Aerosol-cloud interactions in global models of indirect aerosol radiative forcing

The sensitivity of cloud optical properties with respect to parameters that affect aerosol activation is examined. Of particular interest are the effect of volatile gases (such as HNO3), slightly soluble and surfactant species. An adiabatic parcel model is used to simulate cloud droplet formation. Cloud optical properties are calculated from these simulations

Understanding Aerosol-Cloud-Climate Interactions

2009 program of the “Open Forum on Energy and the Environment”, presented on April 2, 2009, from 4:30 PM-5:30 PM in room L1255, Ford Environmental Science & Technology Building (ES&T) on the Georgia Tech campus.The Impact of CO₂ on Global Climate ChangeRuntime: 60:51 minute

Continued development of the ISORROPIA aerosol thermodynamic equilibrium model

Issued as final reportUnited States. Dept. of Commerc

Global Distribution of Cloud Droplet Number Concentration, Autoconversion Rate, and Aerosol Indirect Effect Under Diabatic Droplet Activation

This study presents a global assessment of the sensitivity of droplet number to diabatic activation (i.e., including effects from entrainment of dry air) and its first-order tendency on indirect forcing and autoconversion. Simulations were carried out with the NASA Global Modeling Initiative (GMI) atmospheric and transport model using climatological metereorological fields derived from the former NASA Data Assimilation Office (DAO), the NASA Finite volume GCM (FVGCM) and the Goddard Institute for Space Studies version II (GISS) GCM. Cloud droplet number concentration (CDNC) is calculated using a physically based prognostic parameterization that explicitly includes entrainment effects on droplet formation. Diabatic activation results in lower CDNC, compared to adiabatic treatment of the process. The largest decrease in CDNC (by up to 75 percent) was found in the tropics and in zones of moderate CCN concentration. This leads to a global mean effective radius increase between 0.2-0.5 micrometers (up to 3.5 micrometers over the tropics), a global mean autoconversion rate increase by a factor of 1.1 to 1.7 (up to a factor of 4 in the tropics), and a 0.2-0.4 W m(exp -2) decrease in indirect forcing. The spatial patterns of entrainment effects on droplet activation tend to reduce biases in effective radius (particularly in the tropics) when compared to satellite retrievals. Considering the diabatic nature of ambient clouds, entrainment effects on CDNC need to be considered in GCM studies of the aerosol indirect effect

Changes in dissolved iron deposition to the oceans driven by human activity: a 3-D global modelling study

The global atmospheric iron (Fe) cycle is parameterized in the global 3-D chemical transport model TM4-ECPL to simulate the proton- and the organic ligand-promoted mineral-Fe dissolution as well as the aqueous-phase photochemical reactions between the oxidative states of Fe (III/II). Primary emissions of total (TFe) and dissolved (DFe) Fe associated with dust and combustion processes are also taken into account, with TFe mineral emissions calculated to amount to ~ 35 Tg-Fe yr−1 and TFe emissions from combustion sources of ~ 2 Tg-Fe yr−1. The model reasonably simulates the available Fe observations, supporting the reliability of the results of this study. Proton- and organic ligand-promoted Fe dissolution in present-day TM4-ECPL simulations is calculated to be ~ 0.175 Tg-Fe yr−1, approximately half of the calculated total primary DFe emissions from mineral and combustion sources in the model (~ 0.322 Tg-Fe yr−1). The atmospheric burden of DFe is calculated to be ~ 0.024 Tg-Fe. DFe deposition presents strong spatial and temporal variability with an annual flux of ~ 0.496 Tg-Fe yr−1, from which about 40 % (~ 0.191 Tg-Fe yr−1) is deposited over the ocean. The impact of air quality on Fe deposition is studied by performing sensitivity simulations using preindustrial (year 1850), present (year 2008) and future (year 2100) emission scenarios. These simulations indicate that about a 3 times increase in Fe dissolution may have occurred in the past 150 years due to increasing anthropogenic emissions and thus atmospheric acidity. Air-quality regulations of anthropogenic emissions are projected to decrease atmospheric acidity in the near future, reducing to about half the dust-Fe dissolution relative to the present day. The organic ligand contribution to Fe dissolution shows an inverse relationship to the atmospheric acidity, thus its importance has decreased since the preindustrial period but is projected to increase in the future. The calculated changes also show that the atmospheric DFe supply to the globe has more than doubled since the preindustrial period due to 8-fold increases in the primary non-dust emissions and about a 3-fold increase in the dust-Fe dissolution flux. However, in the future the DFe deposition flux is expected to decrease (by about 25 %) due to reductions in the primary non-dust emissions (about 15 %) and in the dust-Fe dissolution flux (about 55 %). The present level of atmospheric deposition of DFe over the global ocean is calculated to be about 3 times higher than for 1850 emissions, and about a 30 % decrease is projected for 2100 emissions. These changes are expected to impact most on the high-nutrient–low-chlorophyll oceanic regions

Ice multiplication from ice-ice collisions in the high Arctic: Sensitivity to ice habit, rimed fraction, ice type and uncertainties in the numerical description of the process

Atmospheric models often fail to correctly reproduce the microphysical structure of Arctic mixed-phase clouds and underpredict ice water content even when the simulations are constrained by observed levels of ice nucleating particles. In this study we investigate whether ice multiplication from breakup upon ice-ice collisions, a process missing in most models, can account for the observed cloud ice in a stratocumulus cloud observed during the Arctic Summer Cloud Ocean Study (ASCOS) campaign. Our results indicate that the efficiency of this process in these conditions is weak; increases in fragment generation are compensated for by subsequent enhancement of precipitation and subcloud sublimation. Activation of collisional breakup improves the representation of cloud ice content, but cloud liquid remains overestimated. In most sensitivity simulations, variations in ice habit and prescribed rimed fraction have little effect on the results. A few simulations result in explosive multiplication and cloud dissipation; however, in most setups, the overall multiplication effects become substantially weaker if the precipitation sink is enhanced through cloud-ice-to-snow autoconversion. The largest uncertainty stems from the correction factor for ice enhancement due to sublimation included in the breakup parameterization; excluding this correction results in rapid glaciation, especially in simulations with plates. Our results indicate that the lack of a detailed treatment of ice habit and rimed fraction in most bulk microphysics schemes is not detrimental for the description of the collisional breakup process in the examined conditions as long as cloud-ice-to-snow autoconversion is considered

Importance of composition and hygroscopicity of BC particles to the effect of BC mitigation on cloud properties: Application to California conditions

Black carbon (BC) has many effects on climate including the direct effect on atmospheric absorption, indirect and semi-direct effects on clouds, snow effects, and others. While most of these are positive (warming), the first indirect effect is negative and quantifying its magnitude in addition to other BC feedbacks is important for supporting policies that mitigate BC. We use the detailed aerosol chemistry parcel model of Russell and Seinfeld (1998), observationally constrained by initial measured aerosol concentrations from five California sites, to provide simulated cloud drop number (CDN) concentrations against which two GCM calculations – one run at the global scale and one nested from the global-to-regional scale are compared. The GCM results reflect the combined effects of their emission inventories, advection schemes, and cloud parameterizations. BC-type particles contributed between 16 and 20% of cloud droplets at all sites even in the presence of more hygroscopic particles. While this chemically detailed parcel model result is based on simplified cloud dynamics and does not consider semi-direct or cloud absorption effects, the cloud drop number concentrations are similar to the simulations of both Chen et al. (2010b) and Jacobson (2010) for the average cloud conditions in California. Reducing BC particle concentration by 50% decreased the cloud droplet concentration by between 6% and 9% resulting in the formation of fewer, larger cloud droplets that correspond to a lower cloud albedo. This trend is similar to Chen et al. (2010b) and Jacobson (2010) when BC particles were modeled as hygroscopic. This reduction in CDN in California due to the decrease in activated BC particles supports the concern raised by Chen et al. (2010a) that the cloud albedo effect of BC particles has a cooling effect that partially offsets the direct forcing reduction if other warming effects of BC on clouds are unchanged. These results suggests that for regions like the California sites studied here, where BC mitigation targets fossil fuel sources, a critical aspect of the modeled reduction is the chemical composition and associated hygroscopicity of the BC particles removed as well as their relative contribution to the atmospheric particle concentrations

Bioavailable atmospheric phosphorous supply to the global ocean: a 3-D global modeling study

The atmospheric cycle of phosphorus (P) is parameterized here in a state-of-the-art global 3-D chemistry transport model, taking into account primary emissions of total P (TP) and soluble P (DP) associated with mineral dust, combustion particles from natural and anthropogenic sources, bioaerosols, sea spray and volcanic aerosols. For the present day, global TP emissions are calculated to be roughly 1.33 Tg-P yr−1, with the mineral sources contributing more than 80 % to these emissions. The P solubilization from mineral dust under acidic atmospheric conditions is also parameterized in the model and is calculated to contribute about one-third (0.14 Tg-P yr−1) of the global DP atmospheric source. To our knowledge, a unique aspect of our global study is the explicit modeling of the evolution of phosphorus speciation in the atmosphere. The simulated present-day global annual DP deposition flux is 0.45 Tg-P yr−1 (about 40 % over oceans), showing a strong spatial and temporal variability. Present-day simulations of atmospheric P aerosol concentrations and deposition fluxes are satisfactory compared with available observations, indicating however an underestimate of about 70 % on current knowledge of the sources that drive the P atmospheric cycle. Sensitivity simulations using preindustrial (year 1850) anthropogenic and biomass burning emission scenarios showed a present-day increase of 75 % in the P solubilization flux from mineral dust, i.e., the rate at which P is converted into soluble forms, compared to preindustrial times, due to increasing atmospheric acidity over the last 150 years. Future reductions in air pollutants due to the implementation of air-quality regulations are expected to decrease the P solubilization flux from mineral dust by about 30 % in the year 2100 compared to the present day. Considering, however, that all the P contained in bioaerosols is readily available for uptake by marine organisms, and also accounting for all other DP sources, a total bioavailable P flux of about 0.17 Tg-P yr−1 to the oceans is derived. Our calculations further show that in some regions more than half of the bioavailable P deposition flux to the ocean can originate from biological particles, while this contribution is found to maximize in summer when atmospheric deposition impact on the marine ecosystem is the highest due to ocean stratification. Thus, according to this global study, a largely unknown but potentially important role of terrestrial bioaerosols as suppliers of bioavailable P to the global ocean is also revealed. Overall, this work provides new insights to the atmospheric P cycle by demonstrating that biological materials are important carriers of bioavailable P, with very important implications for past and future responses of marine ecosystems to global change