Trace gas and aerosol interactions in the fully coupled model of aerosol-chemistry-climate ECHAM5-HAMMOZ: 1. Model description and insights from the spring 2001 TRACE-P experiment

In this paper, we introduce the ECHAM5-HAMMOZ aerosol- chemistry-climate model that includes fully interactive simulations of Ox-NOx-hydrocarbons chemistry and of aerosol microphysics (including prognostic size distribution and mixing state of aerosols) implemented in the General Circulation Model ECHAM5. The photolysis rates used in the gas chemistry account for aerosol and cloud distributions and a comprehensive set of heterogeneous reactions is implemented. The model is evaluated with trace gas and aerosol observations provided by the TRACE-P aircraft experiment. Sulfate concentrations are well captured but black carbon concentrations are underestimated. The number concentrations, surface areas, and optical properties are reproduced fairly well near the surface but underestimated in the upper troposphere. CO concentrations are well reproduced in general while ${O}_{3}$ concentrations are overestimated by 10-20 ppbv. We find that heterogeneous chemistry significantly influences the regional and global distributions of a number of key trace gases. Heterogeneous reactions reduce the ozone surface concentrations by 18-23% over the TRACE-P region and the global annual mean ${O}_{3}$ burden by 7%. The annual global mean OH concentration decreases by 10% inducing a 7% increase in the global CO burden. Annual global mean ${HNO}_{3}$ surface concentration decreases by 15% because of heterogenous reaction on mineral dust. A comparison of our results to those from previous studies suggest that the choice of uptake coe±cients for a given species seems to be the critical parameter that determines the global impact of heterogeneous chemistry on a trace gas (rather than the description of aerosol properties and distributions). A prognostic description of the size distribution and mixing state of the aerosols is important, however, to account for the effect of heterogeneous chemistry on aerosols as further discussed in the second of this two-part series.

Chemistry and climate interactions

Luca Pozzoli

Atmospheric trace gases and aerosols and climate interact in many ways. A quantitative assessment of the influence of trace gases and aerosols on climate can only be achieved if the interactions and feedbacks among these three major components are accounted for. The goal of this thesis was to develop, evaluate and apply the ECHAM5-HAMMOZ chemistry-aerosol-climate model. The model includes fully interactive simulations of the NOx-Ox-hydrocarbons chemistry and of the aerosol chemistry and microphysics, the two simulations being embedded into the well established ECHAM5 climate model. In particular, on-line calculation of the photolysis rates (that accounts for aerosols and clouds) and heterogeneous reactions of trace gases on aerosols are accounted for in the model. In addition, the aerosol simulation provides a prognostic representation of the mixing state of the aerosol components, a feature that is particularly important to examine the effect of the SO2 uptake and subsequent sulfate formation on aerosols. A thorough model evaluation of the model was performed using observations from the Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft campaign. We also used ground based measurements from the European network EMEP (SO2 and sulfate), from the north American network IMPROVE (sulfate, black carbon and organic carbon), and from AERONET (aerosol optical depth). The coupled model is able to reproduce fairly well many of the observations over the TRACE-P region, even though some improvements are still needed. For example, we find a mean absolute bias of 20 ppbv (30%) and 40 ppbv (13%) for the simulated O3 and CO, respectively. Sulfate concentrations are represented fairly well, for all the regions considered, while SO2 is overestimated by a factor of 2 in general. Black carbon concentrations are underestimated over the TRACE-P region (mean absolute bias of 80%), most probably because of too low emissions, but well reproduced over north America. The aerosol optical depths compare well with observations at many sites in general, both in terms of annual means and seasonal variations. We show the results from a series of sensitivity simulations which goals are to assess the impact of heterogeneous reactions, photolysis reactions and sulfur chemistry on the regional and global trace gas distribution, and aerosol distribution, composition and optical properties. We found that heterogeneous reactions result in a reduction of 7% in the global O3 burden, and by up to 15% in surface O3 over regions rich in mineral dust. OH burden decreases by 10%, NO and NO2 by 20% and 29%, respectively while CO burden increases by 7%. Our numbers fall in general within the range of previous studies. We find that the effect of aerosols through the modifications of photolysis rates do not affect significantly the trace gas distributions and global burdens, while previous studies suggested larger effect. Heterogeneous reactions reduce the global mean SO2 surface concentration by 14%, while the global burden remains unchanged. This reflects the effect of competing processes. In particular, the depletion in SO2 by direct uptake on sea salt and dust is counterbalanced by the decrease in SO2 oxidation that is associated with the decrease in OH. The balance between the two competing effects differs depending on the regions (SO2 increases by more than +10% over north Africa and Indian Ocean and decreases by up to -20% at high latitudes). These processes, in turn, affect the sulfate formation. We find in general an increase (by up to 4%) in sulfate burden over the oceans because of sea salt uptake of SO2, and a decrease by up to 6% over Sahara and India, where SO2 increases. Our global burden of SO2 and sulfate amount to 0.77 and 0.87 (Tg(S)), respectively, which fall in the range of previous estimates. We find that SO2 uptake on sea salt contributes to the production of 3.69 Tg(S) yr-1 of sulfate (5% of total sulfate production) in good agreement with recent observation-based estimates. Uptake of SO2 on dust only contributes to the production of 0.55 Tg(S) yr-1 (< 1%) of sulfate, but it is an important process as it is responsible for the coating of mineral dust particles. A total of 300 Tg yr-1 of dust are transferred from the insoluble to the soluble mixed modes (56% of total emissions) because of this later process. The total burden of black carbon does not change significantly because of the heterogeneous reactions, but it is redistributed between insoluble/soluble modes. The changes in the mixing state of aerosols produce significant regional variations in aerosol optical depth and absorption. The aerosol optical depth and aerosol absorption increase by 10 to 30% and by 15%, respectively, during winter in the main polluted regions of the north hemisphere because of enhancing absorption efficiency of black carbon mixed with sulfate. On the contrary aerosol absorption decreases by up to 20% over the Atlantic ocean because of enhancing black carbon removal by wet scavenging. ECHAM5-HAMMOZ is a fully coupled model which includes many of the trace gas-aerosol and chemistry-climate interactions, and is thus a tool that allows an integrated assessment of the impact of the major short-life species that contribute to climate change and air quality.

EPFL2007

Trace gas and aerosol interactions in the fully coupled model of aerosol-chemistry-climate ECHAM5-HAMMOZ: 2. Impact of heterogeneous chemistry on the global aerosol distributions

Isabelle Bey, Luca Pozzoli

We use the ECHAM5-HAMMOZ aerosol-chemistry-climate model to quantify the influence of trace gas–aerosol interactions on the regional and global distributions and optical properties of aerosols for present-day conditions. The model includes fully interactive simulations of gas phase and aerosol chemistry including a comprehensive set of heterogeneous reactions. We find that as a whole, the heterogeneous reactions have only a small effect on the

{SO}_{2}

and sulfate burden because of competing effects. The uptake of

{SO}_{2}

on dust and sea salt decreases the

{SO}_{2}

concentrations while the decrease in OH (that results from the uptake of (

{HO}_{2}

{N}_{2}{O}_{5}

, and

{O}_{3}

) tends to increase

{SO}_{2}

(because of reduced oxidation). The sulfate formed in sea salt aerosols from

{SO}_{2}

uptake accounts for 3.7 Tg(S) a−1 (5%) of the total sulfate production. Uptake and subsequent reaction of SO2 on mineral dust contributes to a small formation of sulfate (0.55 Tg(S) a−1,

2008

Aerosol Transport and Distribution

Quentin Bourgeois

The fourth report of the Intergovernmental Panel of Climate Change (IPCC) unambiguously indicates that the climate is changing. Climate change is induced by changes in atmospheric abundances of greenhouse gases and aerosols, solar radiation and land surface properties, which all alter the radiative balance of the Earth. Among them, greenhouse gases and aerosols are likely the compounds affecting the climate the most. While greenhouse gases warm the Earth, aerosols influence its radiative balance by scattering and absorbing solar radiation (the direct effect), and by modifying cloud amount and properties (the indirect effect). The radiative forcing of aerosols on the climate is however the less understood among the various forcings currently considered in the IPCC assessment. This is likely related to the lack of comprehensive and accurate observations of aerosols (and in particular of their vertical distribution) which thus makes global aerosol models difficult to constrain. Recent model intercomparisons have indicated that different assumptions regarding aerosol emissions, formation and growing properties, and removal processes generate large diversities within models. These large diversities are found in particular in the Arctic and the upper troposphere region where extreme surrounding conditions take place, limiting instrument sensitivity and accuracy. The objectives of this thesis are to better quantify the processes driving the aerosol distribution in regions where the uncertainties are the largest, including the Arctic region and the upper troposphere, and to assess the quality of CALIOP observations. For this purpose, we used the fully coupled global climate-aerosol-chemistry ECHAM5-HAMMOZ model conjointly with a suite of remote sensing observations including the CALIOP satellite instrument, which provides the vertical distribution of aerosols. The model predicts the size distribution and composition of aerosols as well as the number concentration of cloud droplets and ice crystals. We first investigated the processes that drive the transport of soluble and insoluble compounds toward the Arctic in the ECHAM5-HAMMOZ model. Recognizing that scavenging processes may be an issue in global models, we "re-visited" their properties in ECHAM5-HAMMOZ. We find that the model better reproduces the aerosol vertical distribution in the northern mid- and high-latitudes, especially in the free troposphere, by decreasing aerosol scavenging coefficients in the model. Using smaller aerosol scavenging coefficients results in an increase of aerosol burden and lifetime, especially in the Arctic. In addition, the Arctic haze phenomenon is better represented in the simulation using decreased aerosol scavenging coefficients. The relative contributions of different processes governing the transport of aerosols from the midlatitudes toward the Arctic together with the relative contributions of different geopolitical source regions were then quantified. We find that Europe and Siberia contribute the most to the Arctic pollution even though Asian anthropogenic emissions are much larger. The model suggests that BC emitted in Siberia and Europe is ten times more efficiently deposited onto the Arctic than BC emitted in Asia. We next investigated an aerosol layer that forms in the vicinity of the tropical tropopause layer (TTL) over the southern Asian and Indian Ocean region. Aerosols in this layer are observed with the CALIOP instrument even though ice clouds partly mask their signal. The aerosol layer follows the Inter Tropical Convergence Zone (ITCZ), which indicates that these aerosols are likely transported during convective processes. The ECHAM5.5-HAM2 model reproduces such an aerosol layer in the TTL over the same region but clearly overestimates CALIOP data. Model results suggest that aerosols in this layer are mostly sulfate particles transported during convective processes and originating from natural sources. The shortwave forcing of this aerosol layer is estimated. Finally, we assessed the accuracy of aerosol extinction retrievals from the CALIOP satellite instrument by comparing them with remote sensing observations such as AERONET, MODIS and MISR over the last four years. Overall, standard CALIOP products underestimate by 50% observed aerosol extinctions. However, this comparison is substantially improved by screening CALIOP data. The comparison of the CALIOP screened product with the ECHAM5.5-HAM2 model shows large disparities in model results. The model reproduces quite well the observed interannual variability and vertical distribution of aerosols in Europe and North Africa while it underestimates them in America and Asia. This is likely due to an underestimate of dust and anthropogenic emissions in North America and Asia.

EPFL2012