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NASA NTRS2016

Calipso Observations of the Dependence of Homo- and Heterogeneous Ice Nucleation in Cirrus Clouds on Latitude, Season and Surface Condition

There are two fundamental mechanisms through which cirrus clouds form; homo- and heterogeneous ice nucleation (henceforth hom and het). The relative contribution of each mechanism to ice crystal production often determines the microphysical and radiative properties of a cirrus cloud. A new satellite remote sensing method is described in this study to estimate cirrus cloud ice particle number concentration and the relative contribution of hom and het to cirrus cloud formation as a function of altitude, latitude, season and surface type (e.g. land vs. ocean). This method uses co-located observations from the Infrared Imaging Radiometer (IIR) and from the CALIOP (Cloud and Aerosol Lidar with Orthogonal Polarization) lidar aboard the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) polar orbiting satellite, employing IIR channels at 10.6 μm and 12.05 μm. The method is applied here to single-layered clouds of visible optical depth between about 0.3 and 3. Two years of Version 3 data have been analyzed for the years 2008 and 2013, with each season characterized in terms of 532 nm cirrus cloud centroid altitude and temperature, the cirrus cloud ice particle number concentration, effective diameter, layer-average ice water content and visible optical depth. Using a conservative criterion for hom cirrus, on average, the sampled cirrus clouds formed through hom occur about 43% of the time in the Arctic and 50% of the time in the Antarctic, and during winter at mid-latitudes in the Northern Hemisphere, hom cirrus occur 37% of the time. Elsewhere (and during other seasons in the Northern Hemisphere mid-latitudes), this hom cirrus fraction is lower. Processes that could potentially explain these observations are discussed, as well as the potential relevancy of these results to ice nucleation studies, climate modeling and jet-stream dynamics.

Mitchell, David L.↗

NASA NTRS1996

Laboratory studies of stratospheric aerosol chemistry

In this report we summarize the results of the two sets of projects funded by the NASA grant NAG2-632, namely investigations of various thermodynamic and nucleation properties of the aqueous acid system which makes up stratospheric aerosols, and measurements of reaction probabilities directly on ice aerosols with sizes corresponding to those of polar stratospheric cloud particles. The results of these investigations are of importance for the assessment of the potential stratospheric effects of future fleets of supersonic aircraft. In particular, the results permit to better estimate the effects of increased amounts of water vapor and nitric acid (which forms from nitrogen oxides) on polar stratospheric clouds and on the chemistry induced by these clouds.

Molina, Mario J.↗

NASA NTRS2002

Ice Cloud Formation and Dehydration in the Tropical Tropopause Layer

Stratospheric water vapor is important not only for its greenhouse forcing, but also because it plays a significant role in stratospheric chemistry. several recent studies have focused on the potential for dehydration due to ice cloud formation in air rising slowly through the tropical tropopause layer. Holton and Gettelman showed that temperature variations associated with horizontal transport of air in the tropopause layer can drive ice cloud formation and dehydration, and Gettelman et al. recently examined the cloud formation and dehydration along kinematic trajectories using simple assumptions about the cloud properties. In this study, we use a Lagrangian, one-dimensional cloud model to further investigate cloud formation and dehydration as air is transported horizontally and vertically through the tropical tropopause layer. Time-height curtains of temperature are extracted from meteorological analyses. The model tracks the growth and sedimentation of individual cloud particles. The regional distribution of clouds simulated in the model is comparable to the subvisible cirrus distribution indicated by SAGE II. The simulated cloud properties depend strongly on the assumed ice supersaturation threshold for ice nucleation. with effective nuclei present (low supersaturation threshold), ice number densities are high (0.1--10 cm(circumflex)-3), and ice crystals do not grow large enough to fall very far, resulting in limited dehydration. With higher supersaturation thresholds, ice number densities are much lower (less than 0.01 cm(circumflex)-3), and ice crystals grow large enough to fall substantially; however, supersaturated air often crosses the tropopause without cloud formation. The clouds typically do not dehydrate the air along trajectories down to the temperature minimum saturation mixing ratio. Rather the water vapor mixing ratio crossing the tropopause along trajectories is typically 10-50% larger than the saturation mixing ratio.

Jensen, Eric↗

NASA NTRS1991

Homogeneous freezing nucleation of stratospheric solution droplets

The classical theory of homogeneous nucleation was used to calculate the freezing rate of sulfuric acid solution aerosols under stratospheric conditions. The freezing of stratospheric aerosols would be important for the nucleation of nitric acid trihydrate particles in the Arctic and Antarctic stratospheres. In addition, the rate of heterogeneous chemical reactions on stratospheric aerosols may be very sensitive to their state. The calculations indicate that homogeneous freezing nucleation of pure water ice in the stratospheric solution droplets would occur at temperatures below about 192 K. However, the physical properties of H2SO4 solution at such low temperatures are not well known, and it is possible that sulfuric acid aerosols will freeze out at temperatures ranging from about 180 to 195 K. It is also shown that the temperature at which the aerosols freeze is nearly independent of their size.

Jensen, Eric J.↗

NASA NTRS1982

Noctilucent clouds - Simulation studies of their genesis, properties and global influences

A numerical model is presented for testing theories of the physical mechanisms of noctiluminescent clouds. The time-dependent, one-dimensional model describes the formation, evolution, and properties of the clouds as interactive ice crystals, meteoric dust, water vapor, and ionized air. Mesopause temperatures below 140 K are found to be necessary for the formation of the clouds, conditions existing only at high latitudes in the summer. No predominant nucleation particle could be identified for the formation of the clouds, although a time period of up to a day was determined as necessary for materialization, which lasts several days. Several atmospheric and environmental conditions were characterized which enhance the appearance of the noctiluminescent clouds. One conclusion reached is that the numerous launches necessary to build a solar power satellite system would not significantly exacerbate noctiluminescent cloud formation.

Turco, R. P.↗

NASA NTRS2002

Ice Cloud Formation and Dehydration in the Tropical Tropopause Layer

Stratospheric water vapor is important not only for its greenhouse forcing, but also because it plays a significant role in stratospheric chemistry. Several recent studies have focused on the potential for dehydration due to ice cloud formation in air rising slowly through the tropical tropopause layer (TTL). Holton and Gettelman showed that temperature variations associated with horizontal transport of air in the TTL can drive ice cloud formation and dehydration, and Gettelman et al. recently examined the cloud formation and dehydration along kinematic trajectories using simple assumptions about the cloud properties. In this study, a Lagrangian, one-dimensional cloud model has been used to further investigate cloud formation and dehydration as air is transported horizontally and vertically through the TTL. Time-height curtains of temperature are extracted from meteorological analyses. The model tracks the growth, advection, and sedimentation of individual cloud particles. The regional distribution of clouds simulated in the model is comparable to the subvisible cirrus distribution indicated by SAGE II. The simulated cloud properties and cloud frequencies depend strongly on the assumed supersaturation threshold for ice nucleation. The clouds typically do not dehydrate the air along trajectories down to the temperature minimum saturation mixing ratio. Rather the water vapor mixing ratio crossing the tropopause along trajectories is 10-50% larger than the saturation mixing ratio. I will also discuss the impacts of Kelvin waves and gravity waves on cloud properties and dehydration efficiency. These simulations can be used to determine whether observed lower stratospheric water vapor mixing ratios can be explained by dehydration associated with in situ TTL cloud formation alone.

Jensen, Eric↗

NASA NTRS2015

How the Assumed Size Distribution of Dust Minerals Affects the Predicted Ice Forming Nuclei

The formation of ice in clouds depends on the availability of ice forming nuclei (IFN). Dust aerosol particles are considered the most important source of IFN at a global scale. Recent laboratory studies have demonstrated that the mineral feldspar provides the most efficient dust IFN for immersion freezing and together with kaolinite for deposition ice nucleation, and that the phyllosilicates illite and montmorillonite (a member of the smectite group) are of secondary importance.A few studies have applied global models that simulate mineral specific dust to predict the number and geographical distribution of IFN. These studies have been based on the simple assumption that the mineral composition of soil as provided in data sets from the literature translates directly into the mineral composition of the dust aerosols. However, these tables are based on measurements of wet-sieved soil where dust aggregates are destroyed to a large degree. In consequence, the size distribution of dust is shifted to smaller sizes, and phyllosilicates like illite, kaolinite, and smectite are only found in the size range 2 m. In contrast, in measurements of the mineral composition of dust aerosols, the largest mass fraction of these phyllosilicates is found in the size range 2 m as part of dust aggregates. Conversely, the mass fraction of feldspar is smaller in this size range, varying with the geographical location. This may have a significant effect on the predicted IFN number and its geographical distribution.An improved mineral specific dust aerosol module has been recently implemented in the NASA GISS Earth System ModelE2. The dust module takes into consideration the disaggregated state of wet-sieved soil, on which the tables of soil mineral fractions are based. To simulate the atmospheric cycle of the minerals, the mass size distribution of each mineral in aggregates that are emitted from undispersed parent soil is reconstructed. In the current study, we test the null-hypothesis that simulating the presence of a large mass fraction of phyllosilicates in dust aerosols in the size range 2 m, in comparison to a simple model assumption where this is neglected, does not yield a significant effect on the magnitude and geographical distribution of the predicted IFN number. Results from sensitivity experiments are presented as well.

Dust↗

DOE OSTI2023

Orographic Cirrus and Its Radiative Forcing in NCAR CAM6

Cirrus clouds play an important role in the Earth's radiative energy budget, thereby affecting the climate state and climate change. Orographic gravity wave (OGW)-induced sub-grid scale vertical velocity (i.e., cooling rate) is not resolved by large-scale models and its impact on ice formation in cirrus clouds is not well quantified. In this study, one sub-grid scale OGW scheme (e.g., McFarlane) is used in the Community Atmosphere Model version 6 (CAM6) to generate vertical velocity variance (σw) for cirrus formation. Results from the default model and simulations with the OGW-induced σw are evaluated against the DOE ARM Small Particles in Cirrus (SPARTICUS) campaign observations. The OGW based on the McFarlane scheme increases the sub-grid scale σw over mountains compared to the default model and improves the model agreement with the SPARTICUS observations. Larger σ w due to OGWs can trigger more frequent homogeneous nucleation in orographic cirrus and generates a higher number concentration of ice crystals observed during the SPARTICUS campaign. Moreover, our evaluation of the model simulations against satellite observations indicates that the McFarlane scheme generates high in-cloud ice number concentrations (>200 L -1 ) in the upper troposphere over mountains and high plateaus at mid- and high-latitudes of the winter hemisphere as shown in the observations. More ice crystals with smaller sizes absorb more infrared radiation (+0.523 ± 0.125 W m -2 ). The net radiative cloud forcing change at the top of the atmosphere is +0.330 W m -2 due to the orographic cirrus.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2009

Cloud Imagers Offer New Details on Earth's Health

A stunning red sunset or purple sunrise is an aesthetic treat with a scientific explanation: The colors are a direct result of the absorption or reflectance of solar radiation by atmospheric aerosols, minute particles (either solid or liquid) in the Earth s atmosphere that occur both naturally and because of human activity. At the beginning or end of the day, the Sun s rays travel farther through the atmosphere to reach an observer s eyes and more green and yellow light is scattered, making the Sun appear red. Sunset and sunrise are especially colorful when the concentration of atmospheric particles is high. This ability of aerosols to absorb and reflect sunlight is not just pretty; it also determines the amount of radiation and heat that reaches the Earth s surface, and can profoundly affect climate. In the atmosphere, aerosols are also important as nuclei for the condensation of water droplets and ice crystals. Clouds with fewer aerosols cannot form as many water droplets (called cloud particles), and consequently, do not scatter light well. In this case, more sunlight reaches the Earth s surface. When aerosol levels in clouds are high, however, more nucleation points can form small liquid water droplets. These smaller cloud particles can reflect up to 90 percent of visible radiation to space, keeping the heat from ever reaching Earth s surface. The tendency for these particles to absorb or reflect the Sun s energy - called extinction by astronomers - depends on a number of factors, including chemical composition and the humidity and temperature in the surrounding air; because cloud particles are so small, they are affected quickly by minute changes in the atmosphere. Because of this sensitivity, atmospheric scientists study cloud particles to anticipate patterns and shifts in climate. Until recently, NASA s study of atmospheric aerosols and cloud particles has been focused primarily on satellite images, which, while granting large-scale atmospheric analysis, limited scientists ability to acquire detailed information about individual particles. Now, experiments with specialized equipment can be flown on standard jets, making it possible for researchers to monitor and more accurately anticipate changes in Earth s atmosphere and weather patterns.

Source record↗

NASA NTRS2015

The Dependence of Cirrus Gamma Size Distributions Expressed as Volumes in N(sub 0)-Lambda-Mu Phase Space and Bulk Cloud Properties on Environmental Conditions: Results from the Small Ice Particles in Cirrus Experiment (SPARTICUS)

The variability of cirrus ice microphysical properties is investigated using observations obtained during the Small Particles in Cirrus (SPARTICUS) campaign. An existing approach that represents a size distribution (SD) as a single gamma function using an ellipsoid of equally realizable solutions in (N(sub 0), lambda, mu) phase space is modified to automatically identify multiple modes in SDs and characterize each mode by such an ellipsoid. The modified approach is applied to ice crystals with maximum dimension D greater than15 micrometers collected by the 2-D stereo and 2-D precipitation probes on the Stratton Park Engineering Company Learjet. The dependencies of N(sub 0), mu, and lambda from each mode, total number concentration, bulk extinction, ice water content (IWC), and mass median maximum dimension D(sub mm) as a function of temperature T and cirrus type are then analyzed. The changes in the observed codependencies between N(sub 0), mu, and lambda, bulk extinction, IWC, and D(sub mm) with environmental conditions indicate that particles were larger at higher T during SPARTICUS. At most two modes were observed in any SD during SPARTICUS, with the average boundary between them at 115 micrometers, similar to past studies not using probes with shatter mitigating tips and artifact removal algorithms. The bimodality of the SDs increased with T. This and the differences in N(sub 0), mu, and lambda between the modes suggest that particles with smaller D nucleated more recently than particles with larger D, which grew via vapor deposition and aggregation. Because smaller crystals, whose concentrations are uncertain, make marginal contributions to higher order moments, the use of higher moments for evaluating model fields is suggested.

Ellipsoids↗

NASA NTRS1987

Analysis of mid-tropospheric Space Shuttle exhausted aluminum oxide particles

Aluminum oxide particles from the exhaust of the Space Shuttle were collected immediately after the launch of the SEPEX mission and during the descent over the altitude interval of 7.6-4.6 km. The SEM examination revealed that the particles were spherical and ranged in diameter from about 0.1 micron to 10 microns. Results from the energy dispersive analysis (by an X-ray method) and of the particle chemistry (by electron spectroscopy) confirmed that the particles were predominantly composed of aluminum and oxygen. The particle size distribution of the Al2O3 was bimodal, with one observed peak centered near 2.0 microns; the other distribution mode centered at a diameter of less than 0.3 micron, but could not be accurately located. A mass median diameter was slightly less than 2 microns. Evaluation of ice nucleation activity revealed only a small fraction (about 1 ppm) of active ice nuclei among the Al2O3 particulates.

Cofer, Wesley R., III↗

NASA NTRS1989

Cirrus crystal nucleation by homogeneous freezing of solution droplets

A numerical model consisting of a system of differential equations is used to study cirrus crystal nucleation in a rising parcel containing a distribution of cloud condensation nuclei. The evolution of the particle population and the thermodynamic variables in the parcel are examined. The results suggest that, if homogeneous freezing is not considered, liquid water should be detected below -40 C. If homogeneous freezing is considered, the rapid growth of ice crystals and vapor depletion prevent water saturation from being reached. It is shown that the likelihood of a droplet being frozen is increased by lower temperatures, larger droplet diameter, or lower solution density.

Heymsfield, Andrew J.↗

NASA NTRS1987

Dunes in the north polar region of Mars - Their possible formation from low-density sedimentary aggregates

Low-density aggregates composed of submicron clay aerosols were formed experimentally as the sublimation residues of masses of dust-nucleated ice. These ice-dust mixtures are considered to be possible analogs of materials of Martian north polar deposits. Low-density (0.002 g/cu cm) spheroidal pellets formed from these materials in wind tunnel experiments are studied as possible candidates for the formation of dunes in the north polar region of Mars. It is shown that these particles move like sand grains under conditions of saltation and, taken in sufficient quantities, can form the dunes observed in the north circumpolar erg.

Saunders, R. S.↗

NASA NTRS1994

Real refractive indices of infrared-characterized nitric-acid/ice films: Implications for optical measurements of polar stratospheric clouds

The infrared spectra of nitric-acid/ice films representative of polar stratospheric clouds (PSCs) were collected with simultaneous optical interference measurements to determine the real refractive indices at lambda = 632 nm. Ice and amphorous nitric-acid/ice films were prepared by condensation of water and nitric acid vapors onto a wedged Al2O3 substrate. The real refractive indices of these films were determined from the optical interference of a reflected helium-neon laser during film growth. The indices of the amphorous films varied smoothly from n = 1.30 for ice to n = 1.49 for nitric acid, similar to observations in previous work. We were unable to obtain the refractive index of crystlline films during adsorption because of optical scattering caused by surface roughness. Therefore crystlline nitric acid hydrate films were prepared by annealing amphorous nitric-acid/ice films. Further heating caused desorption of the crystalline hydrate films. During desorption, the refractive indices for ice, NAM (nitric acid monohydrate), alpha- and beta-NAT (nitric acid trihydrate) films were measured using the optical interference technique. In agreement with earlier data, the real refractive indices for ice and NAM determined in desorption were n = 1.30 +/- 0.01 and n = 1.53 +/- 0.03, respectively. The real refractive indices for alpha- and beta-NAT were found to be n = 1.51 +/- 0.01 and n greater than or equal to 1.46, respectively. Our measurements also suggest that the shape of crystalline nitric acid particles may depend on whether they nucleate from the liquid or by vapor deposition. If confirmed by future studies, this observation may provide a means of distinguishing the nucleation mechanism of crystalline PSCs.

Middlebrook, Ann M.↗

NASA NTRS2016

Stability of the Early Mars Atmosphere to Collapse into Permanent Polarcaps

The presence of a permanent CO2 polar ice cap on Mars has important consequences for the planet's climate system. The heat balance of such a cap, which is determined mainly by atmospheric heat transport, and the downward solar in infrared radiative fluxes, determines its surface temperature, which through the vapor pressure relation sets the mean annual surface pressure. On Mars today, for example, the south residual CO2 cap is present year-round with a mean annual temperature of approximately 145 K which corresponds to a mean annual CO2 vapor pressure of approximately 600 Pa. On early Mars, permanent polar caps are also possible especially since the sun was less luminous 3.5-4.0 Gya. Thus, the existence of permanent polar caps on early Mars is central to understanding the nature of the planets climate system in those ancient times and whether or not the atmosphere might have been capable of sustaining conditions suitable for liquid water flowing over the surface as is indicated in the geological record. Forget et al [1] showed that for present orbital properties atmospheric collapse into permanent polar caps could only be prevented for surface pressures roughly between 500 - 3000 hPa. Though follow-on studies confirm and extend the Forget et al. results [2], the full sensitivity of this "window" of stability has not been explored. There are many factors to consider such the albedo of the caps, dust content of the atmosphere, and the presence of water ice clouds. However, we begin our exploration of the stability of the early Martian atmosphere by focusing on the role of CO2 ice clouds. In some preliminary simulations with the Ames Mars General Circulation Model (GCM) we found that atmospheric collapse depends on assumptions regarding the fate of CO2 ice clouds. If, for example, we assume the clouds immediately fall to the surface, then in some cases collapse is favored. On the other hand if the clouds are allowed to fall and evaporate, collapse can be averted. This implies that CO2 ice cloud microphysics is important to the overall stability of the atmosphere. Though the Ames GCM has a sophisticated CO2 cloud microphysics package that includes nucleation, growth, and sedimentation (see accompanying poster by Kahre et al. [3]), we have implemented a simpler scheme based on the Forget et al. [1] approach to CO2 ice clouds. Our goal is to reproduce and expand their study. The key parameter in this approach is the concentration and vertical distribution of cloud condensation nuclei (CCN), i.e., dust particles. Fewer CCN lead to larger particles which fall faster, while higher CCN concentrations lead to smaller particles and thicker clouds that remain suspended for longer periods of time. We plan to explore the stability of the atmosphere to CCN concentrations and distributions and then assess the capability of thick early atmospheres to loft and distribute dust particles (CCN) around the planet. Thus, our work will shed light on the nature of the coupling between the dust and CO2 cycles and the implications it has for the early Mars climate system.

ice cap↗

NASA NTRS1997

A Laboratory Study on the Phase Transition for Polar Stratospheric Cloud Particles

The nucleation and growth of different phases of simulated polar stratospheric cloud (PSC) particles were investigated in the laboratory. Solutions and mixtures of solutions at concentrations 1 to 5 m (molality) of ammonium sulfate, ammonium bisulfate, sodium chloride, sulfuric acid, and nitric acid were supercooled to prescribed temperatures below their equilibrium melting point. These solutions were contained in small diameter glass tubing of volumes ranging from 2.6 to 0.04 ml. Samples were nucleated by insertion of an ice crystal, or in some cases by a liquid nitrogen cooled wire. Crystallization velocities were determined by timing the crystal growth front passages along the glass tubing. Solution mixtures containing aircraft exhaust (soot) were also examined. Crystallization rates increased as deltaT2, where deltaT is the supercooling for weak solutions (2 m or less). The higher concentrated solutions (greater than 3 m) showed rates significantly less than deltaT2. This reduced rate suggested an onset of a glass phase. Results were applied to the nucleation of highly concentrated solutions at various stages of polar stratospheric cloud development within the polar stratosphere.

Teets, Edward H., Jr.↗

DOE OSTI2020

Contrasting aerosol effects on longwave cloud forcing in South East Asia and Amazon simulated with Community Atmosphere Model version 5.3

Aerosols modify cloud microphysical and radiative properties and thus impact the shortwave (SW) and longwave cloud forcing (LWCF). This study first reports the finding of contrasting aerosol effects on LWCF in South East Asia and Amazon in the Community Atmosphere Model version 5.3 (CAM5.3), which corresponds to the sum of LW indirect and semi-direct effects investigated in Ghan et al., (2012). A series of numerical experiments is conducted to decompose the complex aerosol effects on LWCF. Our analysis indicates that the cooling (negative aerosol effects on LWCF) in Amazon is due mainly to the aerosol effects on warm clouds and the inhibition of vertical motion by the aerosol-induced radiative cooling. In contrast, the warming (positive aerosol effects on LWCF) in South East Asia is due mainly to the aerosol effect on homogeneous freezing, thus reducing the ice particle size and prolonging the existence of ice cloud. Our results emphasize that a comprehensive analysis of integrated aerosol effects on both warm and ice clouds is necessary for better understanding the aerosol effects on LWCF.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2012

Performance of McRAS-AC in the GEOS-5 AGCM: Part 1, Aerosol-Activated Cloud Microphysics, Precipitation, Radiative Effects, and Circulation

A revised version of the Microphysics of clouds with Relaxed Arakawa-Schubert and Aerosol-Cloud interaction (McRAS-AC), including, among others, the Barahona and Nenes ice nucleation parameterization, is implemented in the GEOS-5 AGCM. Various fields from a 10-year long integration of the AGCM with McRAS-AC were compared with their counterparts from an integration of the baseline GEOS-5 AGCM, and with satellite data as observations. Generally using McRAS-AC reduced biases in cloud fields and cloud radiative effects are much better over most of the regions of the Earth. Two weaknesses are identified in the McRAS-AC runs, namely, too few cloud particles around 40S-60S, and too high cloud water path during northern hemisphere summer over the Gulf Stream and North Pacific. Sensitivity analyses showed that these biases potentially originated from biases in the aerosol input. The first bias is largely eliminated in a sensitivity test using 50% smaller aerosol particles, while the second bias is much reduced when interactive aerosol chemistry was turned on. The main drawback of McRAS-AC is dearth of low-level marine stratus clouds, probably due to lack of dry-convection, not yet implemented into the cloud scheme. Despite these biases, McRAS-AC does simulate realistic clouds and their optical properties that can improve with better aerosol-input and thereby has the potential to be a valuable tool for climate modeling research because of its aerosol indirect effect simulation capabilities involving prediction of cloud particle number concentration and effective particle size for both convective and stratiform clouds is quite realistic.

Sud, Y. C.↗