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TPSAS-NF1676L-13393-DND

In the two plus decades since it became evident that polar stratospheric clouds (PSCs) play a major role in the springtime depletion of polar ozone, the detailed composition and morphology of PSCs has been an area of interest. Although our PSC knowledge base is substantial, there is still considerable uncertainty in specific key areas related to their composition and formation. Probably the least well understood of these is the nucleation process responsible for the formation of nitric acid trihydrate (NAT) particles and the circumstances under which NAT formation and growth leads to stratospheric denitrification. CALIOP (Cloud-Aerosol LIdar with Orthogonal Polarization) is an excellent instrument for observing PSCs and has already produced an extensive set of PSC observations with unprecedented spatial and temporal resolution covering five winters. These observations are providing new insight into the key remaining questions regarding PSC composition and formation mechanisms. In this paper, we examine the CALIOP PSC observations in combination with a microphysical model in attempt to better understand the underlying physical mechanisms for NAT nucleation. Of particular interest is the early phase of the 2009-2010 Arctic winter when CALIOP frequently observed extended regions of tenuous NAT clouds, clearly before ice was present in the polar vortex. This provides unprecedented large-scale evidence that ice particles are not the only nuclei on which NAT may form. Microphysical model calculations along backward trajectories from these CALIOP NAT cloud observations are used to investigate possible ice-independent, heterogeneous NAT nucleation mechanisms. These analyses will then be expanded to other winters to assess the overall significance of an ice-independent nucleation mechanism for NAT PSCs.

M C Pitts↗

NASA NTRS1991

Plume and wake dynamics, mixing, and chemistry behind an HSCT aircraft

The chemical evolution and mixing and vortical motion of a High Speed Civil Transport's engine exhausts must be analyzed in order to track the gas and its speciation as emissions are mixed to atmospheric scales. Attention is presently given to an analytic model of the wake dynamical processes which accounts for the roll-up of the trailing vorticity, its breakup due to the Crow instability, and the subsequent evolution and motion of the reconnected vorticity. The concentrated vorticity is noted to wrap up the buoyant exhaust and suppress its continued mixing and dilution. The species tracked encompass those which could be heterogeneously reactive on the surfaces of the condensed ice particles, and those capable of reacting with exhaust soot particle surfaces to form active contrail and/or cloud condensation nuclei.

Miake-Lye, R. C.↗

NASA NTRS1990

Microphysical fundamentals governing cirrus cloud growth: Modeling studies

For application to Global Climate Models, large scale numerical models of cirrus cloud formation and maintenance need to be refined to more reliably simulate the effects and feedbacks of high level clouds. A key aspect is how ice crystal growth is initiated in cirrus, which has started a cloud microphysical controversy between camps either believing that heterogeneous or homogeneous drop freezing is predominantly responsible for cold cirrus ice crystal nucleation. In view of convincing evidence for the existence of highly supercooled cloud droplets in the middle and upper troposphere, however, it is concluded that active ice nuclei are rather scarce at cirrus cloud altitudes, and so a new understanding of cirrus cloud formation is needed. This understanding is sought through an examination of cirrus cloud growth models.

Sassen, Kenneth↗

NASA NTRS1991

Water/rock interactions in experimentally simulated dirty snowball and dirty iceball cometary nuclei

In the dirty snowball model for cometary nuclei, comet-nucleus materials are regarded as mixtures of volatile ices and relatively non-volatile minerals or chemical compounds. Carbonaceous chondrite meteorites are regarded as useful analogs for the rocky component. To help elucidate the possible physical geochemistry of cometary nuclei, preliminary results are reported of calorimetric experiments with two-component systems involving carbonaceous chondrites and water ice. Based on collective knowledge of the physics of water ice, three general types of interactions can be expected between water and minerals at sub-freezing temperatures: (1) heterogeneous nucleation of ice by insoluble minerals; (2) adsorption of water vapor by hygroscopic phases; and (3) freezing- and melting-point depression of liquid water sustained by soluble minerals. The relative and absolute magnitude of all three effects are expected to vary with mineral composition.

Gooding, James L.↗

NASA NTRS1994

Microphysical modeling of cirrus. 2: Sensitivity studies

The one-dimensional cirrus model described in part 1 of this issue has been used to study the sensitivity of simulated cirrus microphysical and radiative properties to poorly known model parameters, poorly understood physical processes, and environmental conditions. Model parameters and physical processes investigated include nucleation rate, mode of nucleation (e.g., homogeneous freezing of aerosols and liquid droplets or heterogeneous deposition), ice crystal shape, and coagulation. These studies suggest that the leading sources of uncertainty in the model are the phase change (liquid-solid) energy barrier and the ice-water surface energy which dominate the homogeneous freezing nucleation rate and the coagulation sticking efficiency at low temperatures which controls the production of large ice crystals (radii greater than 100 mcirons). Environmental conditions considered in sensitivity tests were CN size distribution, vertical wind speed, and cloud height. We found that (unlike stratus clouds) variations in the total number of condensation nuclei (NC) have little effect on cirrus microphysical and radiative properties, since nucleation occurs only on the largest CN at the tail of the size distribution. The total number of ice crystals which nucleate has little or no relationship to the number of CN present and depends primarily on the temperature and the cooling rate. Stronger updrafts (more rapid cooling) generate higher ice number densities, ice water content, cloud optical depth, and net radiative forcing. Increasing the height of the clouds in the model leads to an increase in ice number density, a decrease in effective radius, and a decrease in ice water content. The most prominent effect of increasing cloud height was a rapid increase in the net cloud radiative forcing which can be attributed to the change in cloud temperature as well as change in cloud ice size distributions. It has long been recognized that changes in cloud height or cloud area have the greatest potential for causing feedbacks on climate change. Our results suggest that variations in vertical velocity or cloud microphysical changes associatd with cloud height changes may also be important.

Jensen, Eric J.↗

NASA NTRS1998

Soot and Sulfuric Acid from Aircraft: Is There Enough to Cause Detrimental Environmental E-kCTSs?

Aerosol from aircraft can affect the environment in three ways: First, soot aerosol has been implicated to cause Icing-tern ozone depletion at mid-latitudes in the lower stratosphere at a rate of approx. 5% per decade. This effect is in addition and unrelated to the polar ozone holes which are strongly influenced by heterogeneous chemistry on polar stratospheric clouds. Second, the most obvious effect of jet aircraft is the formation of visible contrails in the upper troposphere. The Salt Lake City region experienced an 8% increase in cirrus cloud cover over a 15-year period which covariates with an increase in regional commercial air traffic. If soot particles act as freezing nuclei to cause contrail formation heterogeneously, they would be linked to a secondary effect to cloud modification that very likely is climatologically important. Third, a buildup of soot aerosol could reduce the single scatter albedo of stratospheric aerosol from 0.993+0.004 to 0.98, a critical value that has been postulated to separate stratospheric cooling from warming. Thus arises an important question: Do aircraft emit sufficient amounts of soot to have detrimental effects and warrant emission controls? During the 1996 SUCCESS field campaign, we sampled aerosols in the exhaust wake of a Boeing 757 aircraft and determined emission indices for sulfuric acid (EI(sub H2SO4) = 9.0E-2 and 5.0E-1 g/kg (sub FUEL) for 75 and 675 ppm fuel-sulfur, respectively) and soot aerosol (2.2E-3 less than EI(sub SOOT) = l.lE-2 g/kg (sub FUEL)). The soot particle analysis accounted for their fractal nature, determined electron-microscopically, which enhanced the surface area by a factor of 26 and the volume 11-fold over equivalent-volume spheres. The corresponding fuel-sulfur to H2SO4 conversion efficiency was 10% (for 675 ppmm fuel-S) and 37% (for 75 ppmm fuel-S). Applying the H2SO4 emission index to the 1990 fuel use by the worlds commercial fleets of 1.3E11 kg, a conversion efficiency of 30% of 500 ppmm fuel-S would have led to an annual contribution to the atmospheric sulfur budget by aircraft of 2.E7 kg H2SO4. This is about one part in 1.E4 of anthropogenic sulfate from other sources. The soot emission index given above yielded a 1990 injection of soot aerosol by aircraft of 1.E6 kg. Thus, soot amounts to only five percent of the aerosol generated by aircraft. Its reactivity with ozone would have to be 20 times that of sulfuric acid particles to make it chemically significant. Nevertheless, the findings, of stratospheric soot loadings commensurate with aircraft fuel consumption, based on the emission index given above and the assumption of stratospheric residence times of the order of one year implicate aircraft as stratospheric polluters. A trend similar to soot of H2SO4 aerosol loading could not be deciphered, neither from in situ measurements nor SAGE II satellite extinction, against the "noise" due to volcanic eruptions. Observation of soot particles at 20 km altitude which, if emitted by aircraft were generated at 10-12 km altitude, suggests a displacement of those particles against gravity. Because eddy mixing is virtually absent in the lower stratosphere and isentropic mixing explains lofting to only about 15 km, radiometric forces acting on morphologically and chemically asymmetric soot particles must be considered a possibility. The consequence could be an extended residence time of soot against that of sulfuric acid aerosol that would lower the single scatter albedo with time.

Pueschel, R. F.↗

NASA NTRS1991

Stratospheric soot - Cloud forming properties and transport processes

Soot enters the stratosphere either from the troposphere in deep thunderstorm convection, predominantly in the tropics, from midlatitude forest fires, and directly from aircraft flying above the tropopause. Particles emitted from jet aircraft are relatively ineffective as cloud droplet condensation nuclei (less than 1 percent) compared with those from forest fires (above 50 percent). Chemical and other modification during aging of the particles may influence these results in some circumstances; cloud nucleating properties can be used as a soot tracer. Such aerosols, as they grow to haze drops and ilute in increasing humidity, may form ice particles in the cold polar stratosphere or in tropical cumuli anvils at 18 to 20 km altitude at temperatures as low as -90 C. Ice may also form as particles are removed by descent through troposphere folds and enter midlatitude cirrus at levels below -40 C. In the stratosphere, ice particles may provide surfaces that catalyze heterogeneous chemical reactions; in the upper troposphere, the optical depths of cirrus clouds may be significantly increased.

Hallett, John↗

NASA NTRS2012

Sensitivity of Cirrus and Mixed-phase Clouds to the Ice Nuclei Spectra in McRAS-AC: Single Column Model Simulations

The salient features of mixed-phase and ice clouds in a GCM cloud scheme are examined using the ice formation parameterizations of Liu and Penner (LP) and Barahona and Nenes (BN). The performance of LP and BN ice nucleation parameterizations were assessed in the GEOS-5 AGCM using the McRAS-AC cloud microphysics framework in single column mode. Four dimensional assimilated data from the intensive observation period of ARM TWP-ICE campaign was used to drive the fluxes and lateral forcing. Simulation experiments where established to test the impact of each parameterization in the resulting cloud fields. Three commonly used IN spectra were utilized in the BN parameterization to described the availability of IN for heterogeneous ice nucleation. The results show large similarities in the cirrus cloud regime between all the schemes tested, in which ice crystal concentrations were within a factor of 10 regardless of the parameterization used. In mixed-phase clouds there are some persistent differences in cloud particle number concentration and size, as well as in cloud fraction, ice water mixing ratio, and ice water path. Contact freezing in the simulated mixed-phase clouds contributed to transfer liquid to ice efficiently, so that on average, the clouds were fully glaciated at T approximately 260K, irrespective of the ice nucleation parameterization used. Comparison of simulated ice water path to available satellite derived observations were also performed, finding that all the schemes tested with the BN parameterization predicted 20 average values of IWP within plus or minus 15% of the observations.

Betancourt, R. Morales↗

NASA NTRS1999

Comets after Hyakutake and Hale-Bopp

Being icy, cometary nuclei are the most easily modified bodies in the solar system - even modest heating is sufficient to induce significant weight loss. This sublimative loss and longterm storage far from the sun protect the nucleus against internal warming and ensure that cometary nuclei today contain the least processed material remaining from the early nebula - or perhaps from the natal cloud. The chemical compositions of ices, low temperature-refractory organics, and refractory minerals (and their physical states) provide sensitive probes of the origin and history of this material. The fortunate appearance of Hyakutake and Hale-Bopp has provided a wealth of information on these Oort cloud comets, obtained with a wide range of astronomical approaches. I will review certain key results for these comets, such as chemical abundances, isotopic abundance ratios, nuclear spin statistics, and nuclear vs extended production of "parent volatiles", and will illustrate how these test the origins of cometary material. A comparison with 1P/Halley--a third comet from the giant planet nebular region--will be discussed in the context of heterogeneity among these bodies.

Mumma, Michael J.↗

NASA NTRS2003

Theoretical Studies of the Extra-terrestrial Chemistry of Biogenic Elements and Compounds

Results are presented on the following:(A) Ab initio quantum chemical studies of reactions in astrophysical ices.Theoretical electronic structure calculations were used to investigate reactions between formaldehyde (H2CO) and both hydrogen cyanide (HCN) and isocyanide (HNC) in search of other favorable reactions such as ammonia-formaldehyde addition, which was found in a recent theoretical study to be strongly enhanced when it occurs within cold ices.The present study examines further reactions between this product and H2CO in ices.(B) Heterogeneous hydrogenation of CO and H2CO on icy grain mantles.Formaldehyde (H2CO) and methanol (CH30H) are thought to be produced in the interstellar medium by the successive hydrogenation of carbon monoxide (CO) on grain surfaces. In the gas phase, the steps in which H adds to CO and H2CO possess modest barriers and are too inefficient to account for the observed abundances. Recent laboratory work has confirmed that formaldehyde and methanol are formed when H atoms are deposited on CO ice at 12 K. The present study employed ab initio quantum chemical calculations to investigate the impact of water ice on the sequential hydrogenation of CO.(C) Ice-bound condensed-phase reactions involving formic acid (HCOOH), methylenimine (CH2NH), hydrogen cyanide (HCN), hydrogen isocyanide (HNC), and ammonia ( 3) were investigated in order to characterize possible pathways to larger organic species that are efficient at the cold temperatures prevalent in cometary nuclei and the interstellar medium. (D) Pathways to glycine and other amino acids in ultraviolet-irradiated ices determined via quantum chemical modeling.(E) Photoionization in ultraviolet processing of astrophysical ice analogs at cryogenic temperatures.

Woon, David E.↗