Atmospheric Chemistry General Circulation Model Research Articles

Sensitivities of atmospheric composition and climate to altitude and latitude of hypersonic aircraft emissions

Abstract. Hydrogen-powered hypersonic aircraft are designed to travel in the middle stratosphere at approximately 30–40 km. These aircraft can have a considerable impact on climate-relevant species like stratospheric water vapor, ozone, and methane and thus would contribute to climate warming. The impact of hypersonic aircraft emissions on atmospheric composition and, in turn, on radiation fluxes differs strongly depending on cruise altitude. However, in contrast to variations in the altitude of emission, differences from variations in the latitude of emission are currently unknown. Using an atmospheric chemistry general circulation model, we show that a variation in the latitude of emission can have a larger effect on perturbations and stratospheric-adjusted radiative forcing than a variation in the altitude of emission. Our results include the individual impacts of water vapor and nitrogen oxide emissions, as well as unburned hydrogen, on middle-atmospheric water vapor, ozone, and methane and the resulting radiative forcing. Water vapor perturbation lifetime continues the known tropospheric increase with altitude and reaches almost 6 years in the middle stratosphere. Our results demonstrate how atmospheric composition changes caused by emissions of hypersonic aircraft are controlled by large-scale processes like the Brewer–Dobson circulation and, depending on the latitude of emission, local phenomena like polar stratospheric clouds. The analysis includes a model evaluation of ozone and water vapor with satellite data and a novel approach to reduce simulated years by one-third. A prospect for future hypersonic research is the analysis of seasonal sensitivities and simulations with emissions from combustion of liquefied natural gas instead of liquid hydrogen.

What controls ozone sensitivity in the upper tropical troposphere?

Abstract. Ozone is an important contributor to the radiative energy budget of the upper troposphere (UT). Therefore, observing and understanding the processes contributing to ozone production are important for monitoring the progression of climate change. Nitrogen oxides (NOx ≡ NO + NO2) and volatile organic compounds (VOCs) are two main tropospheric precursors to ozone formation. Depending on their abundances, ozone production can be sensitive to changes in either of these two precursors. Here, we focus on processes contributing to ozone chemistry in the upper tropical troposphere between 30∘ S and 30∘ N latitude, where changes in ozone have a relatively large impact on anthropogenic radiative forcing. Based on modeled trace gas mixing ratios and meteorological parameters simulated by the ECHAM5/MESSy2 Atmospheric Chemistry (EMAC) general circulation model, we analyze a variety of commonly applied metrics including ozone production rates (P(O3)), the formaldehyde (HCHO) to NO2 ratio and the share of methyl peroxy radicals (CH3O2) forming HCHO (α(CH3O2)) for their ability to describe the chemical regime. We show that the distribution of trace gases in the tropical UT is strongly influenced by the varying locations of deep convection throughout the year, and we observe peak values for NOx and P(O3) over the continental areas of South America and Africa where lightning is frequent. We find that P(O3) and its response to NO is unsuitable for determining the dominant regime in the upper troposphere. Instead, α(CH3O2) and the HCHO/NO2 ratio in combination with ambient NO levels perform well as metrics to indicate whether NOx or VOC sensitivity is prevalent. We show that effectively only the knowledge of the availability of NO and HO2 is required to adequately represent O3 precursors and its sensitivity towards them. A sensitivity study with halving, doubling and excluding lightning NOx demonstrates that lightning and its distribution in the tropics are the major determinants of the chemical regimes and ozone formation in the upper tropical troposphere.

The effect of ash, water vapor, and heterogeneous chemistry on the evolution of a Pinatubo-size volcanic cloud

Abstract. We employ the ECHAM5/MESSy2 atmospheric chemistry general circulation model (EMAC) that incorporates calculations of gas-phase and heterogeneous chemistry coupled with the ozone cycle and aerosol formation, transport, and microphysics to calculate the 1991 Pinatubo volcanic cloud. We considered simultaneous injections of SO2, volcanic ash, and water vapor. We conducted multiple ensemble simulations with different injection configurations to test the evolution of SO2, SO42-, ash masses, stratospheric aerosol optical depth, surface area density (SAD), and the stratospheric temperature response against available observations. We found that the volcanic cloud evolution is sensitive to the altitude where volcanic debris is initially injected and the initial concentrations of the eruption products that affect radiative heating and lofting of the volcanic cloud. The numerical experiments with the injection of 12 Mt SO2, 75 Mt of volcanic ash, and 150 Mt of water vapor at 20 km show the best agreement with the observation aerosol optical depth and stratospheric temperature response. Volcanic water injected by eruptive jet and/or intruding through the tropopause accelerates SO2 oxidation. But the mass of volcanic water retained in the stratosphere is controlled by the stratospheric temperature at the injection level. For example, if volcanic materials are released in the cold point above the tropical tropopause, most of the injected water freezes and sediments as ice crystals. The water vapor directly injected into the volcanic cloud increases the SO42- mass and stratospheric aerosol optical depth by about 5 %. The coarse ash comprises 98 % of the ash injected mass. It sediments within a few days, but aged submicron ash could stay in the stratosphere for a few months providing SAD for heterogeneous chemistry. The presence of ash accelerates the SO2 oxidation by 10 %–20 % due to heterogeneous chemistry, radiative heating, lofting, and faster dispersion of volcanic debris. Ash aging affects its lifetime and optical properties, almost doubling the ash radiative heating. The 2.5-year simulations show that the stratospheric temperature anomalies forced by radiative heating of volcanic debris in our experiments with the 20 km injection height agree well with observations and reanalysis data. This indicates that the model captures the long-term evolution and climate effect of the Pinatubo volcanic cloud. The volcanic cloud's initial lofting, facilitated by ash particles' radiative heating, controls the oxidation rate of SO2. Ash accelerates the formation of the sulfate layer in the first 2 months after the eruption. We also found that the interactive calculations of OH and heterogeneous chemistry increase the volcanic cloud sensitivity to water vapor and ash injections. All those factors must be accounted for in modeling the impact of large-scale volcanic injections on climate and stratospheric chemistry.

Modelling mineral dust emissions and atmospheric dispersion with MADE3 in EMAC v2.54

Abstract. It was hypothesized that using mineral dust emission climatologies in global chemistry climate models (GCCMs), i.e. prescribed monthly-mean dust emissions representative of a specific year, may lead to misrepresentations of strong dust burst events. This could result in a negative bias of model dust concentrations compared to observations for these episodes. Here, we apply the aerosol microphysics submodel MADE3 (Modal Aerosol Dynamics model for Europe, adapted for global applications, third generation) as part of the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model. We employ two different representations of mineral dust emissions for our model simulations: (i) a prescribed monthly-mean climatology of dust emissions representative of the year 2000 and (ii) an online dust parametrization which calculates wind-driven mineral dust emissions at every model time step. We evaluate model results for these two dust representations by comparison with observations of aerosol optical depth from ground-based station data. The model results show a better agreement with the observations for strong dust burst events when using the online dust representation compared to the prescribed dust emissions setup. Furthermore, we analyse the effect of increasing the vertical and horizontal model resolution on the mineral dust properties in our model. We compare results from simulations with T42L31 and T63L31 model resolution (2.8∘×2.8∘ and 1.9∘×1.9∘ in latitude and longitude, respectively; 31 vertical levels) with the reference setup (T42L19). The different model versions are evaluated against airborne in situ measurements performed during the SALTRACE mineral dust campaign (Saharan Aerosol Long-range Transport and Aerosol-Cloud Interaction Experiment, June–July 2013), i.e. observations of dust transported from the Sahara to the Caribbean. Results show that an increased horizontal and vertical model resolution is able to better represent the spatial distribution of airborne mineral dust, especially in the upper troposphere (above 400 hPa). Additionally, we analyse the effect of varying assumptions for the size distribution of emitted dust but find only a weak sensitivity concerning these changes. The results of this study will help to identify the model setup best suited for future studies and to further improve the representation of mineral dust particles in EMAC-MADE3.

Development of the global atmospheric chemistry general circulation model BCC-GEOS-Chem v1.0: model description and evaluation

Abstract. Chemistry plays an indispensable role in investigations of the atmosphere; however, many climate models either ignore or greatly simplify atmospheric chemistry, limiting both their accuracy and their scope. We present the development and evaluation of the online global atmospheric chemical model BCC-GEOS-Chem v1.0, coupling the GEOS-Chem chemical transport model (CTM) as an atmospheric chemistry component in the Beijing Climate Center atmospheric general circulation model (BCC-AGCM). The GEOS-Chem atmospheric chemistry component includes detailed tropospheric HOx–NOx–volatile organic compounds–ozone–bromine–aerosol chemistry and online dry and wet deposition schemes. We then demonstrate the new capabilities of BCC-GEOS-Chem v1.0 relative to the base BCC-AGCM model through a 3-year (2012–2014) simulation with anthropogenic emissions from the Community Emissions Data System (CEDS) used in the Coupled Model Intercomparison Project Phase 6 (CMIP6). The model captures well the spatial distributions and seasonal variations in tropospheric ozone, with seasonal mean biases of 0.4–2.2 ppbv at 700–400 hPa compared to satellite observations and within 10 ppbv at the surface to 500 hPa compared to global ozonesonde observations. The model has larger high-ozone biases over the tropics which we attribute to an overestimate of ozone chemical production. It underestimates ozone in the upper troposphere which is likely due either to the use of a simplified stratospheric ozone scheme or to biases in estimated stratosphere–troposphere exchange dynamics. The model diagnoses the global tropospheric ozone burden, OH concentration, and methane chemical lifetime to be 336 Tg, 1.16×106 molecule cm−3, and 8.3 years, respectively, which is consistent with recent multimodel assessments. The spatiotemporal distributions of NO2, CO, SO2, CH2O, and aerosol optical depth are generally in agreement with satellite observations. The development of BCC-GEOS-Chem v1.0 represents an important step for the development of fully coupled earth system models (ESMs) in China.

A modeling study of the regional representativeness of surface ozone variation at the WMO/GAW background stations in China

Abstract Six World Meteorological Organization (WMO)/Global Atmosphere Watch (GAW) stations are located at background sites in China, which constitute a network for monitoring surface ozone, including its long-term temporal variation. In this study, we evaluated the seasonal variation in surface ozone simulated by the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model with the measurements made at these WMO/GAW background stations for the period of 2010–2012, and investigated the regional representativeness of each station with respect to the seasonal variation in surface ozone. We determined the contributions of ozone originating from various tropospheric and stratospheric latitude bands based on EMAC simulations using a tagged tracer approach. The results showed that the predominant contribution to surface ozone was from the troposphere in northern middle-high and tropical latitudes. For each station there was a large surrounding area in which the yearly ozone maximum occurred in the same month as it did at the station, reflecting the regional characteristics of the seasonal variation in surface ozone recorded at the WMO/GAW background stations. Surface ozone in China was found to generally peak in summer over non-monsoon and mid-latitude monsoon regions and in spring over low-latitude monsoon regions, indicating that the regional representativeness of ozone variability in China is significantly influenced by the Asian summer monsoon.

Net ozone production and its relationship to nitrogen oxides and volatile organic compounds in the marine boundary layer around the Arabian Peninsula

Abstract. Strongly enhanced tropospheric ozone (O3) mixing ratios have been reported in the Arabian Basin, a region with intense solar radiation and high concentrations of O3 precursors such as nitrogen oxides (NOx) and volatile organic compounds (VOCs). To analyze photochemical O3 production in the marine boundary layer (MBL) around the Arabian Peninsula, we use shipborne observations of NO, NO2, O3, OH, HO2, HCHO, the actinic flux, water vapor, pressure and temperature obtained during the summer 2017 Air Quality and Climate in the Arabian Basin (AQABA) campaign, and we compare them to simulation results from the ECHAM-MESSy Atmospheric Chemistry (EMAC) general circulation model. Net O3 production rates (NOPRs) were greatest over both the Gulf of Oman and the northern Red Sea (16 ppbv d−1) and over the Arabian Gulf (32 ppbv d−1). The NOPR over the Mediterranean, the southern Red Sea and the Arabian Sea did not significantly deviate from zero; however, the results for the Arabian Sea indicated weak net O3 production of 5 ppbv d−1 as well as net O3 destruction over the Mediterranean and the southern Red Sea with values of −1 and −4 ppbv d−1, respectively. Constrained by HCHO∕NO2 ratios, our photochemistry calculations show that net O3 production in the MBL around the Arabian Peninsula mostly occurs in NOx-limited regimes with a significant share of O3 production occurring in the transition regime between NOx limitation and VOC limitation over the Mediterranean and more significantly over the northern Red Sea and Oman Gulf.

Global aerosol modeling with MADE3 (v3.0) in EMAC (based on v2.53): model description and evaluation

Abstract. Recently, the aerosol microphysics submodel MADE3 (Modal Aerosol Dynamics model for Europe, adapted for global applications, third generation) was introduced as a successor to MADE and MADE-in. It includes nine aerosol species and nine lognormal modes to represent aerosol particles of three different mixing states throughout the aerosol size spectrum. Here, we describe the implementation of the most recent version of MADE3 into the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model, including a detailed evaluation of a 10-year aerosol simulation with MADE3 as part of EMAC. We compare simulation output to station network measurements of near-surface aerosol component mass concentrations, to airborne measurements of aerosol mass mixing ratio and number concentration vertical profiles, to ground-based and airborne measurements of particle size distributions, and to station network and satellite measurements of aerosol optical depth. Furthermore, we describe and apply a new evaluation method, which allows a comparison of model output to size-resolved electron microscopy measurements of particle composition. Although there are indications that fine-mode particle deposition may be underestimated by the model, we obtained satisfactory agreement with the observations. Remaining deviations are of similar size to those identified in other global aerosol model studies. Thus, MADE3 can be considered ready for application within EMAC. Due to its detailed representation of aerosol mixing state, it is especially useful for simulating wet and dry removal of aerosol particles, aerosol-induced formation of cloud droplets and ice crystals as well as aerosol–radiation interactions. Besides studies on these fundamental processes, we also plan to use MADE3 for a reassessment of the climate effects of anthropogenic aerosol perturbations.

Atmospheric chemistry, sources and sinks of carbon suboxide, C<sub>3</sub>O<sub>2</sub>

Abstract. Carbon suboxide, O = C = C = C = O, has been detected in ambient air samples and has the potential to be a noxious pollutant and oxidant precursor; however, its lifetime and fate in the atmosphere are largely unknown. In this work, we collect an extensive set of studies on the atmospheric chemistry of C3O2. Rate coefficients for the reactions of C3O2 with OH radicals and ozone were determined as kOH = (2.6 ± 0.5) × 10−12 cm3 molecule−1 s−1 at 295 K (independent of pressure between ∼ 25 and 1000 mbar) and kO3 < 1.5 × 10−21 cm3 molecule−1 s−1 at 295 K. A theoretical study on the mechanisms of these reactions indicates that the sole products are CO and CO2, as observed experimentally. The UV absorption spectrum and the interaction of C3O2 with water (Henry's law solubility and hydrolysis rate constant) were also investigated, enabling its photodissociation lifetime and hydrolysis rates, respectively, to be assessed. The role of C3O2 in the atmosphere was examined using in situ measurements, an analysis of the atmospheric sources and sinks and simulation with the EMAC atmospheric chemistry–general circulation model. The results indicate sub-pptv levels at the Earth's surface, up to about 10 pptv in regions with relatively strong sources, e.g. influenced by biomass burning, and a mean lifetime of ∼ 3.2 days. These predictions carry considerable uncertainty, as more measurement data are needed to determine ambient concentrations and constrain the source strengths.

Influence of long-period oscillations on the development of droughts in Northern Eurasia

Estimates of the influence of the Atlantic long-period oscillation (ALO) on the formation of droughts in Northern Eurasia were obtained using the results of numerical experiments with the ECHAM5 atmospheric chemistry general circulation model and the mixed layer ocean model. In general, the model results are consistent with the empirical estimates.

Global atmospheric budget of simple monocyclic aromatic compounds

Abstract. The global atmospheric budget and distribution of monocyclic aromatic compounds is estimated, using an atmospheric chemistry general circulation model. Simulation results are evaluated with an ensemble of surface and aircraft observations with the goal of understanding emission, production and removal of these compounds.Anthropogenic emissions provided by the RCP database represent the largest source of aromatics in the model (≃ 23 TgC year−1) and biomass burning from the GFAS inventory the second largest (≃ 5 TgC year−1). The simulated chemical production of aromatics accounts for ≃ 5 TgC year−1. The atmospheric burden of aromatics sums up to 0.3 TgC. The main removal process of aromatics is photochemical decomposition (≃ 27 TgC year−1), while wet and dry deposition are responsible for a removal of ≃ 4 TgC year−1.Simulated mixing ratios at the surface and elsewhere in the troposphere show good spatial and temporal agreement with the observations for benzene, although the model generally underestimates mixing ratios. Toluene is generally well reproduced by the model at the surface, but mixing ratios in the free troposphere are underestimated. Finally, larger discrepancies are found for xylenes: surface mixing ratios are not only overestimated but also a low temporal correlation is found with respect to in situ observations.

Stratospheric sulfur and its implications for radiative forcing simulated by the chemistry climate model EMAC.

Multiyear simulations with the atmospheric chemistry general circulation model EMAC with a microphysical modal aerosol module at high vertical resolution demonstrate that the sulfur gases COS and SO2, the latter from low-latitude and midlatitude volcanic eruptions, predominantly control the formation of stratospheric aerosol. Marine dimethyl sulfide (DMS) and other SO2 sources, including strong anthropogenic emissions in China, are found to play a minor role except in the lowermost stratosphere. Estimates of volcanic SO2 emissions are based on satellite observations using Total Ozone Mapping Spectrometer and Ozone Monitoring Instrument for total injected mass and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat or Stratospheric Aerosol and Gases Experiment for the spatial distribution. The 10 year SO2 and COS data set of MIPAS is also used for model evaluation. The calculated radiative forcing of stratospheric background aerosol including sulfate from COS and small contributions by DMS oxidation, and organic aerosol from biomass burning, is about 0.07W/m2. For stratospheric sulfate aerosol from medium and small volcanic eruptions between 2005 and 2011 a global radiative forcing up to 0.2W/m2 is calculated, moderating climate warming, while for the major Pinatubo eruption the simulated forcing reaches 5W/m2, leading to temporary climate cooling. The Pinatubo simulation demonstrates the importance of radiative feedback on dynamics, e.g., enhanced tropical upwelling, for large volcanic eruptions.

Atmospheric Dispersion of Radioactivity from Nuclear Power Plant Accidents: Global Assessment and Case Study for the Eastern Mediterranean and Middle East

We estimate the contamination risks from the atmospheric dispersion of radionuclides released by severe nuclear power plant accidents using the ECHAM/Modular Earth Submodel System (MESSy) atmospheric chemistry (EMAC) atmospheric chemistry-general circulation model at high resolution (50 km). We present an overview of global risks and also a case study of nuclear power plants that are currently under construction, planned and proposed in the Eastern Mediterranean and Middle East, a region prone to earthquakes. We implemented continuous emissions from each location, making the simplifying assumption that all potential accidents release the same amount of radioactivity. We simulated atmospheric transport and decay, focusing on 137Cs and 131I as proxies for particulate and gaseous radionuclides, respectively. We present risk maps for potential surface layer concentrations, deposition and doses to humans from the inhalation exposure of 131I. The estimated risks exhibit seasonal variability, with the highest surface level concentrations of gaseous radionuclides in the Northern Hemisphere during winter.

Model-simulated trend of surface carbon monoxide for the 2001–2010 decade

Abstract. We present decadal trend estimates of surface carbon monoxide (CO) simulated using the atmospheric chemistry general circulation model ECHAM5/MESSy (EMAC; ECHAM5 and MESSy stand for fifth-generation European Centre Hamburg general circulation model and Modular Earth Submodel System, respectively) based on the emission scenarios Representative Concentration Pathways (RCP) 8.5 for anthropogenic activity and Global Fire Emissions Database (GFED) v3.1 for biomass burning from 2001 through 2010. The spatial distribution of the modeled surface CO is evaluated with monthly data from the Measurements Of Pollution In The Troposphere (MOPITT) thermal infrared product. The global means of correlation coefficient and relative bias for the decade 2001–2010 are 0.95 and −4.29%, respectively. We also find a reasonable correlation (R = 0.78) between the trends of EMAC surface CO and full 10-year monthly records from ground-based observation (World Data Centre for Greenhouse Gases, WDCGG). Over western Europe, eastern USA, and northern Australia, the significant decreases in EMAC surface CO are estimated at −35.5 ± 5.8, −59.6 ± 9.1, and −13.7 ± 9.5 ppbv decade−1, respectively. In contrast, the surface CO increases by +8.9 ± 4.8 ppbv decade−1 over southern Asia. A high correlation (R = 0.92) between the changes in EMAC-simulated surface CO and total emission flux shows that the significant regional trends are attributed to the changes in primary and direct emissions from both anthropogenic activity and biomass burning.

Global risk from the atmospheric dispersion of radionuclides by nuclear power plant accidents in the coming decades

Abstract. We estimate the global risk from the release and atmospheric dispersion of radionuclides from nuclear power plant accidents using the EMAC atmospheric chemistry–general circulation model. We included all nuclear reactors that are currently operational, under construction and planned or proposed. We implemented constant continuous emissions from each location in the model and simulated atmospheric transport and removal via dry and wet deposition processes over 20 years (2010–2030), driven by boundary conditions based on the IPCC A2 future emissions scenario. We present global overall and seasonal risk maps for potential surface layer concentrations and ground deposition of radionuclides, and estimate potential doses to humans from inhalation and ground-deposition exposures to radionuclides. We find that the risk of harmful doses due to inhalation is typically highest in the Northern Hemisphere during boreal winter, due to relatively shallow boundary layer development and limited mixing. Based on the continued operation of the current nuclear power plants, we calculate that the risk of radioactive contamination to the citizens of the USA will remain to be highest worldwide, followed by India and France. By including stations under construction and those that are planned and proposed, our results suggest that the risk will become highest in China, followed by India and the USA.

Modeled global effects of airborne desert dust on air quality and premature mortality

Abstract. Fine particulate matter is one of the most important factors contributing to air pollution. Epidemiological studies have related increased levels of atmospheric particulate matter to premature human mortality caused by cardiopulmonary disease and lung cancer. However, a limited number of investigations have focused on the contribution of airborne desert dust particles. Here we assess the effects of dust particles with an aerodynamic diameter smaller than 2.5 μm (DU2.5) on human mortality for the year 2005. We used the EMAC atmospheric–chemistry general circulation model at high resolution to simulate global atmospheric dust concentrations. We applied a health impact function to estimate premature mortality for the global population of 30 yr and older, using parameters from epidemiological studies. We estimate a global cardiopulmonary mortality of about 402 000 in 2005. The associated years of life lost are about 3.47 million per year. We estimate the global fraction of the cardiopulmonary deaths caused by atmospheric desert dust to be about 1.8%, though in the 20 countries most affected by dust this is much higher, about 15–50%. These countries are primarily found in the so-called "dust belt" from North Africa across the Middle East and South Asia to East Asia

Aerosol pollution potential from major population centers

Abstract. Major population centers (MPCs), or megacities, represent the largest of growing urban agglomerations with major societal and environmental implications. In terms of air quality, they are seen as localized but strong emission sources of aerosols and trace gases which in turn affect air pollution levels in the city or in downwind regions. In the state-of-the-art atmospheric chemistry general circulation model EMAC, generic aerosol and gas-phase tracers with equal emission source strengths at 46 MPC locations are used to study the balance between local pollution build-up and pollution export, either vertically into the upper troposphere or horizontally in the lower troposphere. The insoluble gas-phase tracers with fixed lifetimes are transported with the atmospheric circulation, while the aerosol tracers also undergo gravitational sedimentation as well as dry and wet deposition processes. The strength of low-level tracer export depends on the location of the emission source and prevailing meteorology, in particular on atmospheric stability and the height of the boundary layer and the mixing out of this layer. In contrast, vertical transport of tracer mass depends on the tracer's solubility: the more soluble a tracer is, the less mass reaches altitudes above five kilometers. Hence, the mass of insoluble gas-phase tracer above five kilometers can be up to ten times higher than the hydrophilic aerosol mass from the same source. In the case of aerosol tracers, pollution build-up around the source is determined by meteorological factors which have only indirect effects on tracer lifetime, like surface wind, boundary layer height, and turbulent mixing, as well as those which affect the lifetime of the tracers such as precipitation. The longer a tracer stays in the atmosphere, the lower is the relative importance of the location of the source to the atmospheric mass, and thus the lower is the relative local pollution build-up. We further use aerosol deposition fields to estimate regions with high deposition, that is more than 1% or more than 5% of the corresponding tracer emission deposited in this region. In doing so, we find that the high deposition areas are larger for aerosols with diameters of 10.0 μm, and these differ less between the MPCs than for aerosols with diameters smaller than 2.5 μm due to faster deposition. Furthermore, cities in regions with high precipitation rates or unfavorable geographic locations, e.g., in a basin, suffer most of this high deposition. Most of the high deposition occurs over land, although about 50% of the MPCs are located along coastlines. By folding the aerosol deposition fields with geographical distributions of cropland, pasture, and forest, the impact on different land ecosystems is assessed. In general, forest is exposed most to deposition from MPCs while pastureland is least affected. Moreover, the impact on humans, measured with a threshold exceedance of pollutant surface mixing ratios, is more dependent on population densities than on the size of the area with a certain mixing ratio.

Parameterization of dust emissions in the global atmospheric chemistry-climate model EMAC: impact of nudging and soil properties

Abstract. Airborne desert dust influences radiative transfer, atmospheric chemistry and dynamics, as well as nutrient transport and deposition. It directly and indirectly affects climate on regional and global scales. Two versions of a parameterization scheme to compute desert dust emissions are incorporated into the atmospheric chemistry general circulation model EMAC (ECHAM5/MESSy2.41 Atmospheric Chemistry). One uses a globally uniform soil particle size distribution, whereas the other explicitly accounts for different soil textures worldwide. We have tested these two versions and investigated the sensitivity to input parameters, using remote sensing data from the Aerosol Robotic Network (AERONET) and dust concentrations and deposition measurements from the AeroCom dust benchmark database (and others). The two versions are shown to produce similar atmospheric dust loads in the N-African region, while they deviate in the Asian, Middle Eastern and S-American regions. The dust outflow from Africa over the Atlantic Ocean is accurately simulated by both schemes, in magnitude, location and seasonality. Approximately 70% of the modelled annual deposition data and 70–75% of the modelled monthly aerosol optical depth (AOD) in the Atlantic Ocean stations lay in the range 0.5 to 2 times the observations for all simulations. The two versions have similar performance, even though the total annual source differs by ~50%, which underscores the importance of transport and deposition processes (being the same for both versions). Even though the explicit soil particle size distribution is considered more realistic, the simpler scheme appears to perform better in several locations. This paper discusses the differences between the two versions of the dust emission scheme, focusing on their limitations and strengths in describing the global dust cycle and suggests possible future improvements.

Effects of business-as-usual anthropogenic emissions on air quality

Abstract. The atmospheric chemistry general circulation model EMAC has been used to estimate the impact of anthropogenic emission changes on global and regional air quality in recent and future years (2005, 2010, 2025 and 2050). The emission scenario assumes that population and economic growth largely determine energy and food consumption and consequent pollution sources with the current technologies ("business as usual"). This scenario is chosen to show the effects of not implementing legislation to prevent additional climate change and growing air pollution, other than what is in place for the base year 2005, representing a pessimistic (but plausible) future. By comparing with recent observations, it is shown that the model reproduces the main features of regional air pollution distributions though with some imprecisions inherent to the coarse horizontal resolution (~100 km) and simplified bottom-up emission input. To identify possible future hot spots of poor air quality, a multi pollutant index (MPI), suited for global model output, has been applied. It appears that East and South Asia and the Middle East represent such hotspots due to very high pollutant concentrations, while a general increase of MPIs is observed in all populated regions in the Northern Hemisphere. In East Asia a range of pollutant gases and fine particulate matter (PM2.5) is projected to reach very high levels from 2005 onward, while in South Asia air pollution, including ozone, will grow rapidly towards the middle of the century. Around the Persian Gulf, where natural PM2.5 concentrations are already high (desert dust), ozone levels are expected to increase strongly. The population weighted MPI (PW-MPI), which combines demographic and pollutant concentration projections, shows that a rapidly increasing number of people worldwide will experience reduced air quality during the first half of the 21st century. Following this business as usual scenario, it is projected that air quality for the global average citizen in 2050 would be almost comparable to that for the average citizen in East Asia in the year 2005, which underscores the need to pursue emission reductions.

The 1-way on-line coupled atmospheric chemistry model system MECO(n) – Part 1: Description of the limited-area atmospheric chemistry model COSMO/MESSy

Abstract. The numerical weather prediction model of the Consortium for Small Scale Modelling (COSMO), maintained by the German weather service (DWD), is connected with the Modular Earth Submodel System (MESSy). This effort is undertaken in preparation of a new, limited-area atmospheric chemistry model. Limited-area models require lateral boundary conditions for all prognostic variables. Therefore the quality of a regional chemistry model is expected to improve, if boundary conditions for the chemical constituents are provided by the driving model in consistence with the meteorological boundary conditions. The new developed model is as consistent as possible, with respect to atmospheric chemistry and related processes, with a previously developed global atmospheric chemistry general circulation model: the ECHAM/MESSy Atmospheric Chemistry (EMAC) model. The combined system constitutes a new research tool, bridging the global to the meso-γ scale for atmospheric chemistry research. MESSy provides the infrastructure and includes, among others, the process and diagnostic submodels for atmospheric chemistry simulations. Furthermore, MESSy is highly flexible allowing model setups with tailor made complexity, depending on the scientific question. Here, the connection of the MESSy infrastructure to the COSMO model is documented and also the code changes required for the generalisation of regular MESSy submodels. Moreover, previously published prototype submodels for simplified tracer studies are generalised to be plugged-in and used in the global and the limited-area model. They are used to evaluate the TRACER interface implementation in the new COSMO/MESSy model system and the tracer transport characteristics, an important prerequisite for future atmospheric chemistry applications. A supplementary document with further details on the technical implementation of the MESSy interface into COSMO with a complete list of modifications to the COSMO code is provided.