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Cirrus Cloud Seeding has Potential to Cool Climate

Cirrus clouds, thin ice clouds in the upper troposphere, have a net warming effect on Earth s climate. Consequently, a reduction in cirrus cloud amount or optical thickness would cool the climate. Recent research indicates that by seeding cirrus clouds with particles that promote ice nucleation, their lifetimes and coverage could be reduced. We have tested this hypothesis in a global climate model with a state-of-the-art representation of cirrus clouds and find that cirrus cloud seeding has the potential to cancel the entire warming caused by human activity from pre-industrial times to present day. However, the desired effect is only obtained for seeding particle concentrations that lie within an optimal range. With lower than optimal particle concentrations, a seeding exercise would have no effect. Moreover, a higher than optimal concentration results in an over-seeding that could have the deleterious effect of prolonging cirrus lifetime and contributing to global warming.

Storelvmo, T.↗

Modeling Aerosol Nucleation

The goal of this work has been to understand how nitric acid condenses on cirrus ice cloud particles by analyzing data obtained during the SAGE III Ozone Loss and Validation Experiment (SOLVE) research mission based out of Kiruna, Sweden. Ms. Gamblin simultaneously analyzed gas phase nitric acid data along with particulate NO, data, particulate, vapor and gas-phase water data from several different instruments, particle size data, which included surface area and volume measurements, ozone concentration data as well as temperature, pressure and GPS coordinates of the sampled air parcel. All parameters where held constant with only one allowed to vary in order to determine what controls the extent to which nitric acid will condensation on ice. In addition, this data was compared to theoretical values of nitric acid condensation on ice based upon recent laboratory data. Comparison of these two data sets shows the field data does not agree with what is expected in the laboratory at comparable temperatures and nitric acid pressures. The most significant difference is that surface coverages in the atmosphere were found to be elevated relative to surface coverages measured in the laboratory. The results of this study were accepted for publication by Geophysical Research Letters.

Toon, Owen B.↗

Ice nucleation activity of rocket effluent

An investigation was conducted concerning the ice nucleation activity of the exhaust products of solid rockets. The Voyager I and II payloads were launched from Kennedy Space Center on September 5 and August 20, 1977, respectively. A visible stabilized ground cloud (SGC) consisting of rocket effluent and dust formed downwind. An instrumented aircraft was used to make multiple passes in the SGC. A Mylar bag was rapidly filled with SGC aerosol and then immediately sampled with an ice nucleus counter. Analyses of rocket effluent collected are discussed, taking into account the ice nucleus concentration, particle concentration and size distribution, and the elemental composition of individual particles. A description of laboratory experiments is also presented, giving attention to the elemental composition of individual particles and the ice nucleus concentration.

Parungo, F. P.↗

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↗

SUCCESS Evidence for Cirrus Cloud Ice Nucleation Mechanisms

During the SUCCESS mission, several measurements were made which should improve our understanding of ice nucleation processes in cirrus clouds. Temperature and water vapor concentration were made with a variety of instruments on the NASA DC-8. These observations should provide accurate upper tropospheric humidities. In particular, we will evaluate what humidities are required for ice nucleation. Preliminary results suggest that substantial supersaturations frequently exist in the upper troposphere. The leading-edge region of wave-clouds (where ice nucleation occurs) was sampled extensively at temperatures near -40 and -60C. These observations should give precise information about conditions required for ice nucleation. In addition, we will relate the observed aerosol composition and size distributions to the ice formation observed to evaluate the role of soot or mineral particles on ice nucleation. As an alternative technique for determining what particles act as ice nuclei, numerous samples of aerosols inside ice crystals were taken. In some cases, large numbers of aerosols were detected in each crystal, indicating that efficient scavenging occurred. Analysis of aerosols in ice crystals when only one particle per crystal was detected should help with the ice nucleation issue. Direct measurements of the ice nucleating activity of ambient aerosols drawn into airborne cloud chambers were also made. Finally, measurements of aerosols and ice crystals in contrails should indicate whether aircraft exhaust soot particles are effective ice nuclei.

Jensen, Eric↗

Ice Nucleation in the Tropical Tropopause Layer: Implications for Cirrus Occurrence, Cirrus Microphysical Properties, and Dehydration of Air Entering the Stratosphere

Recent laboratory experiments have advanced our understanding of the physical properties and ice nucleating abilities of aerosol particles atlow temperatures. In particular, aerosols containing organics will transition to a glassy state at low temperatures, and these glassy aerosols are moderately effective as ice nuclei. These results have implications for ice nucleation in the cold Tropical Tropopause Layer (TTL; 13-19 km). We have developed a detailed cloud microphysical model that includes heterogeneous nucleation on a variety of aerosol types and homogeneous freezing of aqueous aerosols. This model has been incorporated into one-dimensional simulations of cirrus and water vapor driven by meteorological analysis temperature and wind fields. The model includes scavenging of ice nuclei by sedimenting ice crystals. The model is evaluated by comparing the simulated cloud properties and water vapor concentrations with aircraft and satellite measurements. In this presentation, I will discuss the relative importance of homogeneous and heterogeneous ice nucleation, the impact of ice nuclei scavenging as air slowly ascends through the TTL, and the implications for the final dehydration of air parcels crossing the tropical cold-point tropopause and entering the tropical stratosphere.

tropopause↗

Ice Nucleation and Dehydration in the Tropical Tropopause Layer

Optically thin cirrus near the tropical tropopause regulate the humidity of air entering the stratosphere, which in turn has a strong influence on the Earth's radiation budget and climate. Recent highaltitude, unmanned aircraft measurements provide evidence for two distinct classes of cirrus formed in the tropical tropopause region: (i) vertically extensive cirrus with low ice number concentrations, low extinctions, and large supersaturations (up to approx. 70%) with respect to ice; and (ii) vertically thin cirrus layers with much higher ice concentrations that effectively deplete the vapor in excess of saturation. The persistent supersaturation in the former class of cirrus is consistent with the long time-scales (several hours or longer) for quenching of vapor in excess of saturation given the low ice concentrations and cold tropical tropopause temperatures. The low-concentration clouds are likely formed on a background population of insoluble particles with concentrations less than 100 L−1 (often less than 20 L−1), whereas the high ice concentration layers (with concentrations up to 10,000 L−1) can only be produced by homogeneous freezing of an abundant population of aqueous aerosols. These measurements, along with past high-altitude aircraft measurements, indicate that the low-concentration cirrus occur frequently in the tropical tropopause region, whereas the high-concentration cirrus occur infrequently. The predominance of the low-concentration clouds means cirrus near the tropical tropopause may typically allow entry of air into the stratosphere with as much as approx. 1.7 times the ice saturation mixing ratio.

dehydration↗

Aircraft-Measured Indirect Cloud Effects from Biomass Burning Smoke in the Arctic and Subarctic

The incidence of wildfires in the Arctic and subarctic is increasing; in boreal North America, for example, the burned area is expected to increase by 200-300 over the next 50-100 years, which previous studies suggest could have a large effect on cloud microphysics, lifetime, albedo, and precipitation. However, the interactions between smoke particles and clouds remain poorly quantified due to confounding meteorological influences and remote sensing limitations. Here, we use data from several aircraft campaigns in the Arctic and subarctic to explore cloud microphysics in liquid-phase clouds influenced by biomass burning. Median cloud droplet radii in smoky clouds were 50 smaller than in background clouds. Based on the relationship between cloud droplet number (N(liq))/ and various biomass burning tracers (BBt/ across the multi-campaign dataset, we calculated the magnitude of subarctic and Arctic smoke aerosol-cloud interactions (ACI, where ACI = (1/3) x dln(N(liq))/dln(BBt)) to be 0.12 out of a maximum possible value of 0.33 that would be obtained if all aerosols were to nucleate cloud droplets. Interestingly, in a separate subarctic case study with low liquid water content (0.02 gm/ cu m) and very high aerosol concentrations (2000-3000 cu m) in the most polluted clouds, the estimated ACI value was only 0.06. In this case, competition for water vapor by the high concentration of CCN strongly limited the formation of droplets and reduced the cloud albedo effect, which highlights the importance of cloud feedbacks across scales. Using our calculated ACI values, we estimate that the smoke-driven cloud albedo effect may decrease shortwave radiative flux by 2 and 4 W/sq or more under some low and homogeneous cloud cover conditions in the subarctic, although the changes should be smaller in high surface albedo regions of the Arctic. We lastly show evidence to suggest that numerous northern latitude background Aitken particles can interact with combustion particles, perhaps impacting their properties as cloud condensation and ice nuclei. However, the influence of background particles on smoke-driven indirect effects is currently unclear.

Arctic↗

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↗

Aircraft-Measured Indirect Cloud Effects from Biomass Burning Smoke in the Arctic and Subarctic

The incidence of wildfires in the Arctic and subarctic is increasing; in boreal North America, for example, the burned area is expected to increase by 200-300% over the next 50-100 years, which previous studies suggest could have a large effect on cloud microphysics, lifetime, albedo, and precipitation. However, the interactions between smoke particles and clouds remain poorly quantified due to confounding meteorological influences and remote sensing limitations. Here, we use data from several aircraft campaigns in the Arctic and subarctic to explore cloud microphysics in liquid-phase clouds influenced by biomass burning. Median cloud droplet radii in smoky clouds were approx. 40- 60% smaller than in background clouds. Based on the relationship between cloud droplet number (N(liq)/ and various biomass burning tracers (BBt/ across the multi-campaign data set, we calculated the magnitude of subarctic and Arctic smoke aerosol-cloud interactions (ACIs, where ACI = (1/3) x dln(N(liq))/dln(BBt)) to be approx. 0.16 out of a maximum possible value of 0.33 that would be obtained if all aerosols were to nucleate cloud droplets. Interestingly, in a separate subarctic case study with low liquid water content (0.02 gm/cu m and very high aerosol concentrations (2000- 3000/ cu cm in the most polluted clouds, the estimated ACI value was only 0.05. In this case, competition for water vapor by the high concentration of cloud condensation nuclei (CCN) strongly limited the formation of droplets and reduced the cloud albedo effect, which highlights the importance of cloud feedbacks across scales. Using our calculated ACI values, we estimate that the smoke-driven cloud albedo effect may decrease local summertime short-wave radiative flux by between 2 and 4 W/sq m or more under some low and homogeneous cloud cover conditions in the subarctic, although the changes should be smaller in high surface albedo regions of the Arctic.We lastly explore evidence suggesting that numerous northern-latitude background Aitken particles can interact with combustion particles, perhaps impacting their properties as cloud condensation and ice nuclei.

cloud microphysics↗

Anvil Glaciation in a Deep Cumulus Updraught over Florida Simulated with the Explicit Microphysics Model. I: Impact of Various Nucleation Processes

Simulations of a cumulonimbus cloud observed in the Cirrus regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) with an advanced version of the Explicit Microphysics Model (EMM) are presented. The EMM has size-resolved aerosols and predicts the time evolution of sizes, bulk densities and axial ratios of ice particles. Observations by multiple aircraft in the troposphere provide inputs to the model, including observations of the ice nuclei and of the entire size distribution of condensation nuclei. Homogeneous droplet freezing is found to be the source of almost all of the ice crystals in the anvil updraught of this particular model cloud. Most of the simulated droplets that freeze to form anvil crystals appear to be nucleated by activation of aerosols far above cloud base in the interior of the cloud ("secondary" or "in cloud" droplet nucleation). This is partly because primary droplets formed at cloud base are invariably depleted by accretion before they can reach the anvil base in the updraught, which promotes an increase with height of the average supersaturation in the updraught aloft. More than half of these aerosols, activated far above cloud base, are entrained into the updraught of this model cloud from the lateral environment above about 5 km above mean sea level. This confirms the importance of remote sources of atmospheric aerosol for anvil glaciation. Other nucleation processes impinge indirectly upon the anvil glaciation by modifying the concentration of supercooled droplets in the upper levels of the mixed-phase region. For instance, the warm-rain process produces a massive indirect impact on the anvil crystal concentration, because it determines the mass of precipitation forming in the updraught. It competes with homogeneous freezing as a sink for cloud droplets. The effects from turbulent enhancement of the warm-rain process and from the nucleation processes on the anvil ice properties are assessed.

Phillips, Vaughan T. J.↗

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↗

Analysis of Ice Nucleating Aerosol Measurements during SUCCESS: April, May 1996

This section describes our research activities during year three of this effort. In the second year, preliminary archive data sets were submitted to the SUCCESS archive. After additional analyses, final versions were prepared and submitted. These are included on the SUCCESS CD-ROM data editions that were recently released by NASA Ames. Over the range of temperature and supersaturation conditions of our measurements (15 to -40 C, and from ice saturation to approximately 15% water supersaturation), IN concentrations ranged from less than 0.1 to approximately 500 per liter, being generally greater at colder temperatures and higher supersaturations. To estimate the potential of aircraft exhaust as a source of IN, we examined data from six days of the field project when the DC-8 was following closely behind other humidity conditions of our measurements. In April 1997, a microphysical workshop was convened at NCAR to select cases for in depth analyses and to address questions about the consistency of cloud ice crystal measurements (size distributions and mass concentrations) and aerosol size distributions. We attended this meeting and contributed to the discussions. A particular concern was identified in the CN measurements. On the DC-8, CN measurements were obtained by four different investigator groups, using commercially available instrumentation. The DC-8 SUCCESS CN data showed long periods where the measurements were in substantial agreement, but there were also periods with large discrepancies. Several possible factors were identified that could help explain these discrepancies, including minimum detectable particle size, response at reduced pressures, and location of sample inlet on the aircraft.

Rogers, D. C.↗

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.↗

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.↗

On the Importance of Small Ice Crystals in Tropical Anvil Cirrus

In situ measurements of ice crystal concentrations and sizes made with aircraft instrumentation over the past two decades have often indicated the presence of numerous relatively small (< 50 m diameter) crystals in cirrus clouds. Further, these measurements frequently indicate that small crystals account for a large fraction of the extinction in cirrus clouds. The fact that the instruments used to make these measurements, such as the Forward Scattering Spectrometer Probe (FSSP) and the Cloud Aerosol Spectrometer (CAS), ingest ice crystals into the sample volume through inlets has led to suspicion that the indications of numerous small ]crystals could be artifacts of large ]crystal shattering on the instrument inlets. We present new aircraft measurements in anvil cirrus sampled during the Tropical Composition, Cloud, and Climate Coupling (TC4) campaign with the 2 ] Dimensional Stereo (2D ]S) probe, which detects particles as small as 10 m. The 2D ]S has detector "arms" instead of an inlet tube. Since the 2D ]S probe surfaces are much further from the sample volume than is the case for the instruments with inlets, it is expected that 2D ]S will be less susceptible to shattering artifacts. In addition, particle inter ]arrival times are used to identify and remove shattering artifacts that occur even with the 2D ]S probe. The number of shattering artifacts identified by the 2D ]S interarrival time analysis ranges from a negligible contribution to an order of magnitude or more enhancement in apparent ice concentration over the natural ice concentration, depending on the abundance of large crystals and the natural small ]crystal concentration. The 2D ]S measurements in tropical anvil cirrus suggest that natural small ]crystal concentrations are typically one to two orders of magnitude lower than those inferred from CAS. The strong correlation between the CAS/2D ]S ratio of small ]crystal concentrations and large ]crystal concentration suggests that the discrepancy is likely caused by shattering of large crystals on the CAS inlet. We argue that past measurements with CAS in cirrus with large crystals present may contain errors due to crystal shattering, and past conclusions derived from these measurements may need to be revisited. Further, we present correlations between CAS spurious concentration and 2D ]S large ]crystal mass from spatially uniform anvil cirrus sampling periods as an approximate guide for estimating quantitative impact of large ]crystal shattering on CAS concentrations in previous datasets. We use radiative transfer calculations to demonstrate that in the maritime anvil cirrus sampled during TC4, small crystals indicated by 2D ]S contribute relatively little cloud extinction, radiative forcing, or radiative heating in the anvils, regardless of anvil age or vertical location in the clouds. While 2D ]S ice concentrations in fresh anvil cirrus may often exceed 1 cm.3, and are observed to exceed 10 cm.3 in turrets, they are typically ~0.1 cm.3 and rarely exceed 1 cm.3 (<1.4% of the time) in aged anvil cirrus. We hypothesize that isolated occurrences of higher ice concentrations in aged anvil cirrus may be caused by ice nucleation driven by either small ]scale convection or gravity waves. It appears that the numerous small crystals detrained from convective updrafts do not persist in the anvil cirrus sampled during TC ]4.

Jensen, E. J.↗