototype strain (MVMp), preferentially infects and kills cancer cells. This intrinsic MVMp oncotropism may depend in part on the early stages of MVMp infection. To test this hypothesis, we investigated the early events of MVMp infection in mouse LA9 fibroblasts and a highly invasive mouse mammary tumor cell line derived from polyomavirus middle T antigen-mediated transformation. Using a combination of fluorescence and electron microscopy, we found that various parameters of the cell migration process affect MVMp infection. We show that, after binding to the plasma membrane, MVMp particles rapidly cluster at the leading edge of migrating cells, which exhibit higher levels of MVMp uptake than non-motile cells. Moreover, promoting cell migration on a fibronectin matrix increased MVMp infection, and induction of epithelial–mesenchymal transition allowed MVMp replication in non-permissive epithelial cells. Hence, we propose that cell migration influences the early stages of MVMp infection. - Highlights: • We document early steps of MVMp infection. • We report that a fibronectin matrix promotes MVMp infection. • We show that cellular migration plays a role in MVMp uptake. • We show that epithelial–mesenchymal transition allows MVMp replication.

60 APPLIED LIFE SCIENCES↗

Analysis of solid uranium particulates on cotton swipes with an automated microextraction-ICP-MS system

Here, an automated microextraction method coupled to an inductively coupled plasma – mass spectrometer (ICP-MS) was developed for the direct analysis of solid uranium particulates on the surface of cotton swipes. The microextraction probe extracts particulates from the sample surface, in a flowing solvent, and directs the removed analyte to an ICP-MS for isotopic determination. The automated system utilizes a mechanical XY stage that is software controlled with the capability of saving and returning to specific locations and a camera focused to the swipe surface for optimal viewing of the extracted locations (i.e., material present). Here, particulates (n = 135) were extracted and measured by ICP-MS, including 35 depleted uranyl nitrate hexahydrate (UN) (used for mass bias corrections), 50 uranyl fluoride (UO 2 F 2 ), and 50 uranyl acetate (UAc) particulates. Blank extractions were performed on the cotton swipes between triplicate sample analyses. Between each swipe extraction, the probe was sent between two wells containing 10% and 5% HNO 3 to clean the probe head and to eliminate any analyte carryover between particulates. The measured 235 U/ 238 U and 234 U/ 238 U isotope ratios for the UO 2 F 2 particulates were 0.00725(8) and 0.000054(4), a percent relative difference (% RD) of –0.041% and –1.7% from the reference isotope ratios determined in-lab through multi-collector ICP-MS analysis of dissolved aliquots of the U material. The UAc samples had a measured 235 U/ 238 U isotope ratio of 0.00206(7), a –0.96% relative difference from the reference value of 0.00208(1). The 234 U/ 238 U and 236 U/ 238 U isotope ratios were 0.000008(1) and 0.000031(4), –5.1% RD and –4.3% RD, respectively. The automated sample stage enabled seamless and rapid particle analysis, leading to a significant increase in throughput versus what was previously possible. Additionally, the saved location capability reduced user sampling error as sampling locations were easily stored and recalled. Analysis of U particles on the swipe surface – including blanks, mass bias, and triplicate extractions – was completed in less than an hour without any sample preparation necessary.

47 OTHER INSTRUMENTATION↗

A very small and super strong zebra pattern burst at the beginning of a solar flare

Microwave emission with spectral zebra pattern structures (ZPs) is frequently observed in solar flares and the Crab pulsar. The previous observations show that ZP is a structure only overlapped on the underlying broadband continuum with slight increments and decrements. This work reports an unusually strong ZP burst occurring at the beginning of a solar flare observed simultaneously by two radio telescopes located in China and the Czech Republic and by the EUV telescope on board NASA's satellite Solar Dynamics Observatory on 2013 April 11. It is a very short and super strong explosion whose intensity exceeds several times that of the underlying flaring broadband continuum emission, lasting for just 18 s. EUV images show that the flare starts from several small flare bursting points (FBPs). There is a sudden EUV flash with extra enhancement in one of these FBPs during the ZP burst. Analysis indicates that the ZP burst accompanying an EUV flash is an unusual explosion revealing a strong coherent process with rapid particle acceleration, violent energy release, and fast plasma heating simultaneously in a small region with a short duration just at the beginning of the flare.

79 ASTRONOMY AND ASTROPHYSICS↗

RAPID COSMIC-RAY ACCELERATION AT PERPENDICULAR SHOCKS IN SUPERNOVA REMNANTS

Perpendicular shocks are shown to be rapid particle accelerators that perform optimally when the ratio u{sub s} of the shock speed to the particle speed roughly equals the ratio 1/η of the scattering rate to the gyro frequency. We use analytical methods and Monte-Carlo simulations to solve the kinetic equation that governs the anisotropy generated at these shocks, and find, for ηu{sub s} ≈ 1, that the spectral index softens by unity and the acceleration time increases by a factor of two compared to the standard result of the diffusive shock acceleration theory. These results provide a theoretical basis for the 30 year old conjecture that a supernova exploding into the wind of a Wolf–Rayet star may accelerate protons to an energy exceeding 10{sup 15} eV.

79 ASTRONOMY AND ASTROPHYSICS↗

Analysis of variances of quasirapidities in collisions of gold nuclei with track-emulsion nuclei

A new method of an analysis of variances was developed for studying n-particle correlations of quasirapidities in nucleus-nucleus collisions for a large constant number n of particles. Formulas that generalize the results of the respective analysis to various values of n were derived. Calculations on the basis of simple models indicate that the method is applicable, at least for n {>=} 100. Quasirapidity correlations statistically significant at a level of 36 standard deviations were discovered in collisions between gold nuclei and track-emulsion nuclei at an energy of 10.6 GeV per nucleon. The experimental data obtained in our present study are contrasted against the theory of nucleus-nucleus collisions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Fast and sensitive measurements of sub-3 nm particles using Condensation Particle Counters For Atmospheric Rapid Measurements (CPC FARM)

New particle formation (NPF) is the atmospheric process whereby gas molecules react and nucleate to form detectable particles. NPF has a strong impact on Earth's radiative balance as it produces roughly half of global cloud condensation nuclei. However, the time resolution and sensitivity of current instrumentation are inadequate in measuring the size distribution of sub-3 nm particles, the particles critical for understanding NPF. Here we present the Condensation Particle Counters For Atmospheric Rapid Measurements (CPC FARM), a method to measure the concentrations of freshly nucleated particles. The CPC FARM consists of five CPCs operating in parallel, each configured to operate at different detectable particle sizes between 1–3 nm. This study explores two methods to calculate the size distribution from the differential measurements across the CPC channels. The performance of both inversion methods was tested against the size distribution measured by a pair of stepping particle mobility sizers (SMPSs) during an ambient air sampling study in Pittsburgh, PA. Observational results indicate that the CPC FARM is more accurate with higher time resolution and sensitivity in the sub-3 nm range compared to the SMPS.

Cheng, Darren [Carnegie Mellon Univ., Pittsburgh, ↗

Particle production with rapidity correlations in proton-nucleus collisions

We illustrate how a generalization of the JIMWLK formalism which treats independently the direct and complex conjugate amplitudes can be used to describe semi-inclusive multiparticle production with rapidity correlations in pA collisions. The evolution equations that are obtained with this formalism are susceptible of numerical implementation as a Langevin process.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Continuum representation of a continuous size distribution of particles engaged in rapid granular flow

Natural and industrial granular flows often consist of several particle sizes, approximately forming a continuous particle size distribution (PSD). Continuous PSDs are ubiquitous, though existing kinetic-theory-based, hydrodynamic models for rapid granular flows are limited to a discrete number of species. The objective of this work is twofold: (i) to determine the number of discrete species required to accurately approximate a continuous PSD and (ii) to validate these results via a comparison with molecular dynamics (MD) simulations of continuous PSDs. With regard to the former, several analytic (Gaussian and lognormal) and experimental (coal and lunar soil simulants) distributions are investigated. Transport coefficients (pressure, shear viscosity, etc.) of the granular mixture given by the polydisperse theory of Garz´o et al. [“Enskog theory for polydisperse granular mixtures. I. Navier-Stokes order transport,” Phys. Rev. E 76, 031303 (2007);“Enskog theory for polydisperse granular mixtures. I. Navier-Stokes order transport,” 76, 031304 (2007)] are compared using an increasing number of species s to approximate the given PSD. These discrete approximations are determined by matching the first 2s moments of the approximation and the given continuous distribution. Relatively few species are required to approximate moderately wide distributions (Gaussian, lognormal), whereas even wider distributions (coal and lunar soil simulants) require a larger number of species. Regarding the second objective, a comparison between MD simulations and kinetictheory predictions for a simple shear flow of both Gaussian and lognormal PSDs reveal essentially no loss of accuracy stemming from the polydisperse theory itself (as compared to theories for monodisperse systems) or from the discrete approximations of continuous PSDs used in the polydisperse theory. C 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4744987]

97 MATHEMATICS AND COMPUTING↗