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Machine reduces gravitational effects interfering with particle growth. Reaction chamber rotates while polymerization of latex proceeds. Motor turns stirrer. Chamber made of stainless steel with glass windows.
The interplay of moist convection and particle growth in the tropopause region of the atmospheres of earth, Uranus, and Neptune has been investigated. It is found that the downward flux of aerosols is not sufficient to dehydrate the earth's stratosphere by chemical dessication, and that the source of Neptune's oversaturated stratosphere is convective penetration of the tropopause by moist convective columns of methane. It is shown that conditions in the troposphere of Uranus are not conducive to the initiation of moist convection.
Coagulation of grains in the solar nebula should result in formation of low-density aggregates with fractal structure. The opacity of the nebula remains much higher than computed for the assumption that particles are compact. Timescales for particle growth, settling to the central plane of the nebula, and formation of planetesimals are lengthened significantly.
Ice particles created in polar stratospheric cooling events are predicted to descend into Type I PSCs and accrete a coating of nitric acid trihydrate (NAT) that inhibits evaporation. Coated particles efficiently strip HNO3 from the atmosphere, providing a mechanism for denitrification without significant dehydration. Coatings that disintegrate may release large particles of NAT that influence subsequent particle growth.
Formation of planetesimals is discussed. The following subject areas are covered: (1) nebular structure; (2) aerodynamics of the solid bodies in the nebula; (3) problems with gravitational instability; (4) particle growth by coagulation; properties of fractal aggregates; and (5) coagulation and settling of fractal aggregates.
In situ aircraft measurements in the lower stratosphere are used to investigate the reactive nitrogen, NO(y), total water, and particle components of the polar stratospheric cloud (PSC) aerosol in the Arctic. The results are compared to findings from the Antarctic derived using similar measurements and interpretive techniques. The Arctic data show that particle volume well above background values is present at temperatures above the frostpoint, confirming the result from the Antarctic that the observed PSCs are not water ice particles. NO(y) measurements inside a PSC are enhanced above ambient values consistent with anisokinetic sampling of particles containing NO(y). In the Arctic data over long segments of several flights, calculations show saturation with respect to nitric acid trihydrate without significant PSC particle growth above background.
This study investigates ice nucleation mechanisms in cold lenticular wave clouds, a cloud type characterized by quasi-steady-state air motions and microphysical properties. It is concluded that homogeneous ice nucleation is responsible for the ice production in these clouds at temperatures below about -33 C. The lack of ice nucleation observed above -33 C indicates a dearth of ice-forming nuclei, and hence heterogeneous ice nucleation, in these clouds. Aircraft measurements in the temperature range -31 to -41 C show the following complement of simultaneous and abrupt changes in cloud properties that indicate a transition from the liquid phase to ice: disappearance of liquid water; decrease in relative humidity from near water saturation to ice saturation; increase in mean particle size; change in particle concentration; and change in temperature due to the release of latent heat. A numerical model of cloud particle growth and homogeneous ice nucleation is used to aid in interpretation of our in situ measurements. The abrupt changes in observed cloud properties compare favorably, both qualitatively and quantitatively, with results from the homogeneous ice nucleation model. It is shown that the homogeneous ice nucleation rates from the measurements are consistent with the temperature-dependent rates employed by the model (within a factor of 100, corresponding to about 1 C in temperature) in the temperature range -35 deg to -38 C. Given the theoretical basis of the modeled rates, it may be reasonable to apply them throughout the -30 to -50 C temperature range considered by the theory.
This study builds upon the microphysical modeling described in Part 1 by deriving formulations for the extinction and absorption coefficients in terms of the size distribution parameters predicted from the micro-physical model. The optical depth and single scatter albedo of a cirrus cloud can then be determined, which, along with the asymmetry parameter, are the input parameters needed by cloud radiation models. Through the use of anomalous diffraction theory, analytical expressions were developed describing the absorption and extinction coefficients and the single scatter albedo as functions of size distribution parameters, ice crystal shapes (or habits), wavelength, and refractive index. The extinction coefficient was formulated in terms of the projected area of the size distribution, while the absorption coefficient was formulated in terms of both the projected area and mass of the size distribution. These properties were formulated as explicit functions of ice crystal geometry and were not based on an 'effective radius.' Based on simulations of the second cirrus case study described in Part 1, absorption coefficients predicted in the near infrared for hexagonal columns and rosettes were up to 47% and 71% lower, respectively, than absorption coefficients predicted by using equivalent area spheres. This resulted in single scatter albedos in the near-infrared that were considerably greater than those predicted by the equivalent area sphere method. Reflectances in this region should therefore be underestimated using the equivalent area sphere approach. Cloud optical depth was found to depend on ice crystal habit. When the simulated cirrus cloud contained only bullet rosettes, the optical depth was 142% greater than when the cloud contained only hexagonal columns. This increase produced a doubling in cloud albedo. In the near-infrared (IR), the single scatter albedo also exhibited a significant dependence on ice crystal habit. More research is needed on the geometrical properties of ice crystals before the influence of ice crystal shape on cirrus radiative properties can be adequately understood. This study provides a way of coupling the radiative properties of absorption, extinction, and single scatter albedo to the microphysical properties of cirrus clouds. The dependence of extinction and absorption on ice crystal shape was not just due to geometrical differences between crystal types, but was also due to the effect these differences had on the evolution of ice particle size spectra. The ice particle growth model in Part 1 and the radiative properties treated here are based on analytical formulations, and thus represent a computationally efficient means of modeling the microphysical and radiative properties of cirrus clouds.
Laser ablation has been used ex situ to create metal nanoparticles for introduction into a reactive pyrolysis flame. By prior synthesis of the metal nanoparticles, the effects of the reactive gases can be clearly separated from the pyrolysis chemistry of a solvent carrier, as when nebulized solutions are used. Moreover, varying reactivity issues associated with particle growth and size are bypassed. Our results show that Fe selectively reacts with CO to produce nanotubes, whereas Ni selectively reacts with C2H2 to produce nanofibers. These observations are interpreted through the donation and withdrawal of electron density between the adsorbate's molecular orbitals and surface atoms of the metal nanoparticle. The rate of reaction of Ni with only C2H2 is found to be greater than the rate with C2H2 and CO. This suggests that CO inhibits the Ni-catalyzed reaction.
A method of making metal oxide clusters in a single stage by reacting a metal oxide with a substoichiometric amount of an acid in the presence of an oxide particle growth terminator and solubilizer. A method of making a ceramer is also disclosed in which the metal oxide clusters are reacted with a functionalized polymer. The resultant metal oxide clusters and ceramers are also disclosed.
A method of making metal oxide clusters in a single stage by reacting a metal oxide with a substoichiometric amount of an acid in the presence of an oxide particle growth terminator and solubilizer. A method of making a ceramer is also disclosed in which the metal oxide clusters are reacted with a functionalized polymer. The resultant metal oxide clusters and ceramers are also disclosed.
Polar stratospheric clouds (PSC) play a primary role in the formation of annual ozone holes over Antarctica during the austral sunrise. Meridional temperature gradients in the lower stratosphere and upper troposphere, caused by strong radiative cooling, induce a broad dynamic vortex centered near the South Pole that decouples and insulates the winter polar airmass. PSC nucleate and grow as vortex temperatures gradually fall below equilibrium saturation and frost points for ambient sulfate, nitrate, and water vapor concentrations (generally below 197 K). Cloud surfaces promote heterogeneous reactions that convert stable chlorine and bromine-based molecules into photochemically active ones. As spring nears, and the sun reappears and rises, photolysis decomposes these partitioned compounds into individual halogen atoms that react with and catalytically destroy thousands of ozone molecules before they are stochastically neutralized. Despite a generic understanding of the ozone hole paradigm, many key components of the system, such as cloud occurrence, phase, and composition; particle growth mechanisms; and denitrification of the lower stratosphere have yet to be fully resolved. Satellite-based observations have dramatically improved the ability to detect PSC and quantify seasonal polar chemical partitioning. However, coverage directly over the Antarctic plateau is limited by polar-orbiting tracks that rarely exceed 80 degrees S. In December 1999, a NASA Micropulse Lidar Network instrument (MPLNET) was first deployed to the NOAA Earth Systems Research Laboratory (ESRL) Atmospheric Research Observatory at the Amundsen-Scott South Pole Station for continuous cloud and aerosol profiling. MPLNET instruments are eye-safe, capable of full-time autonomous operation, and suitably rugged and compact to withstand long-term remote deployment. With only brief interruptions during the winters of 2001 and 2002, a nearly continuous data archive exists to the present.
Saturn's moon Titan has a nitrogen atmosphere comparable to Earth's, with a surface pressure of 1.4 bar. Numerical models reproduce the tropospheric conditions very well but have trouble explaining the observed middle-atmosphere temperatures, composition and winds. The top of the middle-atmosphere circulation has been thought to lie at an altitude of 450 to 500 kilometres, where there is a layer of haze that appears to be separated from the main haze deck. This 'detached' haze was previously explained as being due to the colocation of peak haze production and the limit of dynamical transport by the circulation's upper branch. Herewe report a build-up of trace gases over the south pole approximately two years after observing the 2009 post-equinox circulation reversal, from which we conclude that middle-atmosphere circulation must extend to an altitude of at least 600 kilometres. The primary drivers of this circulation are summer-hemisphere heating of haze by absorption of solar radiation and winter-hemisphere cooling due to infrared emission by haze and trace gases; our results therefore imply that these effects are important well into the thermosphere (altitudes higher than 500 kilometres). This requires both active upper-atmosphere chemistry, consistent with the detection of high-complexity molecules and ions at altitudes greater than 950 kilometres, and an alternative explanation for the detached haze, such as a transition in haze particle growth from monomers to fractal structures.
The fundamental role of polar stratospheric clouds (PSCs) in the depletion of stratospheric ozone is well established. Heterogeneous reactions on PSCs convert the stable chlorine reservoirs HCl and ClONO2 to chlorine radicals that destroy ozone catalytically. PSCs also prolong ozone depletion by delaying chlorine deactivation through the removal of gas-phase HNO3 and H2O by sedimentation of large PSC particles. There has been substantial recent progress in our understanding of PSC processes due to the long-term, vortex-wide observations from the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) lidar on the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) satellite and the MLS (Microwave Limb Sounder) on the Aura satellite. The CALIOP observations provide unprecedented high spatial resolution information on particulate aerosol/PSC morphology and composition, while MLS provides complementary collocated measurements of gas-phase HNO3 and H2O, the major constituents of all PSC particles. The combined analyses of these datasets have enabled better PSC composition discrimination and provided valuable new insight into PSC formation processes and particle growth kinetics. The more than 17 years of CALIOP and MLS data have uniquely captured the primary aspects of the seasonal and multi-year variability of PSCs in the Arctic and Antarctic, enabling the development of a state-of-the-art reference PSC data record and climatology. In this presentation, we highlight the significant advances in our understanding achieved during this golden era of spaceborne PSC observations and identify remaining gaps in our knowledge that future spaceborne lidar missions may help resolve.
Wave amplification by downgoing particles in a common flare model is investigated. The flare is assumed to occur at the top of a coronal magnetic flux loop, and results in the heating of plasma in the flaring region. The hot electrons propagate down the legs of the flux tube towards increasing magnetic field. It is simple to demonstrate that the velocity distributions which result in this model are unstable to both beam instabilities and cyclotron maser action. An explanation is presented for the propagation effects on the distribution, and the properties of the resulting amplified waves are explored, concentrating on cyclotron maser action, which has properties (emission in the z mode below the local gyrofrequency) quite different from maser action by other distributions considered in the context of solar flares. The z mode waves will be damped in the coronal plasma surrounding the flaring flux tube and lead to heating there. This process may be important in the overall energy budget of the flare. The downgoing maser is compared with the loss cone maser, which is more likely to produce observable bursts.
The method of seeded growth was studied for producing mondisperse colloidal silica particles. It was shown that particle size as well as weight percent solids could be controlled by using this method. The particles were characterized by transmission electron microscopy (TEM) and quasielastic light scattering (QELS). The particles were found to have a bimodal size distribution when examined by TEM. The particle size as determined by QELS was found to be roughly 10-20% larger than the particle size as determined by TEM. Furthermore, the polydispersity (standard deviation/mean particle size) as determined by QELS was found to be significantly lower than the polydispersity as determined by TEM. This underscores the importance of using TEM as a characterization technique for determining particle monodispersity. It was also noted that there was an increase in particle roughness as the weight percent of the silica particles increased and a new nucleation of particles was observed as the weight percent approached 13%. A recipe for producing monodisperse silica particles in the 150 nm size range is presented.
Growth of nitric acid trihydrate (NAT) particles on background stratospheric aerosols is examined for an isolated air parcel cooled at a uniform rate. During the process of nucleation, the saturation ratio of HNO3 vapor reaches a maximum value between 2 and 15, corresponding to supercooling by 1-4 K. If cooling rates exceed 0.5-1 K/day, small particles of NAT are produced. A major fraction of the available condensation nuclei is activated and removal of HNO3 by gravitational settling is slow. If cooling rates are less than 0.5-1 K/day, the number of aerosols that nucleate is reduced, leading to differential growth of large NAT particles. Observations of 5 micron radius particles in clouds at temperatures above the water frost point may reflect condensation of NAT on ice particles that fall through a column of air as it is cooled. Rapid condensation of HNO3 on ice particles is promoted by the high supersaturation attained during nucleation and maintained during subsequent cooling. This process provides a mechanism for irreversible removal of HNO3.
An exploratory study, dealing with the preparation of well-defined particulate metal deposits that can be used in model studies of catalytic reactions, was performed. Small metal particles of Fe and Pd were grown in situ in an electron microscope by vapor deposition onto different phase of electron transparent alumina substrates. The results show that characteristic properties of the deposits, such as particle density, size distribution, habit, and orientation, are strongly dependent on the cleanliness, phase, and crystallographic orientation of the alumina substrate; also, the deposition conditions can be chosen in such a way as to reproducibly manipulate the overall deposit structure.