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68 records · Page 4

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↗

Role of Gravity Waves in Determining Cirrus Cloud Properties

Cirrus clouds are important in the Earth's radiation budget. They typically exhibit variable physical properties within a given cloud system and from system to system. Ambient vertical motion is a key factor in determining the cloud properties in most cases. The obvious exception is convectively generated cirrus (anvils), but even in this case, the subsequent cloud evolution is strongly influenced by the ambient vertical motion field. It is well know that gravity waves are ubiquitous in the atmosphere and occur over a wide range of scales and amplitudes. Moreover, researchers have found that inclusion of statistical account of gravity wave effects can markedly improve the realism of simulations of persisting large-scale cirrus cloud features. Here, we use a 1 -dimensional (z) cirrus cloud model, to systematically examine the effects of gravity waves on cirrus cloud properties. The model includes a detailed representation of cloud microphysical processes (bin microphysics and aerosols) and is run at relatively fine vertical resolution so as to adequately resolve nucleation events, and over an extended time span so as to incorporate the passage of multiple gravity waves. The prescribed gravity waves "propagate" at 15 m s (sup -1), with wavelengths from 5 to 100 km, amplitudes range up to 1 m s (sup -1)'. Despite the fact that the net gravity wave vertical motion forcing is zero, it will be shown that the bulk cloud properties, e.g., vertically-integrated ice water path, can differ quite significantly from simulations without gravity waves and that the effects do depend on the wave characteristics. We conclude that account of gravity wave effects is important if large-scale models are to generate realistic cirrus cloud property climatology (statistics).

OCStarr, David↗

Advancements in the Representation of Cloud-Aerosol Microphysics in the GEOS-5 AGCM

Despite numerous challenges, the physical parameterization of cloud-aerosol interactions in atmospheric GCMs has become a top priority for advancement because of our need to simulate and understand past, current, and future indirect effects of aerosols on clouds. The challenges stem from the involvement of wide range of cloud-scale dynamics and aerosol activation physical processes. Cloud dynamics modulate cloud areal extent and condensate, while aerosol activation depends on aerosol mass load, size distribution, internal mixing state, and nucleating properties, and ultimately determines cloud optical properties via particle sizes. Both macro- and micro-scale processes are obviously important for cloud-radiation interactions. We will present the main features of cloud microphysical properties in the GEOS- 5 Atmospheric GCM (AGCM) as simulated by the McRAS-AC (Microphysics of Clouds with Relaxed Arakawa-Schubert and Aerosol-Cloud interaction) scheme. McRAS-AC uses Fountoukis and Nenes (2005) aerosol activation for liquid clouds, and has an option for either Liu and Penner (2005) or Barahona and Nenes (2008, 2009) aerosol activation for ice clouds. Aerosol loading (on-line or climatological) comes from GOCART, with an assumed log-normal size distribution. Other features of McRAS-AC are level-by-level cloud-scale thermodynamics, and Seifert-Beheng (2001)-type precipitation microphysics, particularly from moist convection. Results from Single-Column Model simulations will be shown to demonstrate how cloud radiative properties, lifetimes, and precipitation are influenced by different parameterization assumptions. Corresponding fields from year-long simulations of the full AGCM will also be presented with geographical distributions of cloud effective particle sizes compared to satellite retrievals. While the primary emphasis will be on current climate, simulation results with perturbed aerosol loadings will also be shown to expose the radiative sensitivity of the microphysical parameterization.

Lee, D.↗

Influence of convection on free growth of dendrite crystals from solution

The free growth of dendrites in a uniformly supercooled solution was examined using cine photography with a Schlieren optical system. Crystals were grown in the bulk of the solution from a centrally located capillary tube, nucleated at the interface with a liquid nitrogen cooled wire. Crystals propagated along the tube, the slower growing orientations eliminated, and emerged at the tip, usually growing parallel to the tube direction. For both sodium sulfate decahydrate from its solution and ice from sodium chloride solution, growth rate and fineness of dendrites increased with supercooling. In sodium sulfate, upward convection of the less dense depleted solution occurs; downward convection was observed for the rejected, more concentrated sodium chloride solution. In both cases, there was a spatial and temporal delay in the release of the convective plume from the moving dendrite tip. The role of this convection on the growth characteristics and the production of secondary crystals is examined. A proposed low-g experiment to examine differences in growth rate, crystal texture, and secondary nucleation in a reduced convective regime where molecular diffusion is the dominant transfer process is discussed.

Hallett, J.↗

Permafrost and Subsurface Ice in the Solar System

The properties and behavior of planetary permafrost are discussed with reference to the ability of such surfaces to sustain loads characteristics of spacecraft landing and planetary bases. In most occurrences, water ice is in close proximity to, or in contact with, finely divided silicate mineral matter. When ice contacts silicate mineral surfaces, a liquid-like, transition zone is created. Its thickness ranges from several hundred Angstron units at temperatures near 0 degrees C to about three Angstrom units at -150 degrees C. When soluble substances are present, the resulting brine enlarges the interfacial zone. When clays are involved, although the interfacial zone may be small, its extent is large. The unfrozen, interfacial water may amount to 100% or more weight at a temperature of -5 degrees C. The presence of this interfacial unfrozen water acts to confer plasticity to permafrost, enabling it to exhibit creep at all imposed levels of stress. Nucleation processes and load-bearing capacity are examined.

Anderson, D. M.↗

Modeling Macro- and Micro-Scale Turbulent Mixing and Chemistry in Engine Exhaust Plumes

Simulation of turbulent mixing and chemical processes in the near-field plume and plume-vortex regimes has been successfully carried out recently using a reduced gas phase kinetics mechanism which substantially decreased the computational cost. A detailed mechanism including gas phase HOx, NOx, and SOx chemistry between the aircraft exhaust and the ambient air in near-field aircraft plumes is compiled. A reduced mechanism capturing the major chemical pathways is developed. Predictions by the reduced mechanism are found to be in good agreement with those by the detailed mechanism. With the reduced chemistry, the computer CPU time is saved by a factor of more than 3.5 for the near-field plume modeling. Distributions of major chemical species are obtained and analyzed. The computed sensitivities of major species with respect to reaction step are deduced for identification of the dominant gas phase kinetic reaction pathways in the jet plume. Both the near field plume and the plume-vortex regimes were investigated using advanced mixing models. In the near field, a stand-alone mixing model was used to investigate the impact of turbulent mixing on the micro- and macro-scale mixing processes using a reduced reaction kinetics model. The plume-vortex regime was simulated using a large-eddy simulation model. Vortex plume behind Boeing 737 and 747 aircraft was simulated along with relevant kinetics. Many features of the computed flow field show reasonable agreement with data. The entrainment of the engine plumes into the wing tip vortices and also the partial detrainment of the plume were numerically captured. The impact of fluid mechanics on the chemical processes was also studied. Results show that there are significant differences between spatial and temporal simulations especially in the predicted SO3 concentrations. This has important implications for the prediction of sulfuric acid aerosols in the wake and may partly explain the discrepancy between past numerical studies (that employed parabolic or temporal approximations) and the measured data. Finally to address the major uncertainty in the near-field plume modeling related to the plume processing of sulfur compounds and advanced model was developed to evaluate its impact on the chemical processes in the near wake. A comprehensive aerosol model is developed and it is coupled with chemical kinetics and the axisymmetric turbulent jet flow models. The integrated model is used to simulate microphysical processes in the near-field jet plume, including sulfuric acid and water binary homogeneous nucleation, coagulation, non-equilibrium heteromolecular condensation, and sulfur-induced soot activation. The formation and evolution of aerosols are computed and analyzed. The computed results show that a large number of ultra-fine (0.3--0.6 nm in radius) volatile HSO4 - HO embryos are generated in the near-field plume. These embryos further grow in size by self coagulation and condensation. Soot particles can be activated by both heterogeneous nucleation and scavenging of H2SO4-H2O aerosols. These activated soot particles can serve as water condensation nuclei for contrail formation. Conditions under which ice contrails can form behind aircrafts are studied. The sensitivities of the threshold temperature for contrail formation with respect to aircraft propulsion efficiency, relative humidity, and ambient pressure are evaluated. The computed aerosol properties for different extent of fuel sulfur conversion to S(VI) (SO3 and H2SO4) in engine are examined and the results are found to be sensitive to this conversion fraction.

Menon, Suresh↗

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↗

Metamorphism of Cosmic Dust: Processing from Circumstellar Outflows to the Cometary Regolith

Nucleation is a non-equilibrium process: the products of this process are seldom the most thermodynamically stable condensates but are instead those which form fastest. It should therefore not be surprising that grains formed in a circumstellar outflow will undergo some degree of metamorphism if they are annealed or are exposed to a chemically active reagent. Metamorphism of refractory particles continues in the interstellar medium (ISM) where the driving forces are sputtering by cosmic ray particles, annealing by high energy photons and grain destruction in supernova generated shocks. Studies of the depletion of the elements from the gas phase of the interstellar medium tell us that if grain destruction occurs with high efficiency in the ISM, then there must be some mechanism by which grains can be formed in the ISM. Various workers have shown that refractory mantles could form on refractory cores by radiation processing of organic ices. A similar process may operate to produce refractory inorganic mantles on grain cores which survived the supernova shocks. Most grains in a cloud which collapses to form a star will be destroyed; many of the surviving grains will be severely processed. Grains in the outermost regions of the nebula may survive relatively unchanged by thermal processing or hydration. It is these grains which we hope to find in comets. However, only those grains encased in ice at low temperature can be considered pristine since a considerable degree of hydrous alteration might occur in a cometary regolith if the comet enters the inner solar system. Some discussion of the physical, chemical and isotopic properties of a refractory grain at each stage of its life cycle will be attempted based on the limited laboratory data available to date. Suggestions will be made concerning the types of experimental data which are needed in order to better understand the processing history of cosmic dust.

Nuth, Joseph A., III↗

A42F-03: Small-Scale Variability in Tropical Tropopause Layer Humidity

Recent advances in statistical parameterizations of cirrus cloud processes for use in global models are highlighting the need for information about small-scale fluctuations in upper tropospheric humidity and the physical processes that control the humidity variability. To address these issues, we have analyzed high-resolution airborne water vapor measurements obtained in the Airborne Tropical TRopopause EXperiment (ATTREX) over the tropical Pacific between 14 and 20 km. Using accurate and precise 1-Hz water vapor measurements along approximately-level aircraft flight legs, we calculate structure functions spanning horizontal scales ranging from about 0.2 to 50 km, and we compare the water vapor variability in the lower (about 14 km) and upper (16-19 km) Tropical Tropopause Layer (TTL). We also compare the magnitudes and scales of variability inside TTL cirrus versus in clear-sky regions. The measurements show that in the upper TTL, water vapor concentration variance is stronger inside cirrus than in clear-sky regions. Using simulations of TTL cirrus formation, we show that small variability in clear-sky humidity is amplified by the strong sensitivity of ice nucleation rate to supersaturation, which results in highly-structured clouds that subsequently drive variability in the water vapor field. In the lower TTL, humidity variability is correlated with recent detrainment from deep convection. The structure functions indicate approximately power-law scaling with spectral slopes ranging from about minus 5 divided by 3, to minus 2.

water vapor↗

Studies of Ice Nucleating Aerosol Particles in Arctic Cloud Systems

The focus of this research is to improve the understanding of ice nucleating aerosol particles (IN) and the role they play in ice formation in Arctic clouds. IN are important for global climate issues in a variety of ways. The primary effect is their role in determining the phase (liquid or solid) of cloud particles. The microscale impact is on cloud particle size, growth rate, shape, fall speed, concentration, radiative properties, and scavenging of gases and aerosols. On a larger scale, ice formation affects the development of precipitation (rate, amount, type, and distribution), latent heat release (rate and altitude), ambient humidity, the persistence of clouds, and cloud albedo. The overall goals of our FIRE 3 research are to characterize the concentrations and variability of Arctic IN during the winter-spring transition, to compare IN measurements with ice concentrations in Arctic clouds, and to examine selected IN samples for particle morphology and chemical there are distinguishable chemical signatures. The results can be combined with other measurements of aerosols, gaseous species, and cloud characteristics in order to understand the processes that determine the phase and concentration of cloud particles.

Rogers, David C.↗

Highly Supercooled Riming and Unusual Triple-Frequency Radar Signatures Over McMurdo Station, Antarctica

Riming of ice crystals by supercooled water droplets is an efficient ice growth process, but its basic properties are still poorly known. While it has been shown to contribute significantly to surface precipitation at mid-latitudes, little is known about its occurrence at high latitudes. In Antarctica, two competing effects can influence the occurrence of riming: (i) the scarcity of supercooled liquid water clouds due to the extremely low tropospheric temperatures and (ii) the low aerosol concentration, which may lead to the formation of fewer and larger supercooled drops potentially resulting in an enhanced riming efficiency. In this work, by exploiting the deployment of an unprecedented number of multiwavelength remote sensing systems (including triple-frequency radar measurements) in West Antarctica, during the Atmospheric Radiation Measurements West Antarctic Radiation Experiment (AWARE) field campaign, we evaluate the riming incidence at McMurdo Station and find that riming occurs at much lower temperatures when compared to previous results in the mid-latitudes. This suggests the possible occurrence of a common atmospheric state over Antarctica that includes a rather stable atmosphere inhibiting turbulent mixing, and a high riming efficiency driven by large cloud droplets. We then focus on a peculiar case study featuring a persistent layer with a particularly pronounced riming signature in triple-frequency radar data but only a relatively modest amount of supercooled liquid water. In-depth analysis of the radar observations suggests that such signatures can only be explained by the combined effects of moderately rimed aggregates or similarly shaped florid polycrystals and a narrow particle size distribution (PSD). Simulations of this case study performed with a one-dimensional bin model indicate that similar triple-frequency radar observations can be reproduced when narrow PSDs are simulated. Such narrow PSDs can in turn be explained by two key factors: (i) the presence of a shallow homogeneous droplet or humidified aerosol freezing layer aloft seeding an underlying supercooled liquid layer, and (ii) the absence of turbulent mixing throughout a stable polar atmosphere that sustains narrow PSDs, as hydrometeors grow from the nucleation region aloft to ice particles of several millimeters in size, by vapor deposition and then riming.

Riming↗

Formation of a Tropopause Cirrus Layer Observed over Florida during CRYSTAL-FACE

On July 13, 2002 a widespread, subvisible tropopause cirrus layer occurred over the Florida region. This cloud was observed in great detail with the NASA Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) instrumentation, including in situ measurements with the WB-57 aircraft. In this paper, we use the 13 July cloud as a case study to evaluate the physical processes controlling the formation and evolution of tropopause cirrus layers. Microphysics measurements indicate that ice crystal diameters in the cloud layer ranged from about 7 to 50 microns, and the peak number mode was about 10-25 microns. In situ water vapor and temperature measurements in the cloud indicated supersaturation with respect to ice throughout, with ice saturation ratios as large as 1.8. Even when the ice surface area density was as high as about 500 sq microns/cu cm, ice supersaturations of 20-30% were observed. Trajectory analysis shows that the air sampled near the tropopause on this day generally came from the north and cooled considerably during the previous few days. Examination of infrared satellite imagery along air parcel back trajectories from the WB-57 flight track indicates that the tropopause cloud layer formation was, in general, not simply left over ice from recently generated anvil cirrus. Simulations of cloud formation using time-height curtains of temperature along the trajectory paths show that the cloud could have formed in situ near the tropopause as the air was advected into the south Florida region and cooled to unusually low temperatures. If we assume a high threshold for ice nucleation via homogeneous freezing of aqueous sulfate aerosols, the model reproduces the observed cloud structure, ice crystal size distributions, and ice supersaturation statistics. Inclusion of observed gravity wave temperature perturbations in the simulations is essential to reproduce the observed cloud properties. Without waves, crystal number densities are too low, crystal sizes are too large, and the crystals fall out too fast, leaving very little cloud persisting at the end of the simulations. In the cloud simulations, coincidence of high supersaturations and high surface areas can be produced by either recent nucleation or sedimentation of crystals into supersaturated layers. The agreement between model results and observed supersaturations is improved somewhat if we assume that the steady state relative humidity within cirrus at T<200 K is enhanced by about 30%. The WB-57 measurements and the model results suggest that the cloud layer irreversibly dehydrated air near the tropopause.

Jensen, Eric↗

Development of Two-Moment Cloud Microphysics for Liquid and Ice Within the NASA Goddard Earth Observing System Model (GEOS-5)

This work presents the development of a two-moment cloud microphysics scheme within the version 5 of the NASA Goddard Earth Observing System (GEOS-5). The scheme includes the implementation of a comprehensive stratiform microphysics module, a new cloud coverage scheme that allows ice supersaturation and a new microphysics module embedded within the moist convection parameterization of GEOS-5. Comprehensive physically-based descriptions of ice nucleation, including homogeneous and heterogeneous freezing, and liquid droplet activation are implemented to describe the formation of cloud particles in stratiform clouds and convective cumulus. The effect of preexisting ice crystals on the formation of cirrus clouds is also accounted for. A new parameterization of the subgrid scale vertical velocity distribution accounting for turbulence and gravity wave motion is developed. The implementation of the new microphysics significantly improves the representation of liquid water and ice in GEOS-5. Evaluation of the model shows agreement of the simulated droplet and ice crystal effective and volumetric radius with satellite retrievals and in situ observations. The simulated global distribution of supersaturation is also in agreement with observations. It was found that when using the new microphysics the fraction of condensate that remains as liquid follows a sigmoidal increase with temperature which differs from the linear increase assumed in most models and is in better agreement with available observations. The performance of the new microphysics in reproducing the observed total cloud fraction, longwave and shortwave cloud forcing, and total precipitation is similar to the operational version of GEOS-5 and in agreement with satellite retrievals. However the new microphysics tends to underestimate the coverage of persistent low level stratocumulus. Sensitivity studies showed that the simulated cloud properties are robust to moderate variation in cloud microphysical parameters. However significant sensitivity in ice cloud properties was found to variation in the dispersion of the ice crystal size distribution and the critical size for ice autoconversion. The implementation of the new microphysics leads to a more realistic representation of cloud processes in GEOS-5 and allows the linkage of cloud properties to aerosol emissions.

Aerosol-Cloud Interactions↗

Stratospheric Heterogeneous Chemistry and Microphysics: Model Development, Validation and Applications

The objectives of this project are to: define the chemical and physical processes leading to stratospheric ozone change that involve polar stratospheric clouds (PSCS) and the reactions occurring on the surfaces of PSC particles; study the formation processes, and the physical and chemical properties of PSCS, that are relevant to atmospheric chemistry and to the interpretation of field measurements taken during polar stratosphere missions; develop quantitative models describing PSC microphysics and heterogeneous chemical processes; assimilate laboratory and field data into these models; and calculate the extent of chemical processing on PSCs and the impact of specific microphysical processes on polar composition and ozone depletion. During the course of the project, a new coupled microphysics/physical-chemistry/ photochemistry model for stratospheric sulfate aerosols and nitric acid and ice PSCs was developed and applied to analyze data collected during NASA's Arctic Airborne Stratospheric Expedition-II (AASE-II) and other missions. In this model, detailed treatments of multicomponent sulfate aerosol physical chemistry, sulfate aerosol microphysics, polar stratospheric cloud microphysics, PSC ice surface chemistry, as well as homogeneous gas-phase chemistry were included for the first time. In recent studies focusing on AASE measurements, the PSC model was used to analyze specific measurements from an aircraft deployment of an aerosol impactor, FSSP, and NO(y) detector. The calculated results are in excellent agreement with observations for particle volumes as well as NO(y) concentrations, thus confirming the importance of supercooled sulfate/nitrate droplets in PSC formation. The same model has been applied to perform a statistical study of PSC properties in the Northern Hemisphere using several hundred high-latitude air parcel trajectories obtained from Goddard. The rates of ozone depletion along trajectories with different meteorological histories are presently being systematically evaluated to identify the principal relationships between ozone loss and aerosol state. Under this project, we formulated a detailed quantitative model that predicts the multicomponent composition of sulfate aerosols under stratospheric conditions, including sulfuric, nitric, hydrochloric, hydrofluoric and hydrobromic acids. This work defined for the first time the behavior of liquid ternary-system type-1b PSCS. The model also allows the compositions and reactivities of sulfate aerosols to be calculated over the entire range of environmental conditions encountered in the stratosphere (and has been incorporated into a trajectory/microphysics model-see above). Important conclusions that derived from this work over the last few years include the following: the HNO3 content of liquid-state aerosols dominate PSCs below about 195 K; the freezing of nitric acid ice from sulfate aerosol solutions is likely to occur within a few degrees K of the water vapor frost point; the uptake and reactions of HCl in liquid aerosols is a critical component of PSC heterogeneous chemistry. In a related application of this work, the inefficiency of chlorine injection into the stratosphere during major volcanic eruptions was explained on the basis of nucleation of sulfuric acid aerosols in rising volcanic plumes leading to the formation of supercooled water droplets on these aerosols, which efficiently scavenges HCl via precipitation.

Turco, Richard P.↗