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At least 73 records · Page 4

O 2 -Oxidation of Individual Graphite and Graphene Nanoparticles in the 1200 – 2200 K Range: Particle-to-Particle Variations and the Evolution of the Reaction Rates and Optical Properties

The kinetics for O 2 oxidation of individual graphite and graphene platelet nanoparticles (NPs) were studied as a function of temperature (1200 to 2200 K) at varying oxygen partial pressures, using a single nanoparticle mass spectrometry method. NP temperature (TNP) was measured by measuring the NP thermal emission spectra during the kinetics studies. The initial oxidation efficiency is found to peak in the 1200 to 1500 K range, dropping by an order of magnitude as TNP was increased above 2000 K. There were large NP-to-NP variations in the oxidation rates, attributed to variations in the NP surface structure. In addition, the oxidation efficiencies evolved, non-monotonically, as the NPs reacted, decreasing by factors of between 10 and 300. This evolution of reactivity is attributed to changes in the NP surface structure due to the combination of oxidation and annealing. In conclusion, the optical properties, including wavelength dependence of the emissivity and the absorption cross section for the 532 nm heating laser, also tended to evolve as the NPs oxidized, but differently for each individual NP, presumably reflecting differences in the initial structures and their evolution.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Observations and Parameterizations of Particle Size Distributions in Deep Tropical Cirrus and Stratiform Precipitation Clouds: Results from In-Situ Observations in TRMM Field Campaigns

In this study, we report on the evolution of particle size distributions (PSDs) and habits as measured during slow, Lagrangian-type spiral descents through deep subtropical and tropical cloud layers in Florida, Brazil, and Kwajalein, Marshall Islands, most of which were precipitating. The objective of the flight patterns was to learn more about how the PSDs evolved in the vertical and to obtain information of the vertical structure of microphysical properties. New instrumentation yielding better information on the concentrations of particles in the size (D) range between 0.2 and 2 cm, as well as improved particle imagery, produced more comprehensive observations for tropical stratiform precipitation regions and anvils than have been available previously. Collocated radar observations provided additional information on the vertical structure of the cloud layers sampled. Most of the spirals began at cloud top, with temperatures (T) as low as -50 C, and ended at cloud base or below the melting layer (ML). The PSDs broadened from cloud top towards cloud base, with the largest particles increasing in size from several millimeters at cloud top to one centimeter or larger towards cloud base. Some continued growth was noted in the upper part of the ML. Concentrations of particles less than 1 mm in size decreased with decreasing height. The result was a consistent change in the PSDs in the vertical. Similarly, systematic changes in the size dependence of the particle cross-sectional area was noted with decreasing height. Aggregation-as ascertained from both the changes in the PSDs and evolution of particle habits as observed in high detail with the cloud particle imager (CPI) probe-was responsible for these trends. The PSDs were generally well-represented by gamma distributions of the form N = N0 gamma D microns e- lambda gamma D that were fitted to the PSDs over 1-km horizontal intervals throughout the spirals. The intercept (N0 gamma), slope (lambda gamma), and dispersion (microns) values were derived for each PSD. Exponential curves (N = N0e- lambdaD; micron = 0) were also fitted to the distributions. The lambda gamma values for given spirals varied systematically with temperature as did the values of lambda (exponential), and the data generally conformed to values found in previous studies involving exponential fits to size distributions in mid-latitude frontal and cirrus layers. Considerable variability often noted in the PSD properties during the loops of individual spirals was manifested primarily in large changes in N0 gamma and N0, but micron, lambda gamma and lambda remained fairly stable. Temperature is not found to be the sole factor controlling lambda gamma or lambda but is a primary one. Direct relationships were found between lambda gamma and N0 gamma or lambda gamma and micron for the gamma distributions and lambda and N0 for the exponential. The latter relationship was not found as distinctly in earlier studies; observed PSDs in this study had better fidelity with less scatter. The micron values changed monotonically with T over the range of temperatures and were directly related to N0 gamma or lambda gamma, thereby reducing the number of variables in the PSD functional equation to two. In the upper part of the ML, N0 and lambda continued to decrease, and in the lower part these values began to increase as the largest particles melted. We developed general expressions relating various bulk microphysical, radar, and radiative transfer-related variables to N0 gamma and lambda gamma, useful for both tropical and mid-latitude clouds. These relationships facilitate the specification of a number of bulk properties in cloud and climate models. The results presented in this paper apply best to temperatures between 0 and -40 C, for which the measured radar reflectivities fall in the range of 0 to 25 dBZe.

Heymsfield, Andrew J.↗

The role of cometary particle coalescence in chemical evolution

Important prebiotic organic compounds might have been transported to earth in dust or produced in vapor clouds resulting from atmospheric explosions or impacts of comets. These compounds coalesced in the upper atmosphere with particles ejected from craters formed by impacts of large objects. Coalescence during exposure to UV radiation concentrated organic monomers and enhanced formation of oligomers. Continuing coalescence added material to the growing particles and shielded prebiotic compounds from prolonged UV radiation. These particles settled into the lower atmosphere where they were scavenged by rain. Aqueous chemistry and evaporation of raindrops containing monomers in high temperature regions near the earth's surface also promoted continued formation of oligomers. Finally, these oligomers were deposited in the oceans where continued prebiotic evolution led to the most primitive cell. Results of present studies suggest that prebiotic chemical evolution may be an inevitable consequence of impacting comets during the late accretion of planets anywhere in the universe if oceans remained on those planetary surfaces.

Oberbeck, V. R.↗

Evolution of photon and particle spectra in compact, luminous objects

The physics of high energy photons and particles (especially electrons and positrons) in the compact, high-energy-density of galactic nuclei and quasars was investigated. A numerical code was developed which follows the nonlinear spectral evolution of a pair/photon plasma, due to two-body scattering and interaction process, in an unmagnetized system. The code was applied both to static plasmas and to relativistic expanding winds.

Eilek, Jean A.↗

Evolution of the marker distribution in gyrokinetic $δf$ particle-in-cell simulations

The evolution of the particle weight in a δf particle-in-cell simulation depends on the marker distribution that can evolve in a turbulent field due to turbulent diffusion. When Monte Carlo methods are used to implement the test particle collision operator, or when the particle motion is not strictly Hamiltonian in a collisionless simulation, the marker distribution will evolve along the particle trajectory and, in general, cannot be known exactly. A two-dimensional numerical marker distribution is proposed as an approximation. It is shown to be advantageous over other common methods for evaluating the marker distribution in long-time turbulence simulations. A generalized two-weight δf-method is proposed to mitigate the marker evolution problem.

, Monte Carlo methods↗

Shock-driven dispersal of a corrugated finite-thickness particle layer

A research area emerging in the multiphase flow community is the study of shock-driven multiphase instability (SDMI), a gas–particle analog of the traditional fluid-fluid Richtmyer–Meshkov instability (RMI). In this work, we study the interaction of planar air shocks with corrugated glass particle curtains through the use of numerical simulations with an Eulerian–Lagrangian approach. One objective of this study is to compare the simulated particle curtains to a comparable set of shock tube experiments performed to analyze traditional RMI of a gas curtain. The simulations are set to match the experimental shock Mach numbers and perturbation wavelengths (3.6 and 7.2 mm) while also matching the Atwood number of the experiments to the multiphase Atwood number of the simulations. Varying particle diameters are tested in the simulations to explore the impact of particle diameter on the evolution of the particle curtain. This simulation setup allows for a one-to-one comparison between RMI and SDMI under comparable conditions while also allowing for a separate study into the validity of the use of the multiphase Atwood number to compare the single-phase and multiphase instabilities. In particular, we show that the comparison depends on the diameter of the particles (thus, dependent on the Stokes number of the flow). A second objective of this study is to analyze the effect of the initial particle volume fraction on the evolution of the curtain and the behavior of the instability. This is done through analyzing the effect of the multiphase terms of the vorticity evolution equation on the vorticity deposition in SDMI. Also discussed is the effect of the particle diameter on the multiphase generation terms as well as in the baroclinic vorticity generation term in SDMI as the shock passes over the curtain.

42 ENGINEERING↗

The Thermal Expansion of Ring Particles and the Secular Orbital Evolution of Rings Around Planets and Asteroids

The thermal expansion and contraction of ring particles orbiting a planet or asteroid can cause secular orbit evolution. This effect, called here the thermal expansion effect, depends on ring particles entering and exiting the shadow of the body they orbit. A particle cools off in the shadow and heats up again in the sunshine, suffering thermal contraction and expansion. The changing cross-section it presents to solar radiation pressure plus time lags due to thermal inertia lead to a net along-track force. The effect causes outward drift for rocky particles. For the equatorial orbits considered here, the thermal expansion effect is larger than Poynting-Robertson drag in the inner solar system for particles in the size range approx. 0.001 - 0.02 m. This leads to a net increase in the semimajor axis from the two opposing effects at rates ranging from approx. 0.1 R per million years for Mars to approx. 1 R per million years for Mercury, for distances approx. 2R from the body, where R is the body's radius. Asteroid 243 Ida has approx. 10 R per million years, while a hypothetical Near-Earth Asteroid (NEA) can have faster rates of approx. 0.5 R per thousand years, due chiefly to its small radius compared to the planets. The thermal expansion effect weakens greatly at Jupiter and is overwhelmed by Poynting-Robertson for icy particles orbiting Saturn. Meteoroids in eccentric orbits about the Sun also suffer the thermal expansion effect, but with only approx. 0.0003e2 AU change in semimajor axis over a million years for a 2 m meteoroid orbiting between Mercury and Earth.

Ring particles↗

What Controls Crystal Diversity and Microphysical Variability in Cirrus Clouds?

Abstract Variability of ice microphysical properties like crystal size and density in cirrus clouds is important for climate through its impact on radiative forcing, but challenging to represent in models. For the first time, recent laboratory experiments of particle growth (tied to crystal morphology via deposition density) are combined with a state‐of‐the‐art Lagrangian particle‐based microphysics model in large‐eddy simulations to examine sources of microphysical variability in cirrus. Simulated particle size distributions compare well against balloon‐borne observations. Overall, microphysical variability is dominated by variability in the particles' thermodynamic histories. However, diversity in crystal morphology notably increases spatial variability of mean particle size and density, especially at mid‐levels in the cloud. Little correlation between instantaneous crystal properties and supersaturation occurs even though the modeled particle morphology is directly tied to supersaturation based on laboratory measurements. Thus, the individual thermodynamic paths of each particle, not the instantaneous conditions, control the evolution of particle properties.

54 ENVIRONMENTAL SCIENCES↗

Pinatubo Global- to Micro-Scale Evolution: A Unified Picture from Space, Air, and Ground Measurements

We combine space, air, and ground measurements to develop a composite picture of the post-Pinatubo aerosol, and assess the consistency and uncertainties of various measurement and retrieval techniques. impactor and optical counter measurements, as well as retrievals from optical depth spectra, paint a generally consistent picture of the evolution of particle effective radii, R(sub eff). In the first month after the eruption, although particle numbers increased by orders of magnitude, R(sub eff) was similar to the preeruption value of 4.2 micrometers, because both small (r less than 0.25 micrometers) and large (r greater than 0.6 micrometers) particles increased in number, Over the next 3-6 months, R(sub eff) increased rapidly to about 0.5 micrometers. In general, R(sub eff) continued to increase for about a year after the eruption. The peak wavelength of optical depth spectra increased from initial values of less than 0.42 micrometers to values between 0.78 and 1 micrometer. This coupled evolution in particle size distribution and optical depth spectra helps explain the relationship between the global maps of 0.5 and 1.0-micrometer optical depth derived from the AVHRR and SAGE satellite measurements. It also sets a context for evaluating remaining uncertainties in each of these satellite data products. We also make consensus recommendations for particle composition, shape, and temperature- and wavelength-dependent refractive index, and show how the latter effect on backscatter spectra can influence particle sizes retrieved from multiwavelength lidar measurements.

Russell, Philip B.↗

Cosmic-ray propagation. I.

Charged particle motion in random magnetic field, describing time evolution of particle distribution in pitch angle and position in terms of Fokker- Planck coefficients

INTERPLANETARY MAGNETIC FIELD↗

The dispersive evolution of charged-particle bunches in random magnetic fields

Shortly after a strongly anisotropic beam of charged particles is injected along a guiding magnetic field on which is superimposed a small random conponent, the particle density can be represented by a Gaussian profile whose center moves with the coherent velocity and whose width increases with time at a rate controlled by the coefficient of dispersion. Both parameters depend upon the mean free path, which characterizes scattering by the random fields, and the focusing length, which characterizes spatial variations of the guiding field. These dependencies are known explicitly for the coherent velocity. Formulae for coefficient of dispersion are available only in the limits of very weak and very strong focusing. A new expression for coefficient of dispersion, which spans this gap, is presented.

Earl, J. A.↗

Evolution of Photon and Particle Spectra in Compact, Luminous Objects

Physical conditions in the radiating plasma in the cores of radio-strong quasars and active galactic nuclei cannot be derived from observations until the effects of relativistic aberration are understood. This requires determining both the bulk flow speeds and any wave or signal speed in the parsec-scale nuclear jets. In this project we studied several aspects of such waves. We considered constraints on jet deceleration by mass pickup, and found that bolometric luminosities of the active nuclei cannot constrain core jet speeds usefully. We also simulated observations of ballistic, helical trajectories and helical waves moving directly outwards along the jet. We found that ballistic trajectories are not allowed by the data; the helical features seen are very likely to be helical waves. We believe these are waves propagating in the jet plasma. To this end, we studied waves propagating in relativistic pair plasma jets. In particular, we undertook a program whose goal was to determine the nature of waves which can propagate in relativistic pair plasmas, and how such waves propagating in streaming jet plasma would be observed by an external observer. We developed the possibility of using pulsars as test cases for our models; this takes advantage of new technology in pulsar observations, and the similarity of the physical conditions in the pulsar magnetosphere to the dense, relativistic pair plasmas which exist in radio-strong quasars.

Eilek, Jean A.↗