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Aerosol activation and cloud processing in the global aerosol-climate model ECHAM5-HAM  [PDF]
G. J. Roelofs,P. Stier,J. Feichter,E. Vignati
Atmospheric Chemistry and Physics Discussions , 2006,
Abstract: A parameterization for cloud processing is presented that calculates activation of aerosol particles to cloud drops, cloud drop size, and pH-dependent aqueous phase sulfur chemistry. The parameterization is implemented in the global aerosol-climate model ECHAM5-HAM. The cloud processing parameterization uses updraft speed, temperature, and aerosol size and chemical parameters simulated by ECHAM5-HAM to estimate the maximum supersaturation at the cloud base, and subsequently the cloud drop number concentration (CDNC) due to activation. In-cloud sulfate production occurs through oxidation of dissolved SO2 by ozone and hydrogen peroxide. The model simulates realistic distributions for annually averaged CDNC although it is underestimated especially in remote marine regions. On average, CDNC is dominated by particles from the accumulation mode, with smaller contributions from the Aitken and coarse modes. The simulations indicate that in-cloud sulfate production is a potentially important source of accumulation mode sized cloud condensation nuclei, due to chemical growth of activated Aitken particles and to enhanced coalescence of processed particles. The strength of this source depends on the distribution of produced sulfate over the activated modes. This distribution is affected by uncertainties in many parameters that play a direct role in particle activation, such as the updraft velocity, the aerosol chemical composition and the organic solubility, and the simulated CDNC is found to be relatively sensitive to these uncertainties.
Constraints on interactions between aerosols and clouds on a global scale from a combination of MODIS-CERES satellite data and climate simulations
X. Ma, K. von Salzen,J. Cole
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2010,
Abstract: Satellite-based cloud top effective radius retrieved by the CERES Science Team were combined with simulated aerosol concentrations from CCCma CanAM4 to examine relationships between aerosol and cloud that underlie the first aerosol indirect (cloud albedo) effect. Evidence of a strong negative relationship between sulphate, and organic aerosols, with cloud top effective radius was found for low clouds, indicating both aerosol types are contributing to the first indirect effect on a global scale. Furthermore, effects of aerosol on the cloud droplet effective radius are more pronounced for larger cloud liquid water paths. While CanAM4 broadly reproduces the observed relationship between sulphate aerosols and cloud droplets, it does not reproduce the dependency of cloud top droplet size on organic aerosol concentrations nor the dependency on cloud liquid water path. Simulations with a modified version of the model yield a more realistic dependency of cloud droplets on organic carbon. The robustness of the methods used in the study are investigated by repeating the analysis using aerosol simulated by the GOCART model and cloud top effective radii derived from the MODIS Science Team.
Global model simulations of the impact of ocean-going ships on aerosols, clouds, and the radiation budget  [PDF]
A. Lauer,V. Eyring,J. Hendricks,P. J?ckel
Atmospheric Chemistry and Physics Discussions , 2007,
Abstract: International shipping contributes significantly to the fuel consumption of all transport related activities. Specific emissions of pollutants such as sulfur dioxide (SO2) per kg of fuel emitted are higher than for road transport or aviation. Besides gaseous pollutants, ships also emit various types of particulate matter. The aerosol impacts the Earth's radiation budget directly by scattering and absorbing incoming solar radiation and indirectly by changing cloud properties. Here we use ECHAM5/MESSy1-MADE, a global climate model with detailed aerosol and cloud microphysics, to show that emissions from ships significantly increase the cloud droplet number concentration of low maritime water clouds. Whereas the cloud liquid water content remains nearly unchanged in these simulations, effective radii of cloud droplets decrease, leading to cloud optical thickness increase up to 5–10%. The sensitivity of the results is estimated by using three different emission inventories for present day conditions. The sensitivity analysis reveals that shipping contributes with 2.3% to 3.6% to the total sulfate burden and 0.4% to 1.4% to the total black carbon burden in the year 2000. In addition to changes in aerosol chemical composition, shipping increases the aerosol number concentration, e.g. up to 25% in the size range of the accumulation mode (typically >0.1 μm) over the Atlantic. The total aerosol optical thickness over the Indian Ocean, the Gulf of Mexico and the Northeastern Pacific increases up to 8–10% depending on the emission inventory. Changes in aerosol optical thickness caused by the shipping induced modification of aerosol particle number concentration and chemical composition lead to a change of the net top of the atmosphere (ToA) clear sky radiation of about 0.013 W/m2 to 0.036 W/m2 on global annual average. The estimated all-sky direct aerosol effect calculated from these changes ranges between 0.009 W/m2 and 0.014 W/m2. The indirect aerosol effect of ships on climate is found to be far larger than previously estimated. An indirect radiative effect of 0.19 W/m2 to 0.6 W/m2 (change of the top of the atmosphere shortwave radiative flux) is calculated here, contributing 17% to 39% to the total indirect effect of anthropogenic aerosols. This contribution is high because ship emissions are released in regions with frequent low marine clouds in an otherwise clean environment. In addition, the potential impact of particulate matter on the radiation budget is larger over the dark ocean surface than over polluted regions over land.
Simulating aerosol microphysics with the ECHAM/MADE GCM – Part I: Model description and comparison with observations
A. Lauer, J. Hendricks, I. Ackermann, B. Schell, H. Hass,S. Metzger
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2005,
Abstract: The aerosol dynamics module MADE has been coupled to the general circulation model ECHAM4 to simulate the chemical composition, number concentration, and size distribution of the global submicrometer aerosol. The present publication describes the new model system ECHAM4/MADE and presents model results in comparison with observations. The new model is able to simulate the full life cycle of particulate matter and various gaseous particle precursors including emissions of primary particles and trace gases, advection, convection, diffusion, coagulation, condensation, nucleation of sulfuric acid vapor, aerosol chemistry, cloud processing, and size-dependent dry and wet deposition. Aerosol components considered are sulfate (SO4), ammonium (NH4), nitrate (NO3), black carbon (BC), particulate organic matter (POM), sea salt, mineral dust, and aerosol liquid water. The model is numerically efficient enough to allow long term simulations, which is an essential requirement for application in general circulation models. Since the current study is focusing on the submicrometer aerosol, a coarse mode is not being simulated. The model is run in a passive mode, i.e. no feedbacks between the MADE aerosols and clouds or radiation are considered yet. This allows the investigation of the effect of aerosol dynamics, not interfered by feedbacks of the altered aerosols on clouds, radiation, and on the model dynamics. In order to evaluate the results obtained with this new model system, calculated mass concentrations, particle number concentrations, and size distributions are compared to observations. The intercomparison shows, that ECHAM4/MADE is able to reproduce the major features of the geographical patterns, seasonal cycle, and vertical distributions of the basic aerosol parameters. In particular, the model performs well under polluted continental conditions in the northern hemispheric lower and middle troposphere. However, in comparatively clean remote areas, e.g. in the upper troposphere or in the southern hemispheric marine boundary layer, the current model version tends to underestimate particle number concentrations. Final Revised Paper (PDF, 1829 KB) Discussion Paper (ACPD) Citation: Lauer, A., Hendricks, J., Ackermann, I., Schell, B., Hass, H., and Metzger, S.: Simulating aerosol microphysics with the ECHAM/MADE GCM – Part I: Model description and comparison with observations, Atmos. Chem. Phys., 5, 3251-3276, doi:10.5194/acp-5-3251-2005, 2005. Bibtex EndNote Reference Manager XML
Aerosol activation and cloud processing in the global aerosol-climate model ECHAM5-HAM
G. J. Roelofs, P. Stier, J. Feichter, E. Vignati,J. Wilson
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2006,
Abstract: A parameterization for cloud processing is presented that calculates activation of aerosol particles to cloud drops, cloud drop size, and pH-dependent aqueous phase sulfur chemistry. The parameterization is implemented in the global aerosol-climate model ECHAM5-HAM. The cloud processing parameterization uses updraft speed, temperature, and aerosol size and chemical parameters simulated by ECHAM5-HAM to estimate the maximum supersaturation at the cloud base, and subsequently the cloud drop number concentration (CDNC) due to activation. In-cloud sulfate production occurs through oxidation of dissolved SO2 by ozone and hydrogen peroxide. The model simulates realistic distributions for annually averaged CDNC although it is underestimated especially in remote marine regions. On average, CDNC is dominated by cloud droplets growing on particles from the accumulation mode, with smaller contributions from the Aitken and coarse modes. The simulations indicate that in-cloud sulfate production is a potentially important source of accumulation mode sized cloud condensation nuclei, due to chemical growth of activated Aitken particles and to enhanced coalescence of processed particles. The strength of this source depends on the distribution of produced sulfate over the activated modes. This distribution is affected by uncertainties in many parameters that play a direct role in particle activation, such as the updraft velocity, the aerosol chemical composition and the organic solubility, and the simulated CDNC is found to be relatively sensitive to these uncertainties.
Global model simulations of the impact of ocean-going ships on aerosols, clouds, and the radiation budget  [PDF]
A. Lauer,V. Eyring,J. Hendricks,P. J?ckel
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2007,
Abstract: International shipping contributes significantly to the fuel consumption of all transport related activities. Specific emissions of pollutants such as sulfur dioxide (SO2) per kg of fuel emitted are higher than for road transport or aviation. Besides gaseous pollutants, ships also emit various types of particulate matter. The aerosol impacts the Earth's radiation budget directly by scattering and absorbing the solar and thermal radiation and indirectly by changing cloud properties. Here we use ECHAM5/MESSy1-MADE, a global climate model with detailed aerosol and cloud microphysics to study the climate impacts of international shipping. The simulations show that emissions from ships significantly increase the cloud droplet number concentration of low marine water clouds by up to 5% to 30% depending on the ship emission inventory and the geographic region. Whereas the cloud liquid water content remains nearly unchanged in these simulations, effective radii of cloud droplets decrease, leading to cloud optical thickness increase of up to 5–10%. The sensitivity of the results is estimated by using three different emission inventories for present-day conditions. The sensitivity analysis reveals that shipping contributes to 2.3% to 3.6% of the total sulfate burden and 0.4% to 1.4% to the total black carbon burden in the year 2000 on the global mean. In addition to changes in aerosol chemical composition, shipping increases the aerosol number concentration, e.g. up to 25% in the size range of the accumulation mode (typically >0.1 μm) over the Atlantic. The total aerosol optical thickness over the Indian Ocean, the Gulf of Mexico and the Northeastern Pacific increases by up to 8–10% depending on the emission inventory. Changes in aerosol optical thickness caused by shipping induced modification of aerosol particle number concentration and chemical composition lead to a change in the shortwave radiation budget at the top of the atmosphere (ToA) under clear-sky condition of about 0.014 W/m2 to 0.038 W/m2 for a global annual average. The corresponding all-sky direct aerosol forcing ranges between 0.011 W/m2 and 0.013 W/m2. The indirect aerosol effect of ships on climate is found to be far larger than previously estimated. An indirect radiative effect of 0.19 W/m2 to 0.60 W/m2 (a change in the atmospheric shortwave radiative flux at ToA) is calculated here, contributing 17% to 39% of the total indirect effect of anthropogenic aerosols. This contribution is high because ship emissions are released in regions with frequent low marine clouds in an otherwise clean
Multi-satellite aerosol observations in the vicinity of clouds
T. Várnai, A. Marshak,W. Yang
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2013,
Abstract: Improved characterization of aerosol properties in the vicinity of clouds is important for better understanding two critical aspects of climate: aerosol–cloud interactions and the direct radiative effect of aerosols. Satellite measurements have provided important insights into aerosol properties near clouds, but also suggested that the observations can be affected by 3-D radiative processes and instrument blurring not considered in current data interpretation methods. This study examines systematic cloud-related changes in particle properties and radiation fields that influence satellite measurements of aerosols in the vicinity of low-level maritime clouds. For this, the paper presents a statistical analysis of a yearlong global dataset of co-located MODIS and CALIOP observations and theoretical simulations. The results reveal that CALIOP-observed aerosol particle size and optical thickness, and MODIS-observed solar reflectance increase systematically in a wide transition zone around clouds. It is estimated that near-cloud changes in particle populations – including both aerosols and undetected cloud particles – are responsible for roughly two thirds of the observed increase in 0.55 μm MODIS reflectance. The results also indicate that 3-D radiative processes significantly contribute to near-cloud reflectance enhancements, while instrument blurring contributes significantly only within 1 km from clouds and then quickly diminishes with distance from clouds.
Multi-satellite aerosol observations in the vicinity of clouds  [PDF]
T. Várnai,A. Marshak,W. Yang
Atmospheric Chemistry and Physics Discussions , 2012, DOI: 10.5194/acpd-12-32039-2012
Abstract: Improved characterization of aerosol properties in the vicinity of clouds is important for better understanding two critical aspects of climate: aerosol-cloud interactions and the direct radiative effect of aerosols. Satellite measurements have provided important insights into aerosol properties near clouds, but also suggested that the observations can be affected by 3-D radiative processes and instrument blurring not considered in current data interpretation methods. This study examines systematic changes in particle properties and radiation fields that influence satellite measurements of aerosols in the vicinity of clouds. For this, the paper presents a statistical analysis of a yearlong global dataset of co-located MODIS and CALIOP observations and theoretical simulations. The results reveal that CALIOP-observed aerosol particle size and optical thickness, and MODIS-observed solar reflectance increase systematically in a wide transition zone around clouds. It is estimated that near-cloud changes in particle populations – including both aerosols and undetected cloud particles – are responsible for roughly two thirds of the observed increase in 0.55 μm MODIS reflectance. The results also indicate that 3-D radiative processes significantly contribute to near-cloud reflectance enhancements, while instrument blurring does not.
Global anthropogenic aerosol effects on convective clouds in ECHAM5-HAM  [PDF]
U. Lohmann
Atmospheric Chemistry and Physics Discussions , 2007,
Abstract: Aerosols affect the climate system by changing cloud characteristics in many ways. They act as cloud condensation and ice nuclei and may have an influence on the hydrological cycle. Here we investigate aerosol effects on convective clouds by extending the double moment cloud microphysics scheme developed for stratiform clouds to convective clouds in the ECHAM5 general circulation model. This increases the liquid water path in the tropics and reduces the sensitivity of the liquid water path with increasing aerosol optical depth in better agreement with observations and large-eddy simulation studies. In simulations in which greenhouse gases and aerosols emissions are increased since pre-industrial times, accounting for microphysics in convective clouds matches most closely the observed increase in precipitation. The total anthropogenic aerosol effect since pre-industrial time is slightly reduced from 1.6 to 1.9 W m 2 when microphysics are only included in stratiform clouds to 1.5 W m 2 when microphysics are included both in stratiform and convective clouds.
Global indirect aerosol effects: a review
U. Lohmann,J. Feichter
Atmospheric Chemistry and Physics (ACP) & Discussions (ACPD) , 2005,
Abstract: Aerosols affect the climate system by changing cloud characteristics in many ways. They act as cloud condensation and ice nuclei, they may inhibit freezing and they could have an influence on the hydrological cycle. While the cloud albedo enhancement (Twomey effect) of warm clouds received most attention so far and traditionally is the only indirect aerosol forcing considered in transient climate simulations, here we discuss the multitude of effects. Different approaches how the climatic implications of these aerosol effects can be estimated globally as well as improvements that are needed in global climate models in order to better represent indirect aerosol effects are discussed in this paper.
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