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A Study of Direct and Cloud-Mediated Radiative Forcing of Climate Due to Aerosols

The Intergovernmental Panel on Climate Change (IPCC) has reported that in the southeastern US and eastern China, the general greenhouse warming due to anthropogenic gaseous emissions is dominated by the cooling effect of anthropogenic aerosols. To verify this model prediction in eastern China and southeastern US, we analyzed regional patterns of climate changes at 72 stations in eastern China during 1951- 94 (44 years), and at 52 stations in the southeastern US during 1949-94 (46 years) to detect the fingerprint of aerosol radiative forcing. It was found that the mean rates of change of annual mean daily, maximum, minimum temperatures and diurnal temperature range (DTR) in eastern China were 0.8, -0.2, 1.8, and -2.0 C/100 years respectively, while the mean rates of change of annual mean daily, maximum, minimum temperatures and DTR in the southeastern US were -0.2, -0.6, 0.2, and -0.8 C/100 years, respectively. This indicates that the high rate of increase in annual mean minimum temperature in eastern China results in a slightly warming trend of daily temperature, while the high rate of decrease in annual mean maximum temperature and low rate of increase in annual mean minimum temperature lead to the cooling trend of daily temperature in the southeastern US. We found that the warming from the longwave forcing due to both greenhouse gases and aerosols was completely counteracted by the shortwave aerosol forcing in the southeastern US in the past 46 years. A slightly overall warming trend in eastern China is evident; winters have become milder. This finding is explained by hypothesizing that increasing energy usage during the past 44 years has resulted in more coal and biomass burning, thus increasing the emission of absorbing soot and organic aerosols in eastern China. Such emissions, in addition to well-known Asia dust and greenhouse gases, may be responsible for the winter warming trend in eastern China that we have reported here. The sensitivity of aerosol radiative properties to aerosol composition, size distribution, relative humidity (RH) is examined for the following aerosol systems: inorganic and organic ions (Cl-, Br-, NO3 -, SO4 2-, Na+, NH4 +, K+, Ca2+, Mg2+, HCOO-, CH3COO-, CH3CH2COO-, CH3COCOO-, OOCCOO2-, MSA-1); water-insoluble inorganic and organic compounds (elemental carbon, n-alkanes, SiO2, Al2O3, Fe2O3 and other organic compounds). The partial molar refraction method was used to calculate the real part of the refractive index. It was found that the asymmetry factor increased by approximately 48% with the real part varying from 1.40 to 1.65, and the single scattering albedo decreased by 24% with the imaginary part varying from -0.005 to -0.1. The asymmetry factor increased by 5.4 times with the geometric standard deviation varying from 1.2 to 3.0. The radiation transmission is very sensitive to the change in size distribution; other factors are not as significant. To determine the aerosol direct radiative forcing (ADRF), the aerosol optical depth (AOD) values at the three operational wavelengths (415, 500 and 673 nm) were determined at a regionally representative site, namely, Mt. Gibbs (35.78 deg N, 82.29 deg W, elevation 2006 m) in Mt. Mitchell State Park, NC, and a site located in an adjacent valley (Black Mountain, 35.66 deg N, 82.38 deg W, elevation 951 m) in the southeastern US. The two sites are separated horizontally by 10 km and vertically by 1 km. It was found that the representative total AOD values at 500 nm at the valley site for highly polluted (HP), marine (M) and continental (C) air masses were 0.68 +/- 0.33, 0.29 +/- 0.19 and 0.10 +/- 0.04, respectively. A search-graph method was used to retrieve the columnar size distribution (number concentration N, effective radius reff and geometric standard deviation=?g) from the optical depth observations at three operational wavelengths. The ground albedo, single scattering albedo and imaginary part of the refractive index were calculated using a mathematically unique procedure involving a Mie code and a radiative transfer code in conjunction with the retrieved aerosol size distribution, AOD, and diffuse-direct irradiance ratio. It was found that N, r(eff) and sigma(g) were in the ranges of 10 to 1.7 x 10(exp 4)/cubic cm, 0.09 to 0.68 micrometers and 1.12 to 2.95, respectively. The asymmetry factor and single scattering albedo were in the ranges of 0.63 to 0.75 and 0.74 to 0.97 respectively. The ground albedo for the forested terrain and imaginary part of refractive index were found to be in the ranges of 0.06 to 0.29 and 0.005 to 0.051 respectively. On the basis of these aerosol radiative properties obtained at the research sites and computations using the Column Radiation Model (CRM) of National Center of Atmospheric Research (NCAR) Community Climate Model (CCM3), it was found that the average cloud-free 24-hour ADRF values were -13 +/- 8, -8 +/- 3, -33 +/- 16 W/square m for marine, continental, and polluted air masses, respectively. On the assumption that the fractional coverage of clouds is 0.61, it was estimated that the annual mean ADRF was 7 +/- 2 W/square m in the southeastern US. The review with respect to the current knowledge of organic acids shows that aerosol formate and acetate concentrations range from 0.02 to 5.3 nmol/cubic m and from 0.03 to 12.4 nmol/cubic m respectively, and that between 34% to 77% of formate and between 21% to 66% of acetate are present in the fine fraction of aerosols. It was found that although most (98-99%) of these volatile organic acids were present in the gas phase, their concentrations in the aerosol particles were sufficient to make them a good candidate for cloud condensation nuclei (CCN). It is hypothesized that organic acids are at least one of the primary sources of CCN in the atmosphere due to their ubiquitous presence in the troposphere, especially over the continental forested areas. The results of our measurements at Palmer Station, Antarctica show that the daily average CCN concentrations at 0.3% and 1% supersaturations ranged from 0.3 to 160/cubic cm and from 4 to 168/cubic cm, respectively, during the period from 17 January to 26 February, 1994. New evidence for substantial and definitive CCN enhancement near and within cloud has been observed at Mt. Mitchell, North Carolina. The results show that the average monthly CCN concentrations were 460 +/- 217, 386 +/- 286, 429 +/- 228 and 238 +/- 134/cubic cm for in-cloud, overcast, clear and rainy conditions, respectively. The typical CCN spectra show that there were a lot of small CCN produced and the ion concentrations (especially H+ and SO4 2-) were very high during the CCN enhancement period. The significantly positive correlation between black carbon (BC) and CCN at 1% supersaturation indicates that a percentage of the BC measured at the site may be in the form of an internal mixture and participated in the formation of CCN.

Yu, Shao-Cai↗

Evaluation of Global Simulations of Aerosol Particle and Cloud Condensation Nuclei Number, with Implications for Cloud Droplet Formation

A total of 16 global chemistry transport models and general circulation models have participated in this study; 14 models have been evaluated with regard to their ability to reproduce the near-surface observed number concentration of aerosol particles and cloud condensation nuclei (CCN), as well as derived cloud droplet number concentration (CDNC). Model results for the period 2011-2015 are compared with aerosol measurements (aerosol particle number, CCN and aerosol particle composition in the submicron fraction) from nine surface stations located in Europe and Japan. The evaluation focuses on the ability of models to simulate the average across time state in diverse environments and on the seasonal and short-term variability in the aerosol properties. There is no single model that systematically performs best across all environments represented by the observations. Models tend to underestimate the observed aerosol particle and CCN number concentrations, with average normalized mean bias (NMB) of all models and for all stations, where data are available, of -24% and -35% for particles with dry diameters > 50 and > 120nm, as well as -36% and -34% for CCN at supersaturations of 0.2% and 1.0%, respectively. However, they seem to behave differently for particles activating at very low supersaturations (< 0.1%) than at higher ones. A total of 15 models have been used to produce ensemble annual median distributions of relevant parameters. The model diversity (defined as the ratio of standard deviation to mean) is up to about 3 for simulated N3 (number concentration of particles with dry diameters larger than 3 nm) and up to about 1 for simulated CCN in the extra-polar regions. A global mean reduction of a factor of about 2 is found in the model diversity for CCN at a supersaturation of 0.2% (CCN(0.2)) compared to that for N3, maximizing over regions where new particle formation is important. An additional model has been used to investigate potential causes of model diversity in CCN and bias compared to the observations by performing a perturbed parameter ensemble (PPE) accounting for uncertainties in 26 aerosol-related model input parameters. This PPE suggests that biogenic secondary organic aerosol formation and the hygroscopic properties of the organic material are likely to be the major sources of CCN uncertainty in summer, with dry deposition and cloud processing being dominant in winter. Models capture the relative amplitude of the seasonal variability of the aerosol particle number concentration for all studied particle sizes with available observations (dry diameters larger than 50, 80 and 120nm). The short-term persistence time (on the order of a few days) of CCN concentrations, which is a measure of aerosol dynamic behavior in the models, is underestimated on average by the models by 40% during winter and 20% in summer.

cloud droplets↗

Impacts of Varying Concentrations of Cloud Condensation Nuclei On Deep Convective Cloud Updrafts – A Multimodel Assessment

This study presents results from a model intercomparison project, focusing on the range of responses in deep convective cloud updrafts to varying cloud condensation nuclei (CCN) concentrations amongst seven, state-of-the-art, cloud-resolving models. Simulations of scattered convective clouds near Houston, Texas are conducted, after being initialized with both relatively low and high CCN concentrations. Deep convective updrafts are identified, and trends in the updraft intensity and frequency are assessed. The factors contributing to the vertical velocity tendencies are examined to identify the physical processes associated with the CCN-induced, updraft changes. The models show several consistent trends. In general, the changes between the High- CCN and Low-CCN simulations in updraft magnitudes throughout the depth of the troposphere are within 15% for all of the models. All models produce stronger (~+5-15%) mean updrafts from ~4–7 km above ground level (AGL) in the High-CCN simulations, followed by a waning response up to ~8 km AGL in most of the models. Thermal buoyancy was more sensitive than condensate loading to varying CCN concentrations in most of the models and more impactful in the mean updraft responses. However, there are also differences between the models. The change in the amount of deep convective updrafts varies significantly. Furthermore, approximately half the models demonstrate neutral-to-weaker (~-5-0%) updrafts above ~8 km AGL, while the other models show stronger (~+10%) updrafts in the High-CCN simulations. The combination of the CCN-induced impacts on the buoyancy and vertical perturbation pressure gradient terms better explains these middle- and upper-tropospheric updraft trends than the buoyancy terms alone.

deep convective cloud updrafts↗

Observations of anthropogenic cloud condensation nuclei

Cloud Condensation Nuclei (CCN) concentrations and spectral measurements obtained with the DRI instantaneous CCN spectrometer (Hudson, 1989) over the last few years are presented. The climatic importance of cloud microphysics has been pointed out. The particles which affect cloud microphysics are cloud condensation nuclei (CCN). The commonly-observed order of magnitude difference in cloud droplet concentrations between maritime and continental air masses (i.e., Squires, 1958) was determined to be caused by systematic differences in the concentrations of CCN between continental and maritime air masses (e.g., Twomey and Wojciechowski, 1969). Twomey (1977) first pointed out that cloud microphysics also affects the radiative properties of clouds. Thus continental and anthropogenic CCN could affect global temperature. Resolution of this Twomey effect requires answers to two questions - whether antropogenic CCN are a significant contribution to atmospheric CCN, and whether they are actually affecting cloud microphysics to an extent which is of climatic importance. The reasons for the contrast between continental and maritime CCN concentration are not understood. The question of the relative importance of anthropogenic CCN is addressed. These observations should shed light on this complex question although further research is being conducted in order to produce more quantitative answers. Accompanying CN measurements made with a TSI 3020 condensation nucleus (CN) counter are also presented.

Hudson, James G.↗

Use of In Situ Cloud Condensation Nuclei, Extinction, and Aerosol Size Distribution Measurements to Test a Method for Retrieving Cloud Condensation Nuclei Profiles From Surface Measurements

If the aerosol composition and size distribution below cloud are uniform, the vertical profile of cloud condensation nuclei (CCN) concentration can be retrieved entirely from surface measurements of CCN concentration and particle humidification function and surface-based retrievals of relative humidity and aerosol extinction or backscatter. This provides the potential for long-term measurements of CCN concentrations near cloud base. We have used a combination of aircraft, surface in situ, and surface remote sensing measurements to test various aspects of the retrieval scheme. Our analysis leads us to the following conclusions. The retrieval works better for supersaturations of 0.1% than for 1% because CCN concentrations at 0.1% are controlled by the same particles that control extinction and backscatter. If in situ measurements of extinction are used, the retrieval explains a majority of the CCN variance at high supersaturation for at least two and perhaps five of the eight flights examined. The retrieval of the vertical profile of the humidification factor is not the major limitation of the CCN retrieval scheme. Vertical structure in the aerosol size distribution and composition is the dominant source of error in the CCN retrieval, but this vertical structure is difficult to measure from remote sensing at visible wavelengths.

Ghan, Stephen J.↗

Dilution of Boundary Layer Cloud Condensation Nucleus Concentrations by Free Tropospheric Entrainment During Marine Cold Air Outbreaks

Recent aircraft measurements over the northwest Atlantic enable an investigation of how entrainment from the free troposphere (FT) impacts cloud condensation nucleus (CCN) concentrations in the marine boundary layer (MBL) during cold-air outbreaks (CAOs), motivated by the role of CCN in mediating transitions from closed to open-cell regimes. Observations compiled over eight flights indicate predominantly far lesser CCN concentrations in the FT than in the MBL. For one flight, a fetch-dependent MBL-mean CCN budget is compiled from estimates of sea-surface fluxes, entrainment of FT air, and hydrometeor collision-coalescence, based on in-situ and remote-sensing measurements. Results indicate a dominant role of FT entrainment in reducing MBL CCN concentrations, consistent with satellite-observed trends in droplet number concentration upwind of CAO cloud-regime transitions over the northwest Atlantic. Relatively scant CCN may widely be associated with FT dry intrusions, and should accelerate cloud-regime transitions where underlying MBL air is CCN-rich, thereby reducing regional albedo.

Boundary Layer Cloud Condensation Nucleus Concentr↗

The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

Cloud microphysics are inevitably affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distributions parameterized as spectral bin microphysics are needed to explicitly study the effects of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates for convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensemble (GCE) model. The formulation for the explicit spectral-bin microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e.,pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), graupel and frozen drops/hail]. Each type is described by a special size distribution function containing many categories (i.e. 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.A spectral-bin microphysical model is very expensive from a from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep tropical clouds in the west Pacific warm pool region using identical thermodynamic conditions but with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. Besides the initial differences in aerosol concentration, preliminary results indicate that the low CCN concentration case produces rainfall at the surface sooner than the high CCN case but has less cloud water mass aloft. Because the spectral-bin model explicitly calculates and allows for the examination of both the mass and number concentration of species in each size categor, a detailed analysis of the instantaneous size spectrum can be obtained for the two cases. It is shown that since the low CCN case produces fewer droplets, larger sized develop due to the greater condensational and collectional growth, leading to a broader size spectrum in comparison to the high CCN case.

Tao, Wei-Kuo↗

The Impact of Aerosols on Cloud and Precipitation Processes: Cloud-Resolving Model Simulations

Cloud microphysics are inevitable affected by the smoke particle (CCN, cloud condensation nuclei) size distributions below the clouds. Therefore, size distribution parameterized as spectral bin microphysics are needed to explicitly study the effect of atmospheric aerosol concentration on cloud development, rainfall production, and rainfall rates convective clouds. Recently, two detailed spectral-bin microphysical schemes were implemented into the Goddard Cumulus Ensembel (GCE) model. The formulation for the explicit spectral-bim microphysical processes is based on solving stochastic kinetic equations for the size distribution functions of water droplets (i.e., cloud droplets and raindrops), and several types of ice particles [i.e., pristine ice crystals (columnar and plate-like), snow (dendrites and aggregates), groupel and frozen drops/hall] Each type is described by a special size distribution function containing many categories (i.e., 33 bins). Atmospheric aerosols are also described using number density size-distribution functions.A spectral-bin microphysical model is very expensive from a computational point of view and has only been implemented into the 2D version of the GCE at the present time. The model is tested by studying the evolution of deep cloud systems in the west Pacific warm pool region and in the mid-latitude using identical thermodynamic conditions but with different concentrations of CCN: a low "clean" concentration and a high "dirty" concentration. Besides the initial differences in aerosol concentration, preliminary results indicate that the low CCN concentration case produces rainfall at the surface sooner than the high CCN case but has less cloud water mass aloft. Because the spectral-bim model explicitly calculates and allows for the examination of both the mass and number concentration of cpecies in each size category, a detailed analysis of the instantaneous size spectrum can be obtained for the two cases. It is shown that since the low CCN case produces fever droplets, larger size develop due to greater condencational and collectional growth, leading to a broader size spectrum in comparison to the high CCN case.

Tao, Wei-Kuo↗

On the Effect of Dust Particles on Global Cloud Condensation Nuclei and Cloud Droplet Number

Aerosol-cloud interaction studies to date consider aerosol with a substantial fraction of soluble material as the sole source of cloud condensation nuclei (CCN). Emerging evidence suggests that mineral dust can act as good CCN through water adsorption onto the surface of particles. This study provides a first assessment of the contribution of insoluble dust to global CCN and cloud droplet number concentration (CDNC). Simulations are carried out with the NASA Global Modeling Initiative chemical transport model with an online aerosol simulation, considering emissions from fossil fuel, biomass burning, marine, and dust sources. CDNC is calculated online and explicitly considers the competition of soluble and insoluble CCN for water vapor. The predicted annual average contribution of insoluble mineral dust to CCN and CDNC in cloud-forming areas is up to 40 and 23.8%, respectively. Sensitivity tests suggest that uncertainties in dust size distribution and water adsorption parameters modulate the contribution of mineral dust to CDNC by 23 and 56%, respectively. Coating of dust by hygroscopic salts during the atmospheric aging causes a twofold enhancement of the dust contribution to CCN; the aged dust, however, can substantially deplete in-cloud supersaturation during the initial stages of cloud formation and can eventually reduce CDNC. Considering the hydrophilicity from adsorption and hygroscopicity from solute is required to comprehensively capture the dust-warm cloud interactions. The framework presented here addresses this need and can be easily integrated in atmospheric models.

Karydis, V. A.↗

Dimethylsulfide/cloud condensation nuclei/climate system - Relevant size-resolved measurements of the chemical and physical properties of atmospheric aerosol particles

The mass and number relationships occurring within the atmospheric dimethylsulfide/cloud condensation nuclei (CCN)/climate system, using simultaneous measurements of particulate phase mass size distributions of nss SO4(2-), methanesulfonic acid (MSA), and NH4(+); number size distributions of particles having diameters between 0.02 and 9.6 microns; CCN concentrations at a supersaturation of 0.3 percent; relative humidity; and temperature, obtained for the northeastern Pacific Ocean in April and May 1991. Based on these measurements, particulate nss SO4(2-), MSA, and NH4(+) mass appeared to be correlated with both particle effective surface area and number in the accumulation mode size range (0.16 to 0.5 micron). No correlations were found in the size range below 0.16 micron. A correlation was also found between nss SO4(2-) mass and the CCN number concentration, such that a doubling of the SO4(2-) mass corresponded to a 40 percent increase in the CCN number concentration. However, no correlation was found between MSA mass and CCN concentration.

Quinn, P. K.↗

A Balloon-Borne Cloud Condensation Nuclei Counter

A balloon-borne instrument was constructed for observations of vertical profiles of cloud condensation nucleus (CCN) concentrations, active at 1% supersaturation. Droplet concentration in the static thermal-gradient diffusion chamber is deduced from the amount of scattered laser light detected by a photodetector. The photodetector is calibrated using a video camera and computer system to count the number of droplets produced from NaCl aerosol. Preliminary data are available from nine early morning profiles obtained at Laramie, Wyoming, between June 1995 and January 1997. To complement the CCN measurements, instruments that measure condensation nuclei (CN) and aerosols with diameter greater than 0.30 micrometers (D(sub 0.3) were also included on the balloon package. CCN concentrations exhibited a general decrease from the surface to the top of the boundary layers, were generally uniform through well-mixed layers, and show variability above well-mixed layers. In general, the structure of the CCN profile appears to be closely related to the structure in the CN and D(sub 0.3) profiles. Summer profiles generally have CCN concentration greater than 200/cu cm up to 500 mbar, whereas winter profiles are less than 200/cu cm at all levels.

Delene, David J.↗

Radiative Importance of Aerosol-Cloud Interaction

Aerosol particles are input into the troposphere by biomass burning, among other sources. These aerosol palls cover large expanses of the earth's surface. Aerosols may directly scatter solar radiation back to space, thus increasing the earth's albedo and act to cool the earth's surface and atmosphere. Aerosols also contribute to the earth's energy balance indirectly. Hygroscopic aerosol act as cloud condensation nuclei (CCN) and thus affects cloud properties. In 1977, Twomey theorized that additional available CCN would create smaller but more numerous cloud droplets in a cloud with a given amount of liquid water. This in turn would increase the cloud albedo which would scatter additional radiation back to space and create a similar cooling pattern as the direct aerosol effect. Estimates of the magnitude of the aerosol indirect effect on a global scale range from 0.0 to -4.8 W/sq m. Thus the indirect effect can be of comparable magnitude and opposite in sign to the estimates of global greenhouse gas forcing Aerosol-cloud interaction is not a one-way process. Just as aerosols have an influence on clouds through the cloud microphysics, clouds have an influence on aerosols. Cloud droplets are solutions of liquid water and CCN, now dissolved. When the cloud droplet evaporates it leaves behind an aerosol particle. This new particle does not have to have the same properties as the original CCN. In fact, studies show that aerosol particles that result from cloud processing are larger in size than the original CCN. Optical properties of aerosol particles are dependent on the size of the particles. Larger particles have a smaller backscattering fraction, and thus less incoming solar radiation will be backscattered to space if the aerosol particles are larger. Therefore, we see that aerosols and clouds modify each other to influence the radiative balance of the earth. Understanding and quantifying the spatial and seasonal patterns of the aerosol indirect forcing may have even greater consequences. Presently we know that through the use of fossil fuel and land-use changes we have increased the concentration of greenhouse gases in the atmosphere. In parallel, we have seen a modest increase of global temperature in the last century. These two observations have been linked as cause and effect by climate models, but this connection is still experimentally not verified. The spatial and seasonal distribution of aerosol forcing is different from that of greenhouse gases, thus generating a different spatial fingerprint of climate change. This fingerprint was suggested as a method to identify the response of the climate system to anthropogenic forcing of greenhouse gases and aerosol. The aerosol fingerprint may be the only way to firmly establish the presence (or absence) of human impact on climate. Aerosol-cloud interaction through the indirect effect will be an important component of establishing this fingerprint.

Tsay, Si-Chee↗

Cloud Condensation Nuclei in Fire-3

The centerpiece of this research was the cloud condensation nuclei (CCN) measurements of the Desert Research Institute (DRI) CCN spectrometers on board the NCAR C-130 aircraft during the Arctic Cloud Experiment (ACE) in May, 1998. These instruments operated successfully throughout all eight 10-hour research flights based in Fairbanks and the two ferry flights between Colorado and Fairbanks. Within a few months of completion of ACE the CCN data was edited and put into the archives. A paper was completed and published on the CCN climatology during the previous two FIRE field projects-FIRE 1 based in San Diego in June and July, 1987 and ASTEX based in the Azores Islands in June, 1992. This showed distinct contrasts in concentrations and spectra between continental and maritime CCN concentrations, which depended on air mass trajectories. Pollution episodes from Europe had distinct influences on particle concentrations at low altitudes especially within the boundary layer. At higher altitudes concentrations were similar in the two air mass regimes. Cloudier atmospheres showed lower concentrations especially below the clouds, which were a result mostly of coalescence scavenging.

Source record↗

Cloud Condensation Nuclei Measurements in Tropical Cyclones

The first measurements of cloud condensation nuclei (CCN) within and around tropical cyclones were made with the Desert Research Institute (DRI) CCN spectrometer (Hudson 1909) from a NOAA P-3 Hurricane Hunter aircraft throughout the 2001 season. Two penetrations of the closed eye of Hurricane Erin off the northeast US coast on Sept. 10 showed concentrations consistently well in excess of 1000 per cubic cm at approximately 1.4% supersaturation. Simultaneous condensation nuclei (CN--total particle) concentrations were consistently well in excess of 2000 per cubic cm throughout these closed eye penetrations. These within eye measurements at 4 km altitude for exceeded CCN and CN measurements just outside of the storm at similar altitudes--300 and 600 per cubic cm respectively. These CCN and CN concentrations within this closed eye were far above concentrations in maritime air masses; they are characteristic of continental or polluted air masses. Although there was a possibility that Saharan duct may have gotten into this storm these sub tenth micrometer particles are much too small and much too numerous to be dust. Such high concentrations may have originated from European air pollution, which may have been transported by similar airflow patterns to those that carry Saharan dust across the Atlantic. These high concentrations may be a manifestation of descending air that brings higher concentrations that are often characteristic of the upper troposphere (Clarke and Kapustin 2002). Later in the month measurements in Humberto showed highly variable CCN and CN concentrations that ranged from lots than 5 per cubic cm to more than 1000 per Cubic cm over km scale distances within and around the open eye of this tropical storm/hurricane. These very low concentrations suggest strong cloud scavenging.

Hudson, J. G.↗

The Role of Atmospheric Aerosol Concentration on Deep Convective Precipitation: Cloud-Resolving Model Simulations

Aerosols and especially their effect on clouds are one of the key components of the climate system and the hydrological cycle [Ramanathan et al., 2001]. Yet, the aerosol effect on clouds remains largely unknown and the processes involved not well understood. A recent report published by the National Academy of Science states "The greatest uncertainty about the aerosol climate forcing - indeed, the largest of all the uncertainties about global climate forcing - is probably the indirect effect of aerosols on clouds NRC [2001]." The aerosol effect on Clouds is often categorized into the traditional "first indirect (i.e., Twomey)" effect on the cloud droplet sizes for a constant liquid water path and the "semi-direct" effect on cloud coverage. The aerosol effect on precipitation processes, also known as the second type of aerosol indirect effect, is even more complex, especially for mixed-phase convective clouds. In this paper, a cloud-resolving model (CRM) with detailed spectral-bin microphysics was used to examine the effect of aerosols on three different deep convective cloud systems that developed in different geographic locations: South Florida, Oklahoma and the Central Pacific, In all three cases, rain reaches the ground earlier for the low CCN (clean) case. Rain suppression is also evident in all three cases with high CCN (dirty) case. However, this suppression only occurs during the first hour of the simulations. During the mature stages of the simulations, the effects of increasing aerosol concentration range from rain suppression in the Oklahoma case, to almost no effect in the Florida case, to rain enhancement in the Pacific case. These results show the complexity of aerosol interactions with convection. The model results suggest that evaporative cooling is a key process in determining whether high CCN reduces or enhances precipitation. Stronger evaporative cooling can produce a stronger cold pool and thus stronger low-level convergence through interactions with the low-level wind shear. Consequently, precipitation processes can be more vigorous. For example,, the evaporative cooling is more than two times stronger in the lower troposphere with high CCN for the Pacific case. Sensitivity tests also suggest that ice processes are crucial for suppressing precipitation in the Oklahoma case with high CCN.

Tao, Wei-Kuo↗

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↗

A Large Source of Cloud Condensation Nuclei from New Particle Formation in the Tropics

Cloud condensation nuclei (CCN) can affect cloud properties and therefore the Earth’s radiative balance. New particle formation (NPF) from condensable vapours in the free troposphere has been suggested to contribute to CCN, especially in remote, pristine atmospheric regions, but direct evidence is sparse, and the magnitude of this contribution is uncertain. Here we use in-situ aircraft measurements of vertical profiles of aerosol size distributions to present a global-scale survey of NPF occurrence. We observed intense NPF occurring at high altitude in tropical convective regions over both the Pacific and Atlantic Oceans. Together with the results of chemical-transport models, our findings indicate that NPF persists at all longitudes as a global-scale band in the tropical upper troposphere, covering about 40% of the Earth’s surface. Furthermore, we find that this NPF in the tropical upper troposphere is a globally important source of CCN in the lower troposphere, where they can affect cloud properties. Our findings suggest that the production of CCN, as these new particles descend towards the surface, is currently not adequately captured in global models, because they tend to underestimate both the magnitude of tropical upper tropospheric NPF and the subsequent growth to CCN sizes. This has potential implications for cloud albedo and the global radiative balance.

Atmospheric chemistry↗

Measurements of cloud nuclei in the effluents from launches of liquid- and solid-fueled rockets

Airborne measurements of two types of cloud nuclei, cloud condensation nuclei (CCN) and ice nuclei (IN), were conducted in the stabilized ground clouds which resulted from the launches of a liquid-fueled ATLAS/Centaur rocket and a solid-fueled TITAN III rocket. Results show that the concentrations of CCN in both types of clouds were greater than ambient values for the 2 hours duration of the measurements. The initial production of CCN active at 0.5% supersaturation in the ATLAS and TITAN clouds was found to be equivalent to a 20 and 700 sec emission, respectively, by the city of Denver, Colorado. After the initial production, the clouds continued to generate CCN at a rate of about 1/cu cm sec. However, concentrations of IN in the ATLAS cloud were greater than ambient values for only a short period after launch, and it appears that the nuclei resulted from entrained launch pad and ground debris. The concentrations of IN in the TITAN cloud were found to be at or below ambient levels until about 2 hours after launch when they increased substantially above ambient values.

Hindman, E. E.↗