Atmosphere-Ocean Ozone Exchange – A Global Modeling Study of Biogeochemical, Atmospheric and Water-Side Turbulence Dependencies

The significance of the removal of tropospheric ozone by the oceans, covering ~2/3 of the Earth's surface, has only been addressed in a few studies involving water tank, aircraft, and tower flux measurements. On the basis of results from these few observations of the ozone dry deposition velocity (VdO3), atmospheric chemistry models generally apply an empirical, constant ocean uptake rate of 0.05 cm s-1. This value is substantially smaller than the atmospheric turbulent transport velocity for ozone. On the other hand, the uptake is higher than expected from the solubility of ozone in clean water alone, suggesting that there is an enhancement in oceanic ozone uptake, e.g., through a chemical destruction mechanism. We present an evaluation of a global-scale analysis with a new mechanistic representation of atmosphere-ocean ozone exchange. The applied atmosphere chemistry-climate model includes not only atmospheric but also waterside turbulence and the role of waterside chemical loss processes as a function of oceanic biogeochemistry. The simulations suggest a larger role of biogeochemistry in tropical and subtropical ozone oceanic uptake with a relative small temporal variability, whereas in midlatitude and high-latitude regions, highly variable ozone uptake rates are expected because of the stronger influence of waterside turbulence. Despite a relatively large range in the explicitly calculated ocean uptake rate, there is a surprisingly small sensitivity of simulated Marine Boundary Layer ozone concentrations compared to the sensitivity for the commonly applied constant ocean uptake approach. This small sensitivity points at compensating effects through inclusion of the process-based ocean uptake mechanisms to consider variability in oceanic O3 deposition consistent with that in atmospheric and oceanic physical, chemical, and biological processe

The influence of the vertical distribution of emissions on tropospheric chemistry

The atmospheric chemistry general circulation model EMAC (ECHAM5/MESSy atmospheric chemistry) is used to investigate the effect of height dependent emissions on tropospheric chemistry. In a sensitivity simulation, anthropogenic and biomass burning emissions are released in the lowest model layer. The resulting tracer distributions are compared to those of a former simulation applying height dependent emissions. Although the differences between the two simulations in the free troposphere are small (less than 5%), large differences are present in polluted regions at the surface, in particular for NO<sub>x</sub> (more than 100%), CO (up to 30%) and non-methane hydrocarbons (up to 30%), whereas for OH the differences at the same locations are somewhat lower (15%). Global ozone formation is virtually unaffected by the choice of the vertical distribution of emissions. Nevertheless, local ozone changes can be up to 30%. Model results of both simulations are further compared to observations from field campaigns and to data from measurement stations

The Influence of the Vertical Distribution of Emissions on Tropospheric Chemistry

The atmospheric chemistry general circulation model EMAC (ECHAM5/MESSy atmospheric chemistry) is used to investigate the effect of height dependent emissions on tropospheric chemistry. In a sensitivity simulation, anthropogenic and biomass burning emissions are released in the lowest model layer. The resulting tracer distributions are compared to those of a former simulation applying height dependent emissions. Although the differences between the two simulations in the free troposphere are small (less than 5%), large differences are present in polluted regions at the surface, in particular for NOx (more than 100%), CO (up to 30%) and non-methane hydrocarbons (up to 30%), whereas for OH the differences at the same locations are somewhat lower (15%). Global ozone formation is virtually unaffected by the choice of the vertical distribution of emissions. Nevertheless, local ozone changes can be up to 30%. Model results of both simulations are further compared to observations from field campaigns and to data from measurement stations.JRC.H.2 - Climate chang

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

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 (DU_2.5) 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 Asi

Age-dependent health risk from ambient air pollution: a modelling and data analysis of childhood mortality in middle-income and low-income countries.

BACKGROUND: WHO estimates that, in 2015, nearly 1 million children younger than 5 years died from lower respiratory tract infections (LRIs). Ambient air pollution has a major impact on mortality from LRIs, especially in combination with undernutrition and inadequate health care. We aimed to estimate mortality due to ambient air pollution in 2015, particularly in children younger than 5 years, to investigate to what extent exposure to this risk factor affects life expectancy in different parts of the world. METHODS: Applying results from a recent atmospheric chemistry-general circulation model and health statistics from the WHO Global Health Observatory, combined in integrated exposure-response functions, we updated our estimates of mortality from ambient (outdoor) air pollution. We estimated excess deaths attributable to air pollution by disease category and age group, particularly those due to ambient air pollution-induced LRIs (AAP-LRIs) in childhood. Estimates are presented as excess mortality attributable to ambient air pollution and years of life lost (YLLs). To study recent developments, we calculated our estimates for the years 2010 and 2015. FINDINGS: Overall, 4·55 million deaths (95% CI 3·41 million to 5·56 million) were attributable to air pollution in 2015, of which 727 000 deaths (573 000-865 000) were due to AAP-LRIs. We estimated that AAP-LRIs caused about 237 000 (192 000-277 000) excess child deaths in 2015. Although childhood AAP-LRIs contributed about 5% of air pollution-attributable deaths worldwide, they accounted for 18% of losses in life expectancy, equivalent to 21·5 million (17 million to 25 million) of the total 122 million YLLs due to ambient air pollution in 2015. The mortality rate from ambient air pollution was highest in Asia, whereas the per capita YLLs were highest in Africa. We estimated that in sub-Saharan Africa, ambient air pollution reduces the average life expectancy of children by 4-5 years. In Asia, all-age mortality increased by about 10% between 2010 and 2015, whereas childhood mortality from AAP-LRIs declined by nearly 30% in the same period. INTERPRETATION: Most child deaths due to AAP-LRIs occur in low-income countries in Africa and Asia. A three-pronged strategy is needed to reduce the health effects of ambient air pollution in children: aggressive reduction of air pollution levels, improvements in nutrition, and enhanced treatment of air pollution-related health outcomes. FUNDING: None

Technical Note: An implementation of the dry removal processes DRY DEPosition and SEDImentation in the Modular Earth Submodel System (MESSy)

International audienceWe present the submodels DRYDEP and SEDI for the Modular Earth Submodel System (MESSy). Dry deposition of gases and aerosols is calculated within DRYDEP, whereas SEDI deals with aerosol particle sedimentation. Dry deposition velocities depend on the near-surface turbulence and the physical and chemical properties of the surface cover (e.g. the roughness length, soil pH or leaf stomatal exchange). The dry deposition algorithm used in DRYDEP is based on the big leaf approach and is described in detail within this Technical Note. The sedimentation submodel SEDI contains two sedimentation schemes: a simple upwind zeroth order scheme and a first order approach

Technical note: The MESSy-submodel AIRSEA calculating the air-sea exchange of chemical species

International audienceThe new submodel AIRSEA for the Modular Earth Submodel System (MESSy) is presented. It calculates the exchange of chemical species between the ocean and the atmosphere with a focus on organic compounds. The submodel can be easily extended to a large number of tracers, including highly soluble ones. It is demonstrated that application of explicitly calculated air-sea exchanges with AIRSEA can induce substantial changes in the simulated tracer distributions in the troposphere in comparison to a model version in which this process is neglected. For example, the simulations of acetone, constrained with measured oceanic concentrations, shows relative changes in the atmospheric surface layer mixing ratios over the Atlantic Ocean up to 300%

Technical Note: Coupling of chemical processes with the Modular Earth Submodel System (MESSy) submodel TRACER

International audienceThe implementation of processes related to chemistry into Earth System Models and their coupling within such systems requires the consistent description of the chemical species involved. We provide a tool (written in Fortran95) to structure and manage information about constituents, hereinafter referred to as tracers, namely the Modular Earth Submodel System (MESSy) generic (i.e., infrastructure) submodel TRACER. With TRACER it is possible to define a multitude of tracer sets, depending on the spatio-temporal representation (i.e., the grid structure) of the model. The required information about a specific chemical species is split into the static meta-information about the characteristics of the species, and its (generally in time and space variable) abundance in the corresponding representation. TRACER moreover includes two submodels. One is TRACER_FAMILY, an implementation of the tracer family concept. It distinguishes between two types: type-1 families are usually applied to handle strongly related tracers (e.g., fast equilibrating species) for a specific process (e.g., advection). In contrast to this, type-2 families are applied for tagging techniques. Tagging means the artificial decomposition of one or more species into parts, which are additionally labelled (e.g., by the region of their primary emission) and then processed as the species itself. The type-2 family concept is designed to conserve the linear relationship between the family and its members. The second submodel is TRACER_PDEF, which corrects and budgets numerical negative overshoots that arise in many process implementations due to the numerical limitations (e.g., rounding errors). The submodel therefore guarantees the positive definiteness of the tracers and stabilises the integration scheme. As a by-product, it further provides a global tracer mass diagnostic. Last but not least, we present the submodel PTRAC, which allows the definition of tracers via a Fortran95 namelist, as a complement to the standard tracer definition by application of the TRACER interface routines in the code. TRACER with its submodels and PTRAC can readily be applied to a variety of models without further requirements. The code and a documentation are included in the electronic supplement

Simulating organic species with the global atmospheric chemistry general circulation model ECHAM5/MESSy1: a comparison of model results with observations

The atmospheric-chemistry general circulation model ECHAM5/MESSy1 is evaluated with observations of different organic ozone precursors. This study continues a prior analysis which focused primarily on the representation of atmospheric dynamics and ozone. We use the results of the same reference simulation and apply a statistical analysis using data from numerous field campaigns. The results serve as a basis for future improvements of the model system. ECHAM5/MESSy1 generally reproduces the spatial distribution and the seasonal cycle of carbon monoxide (CO) very well. However, for the background in the Northern Hemisphere we obtain a negative bias (mainly due to an underestimation of emissions from fossil fuel combustion), and in the high latitude Southern Hemisphere a yet unexplained positive bias. The model results agree well with observations of alkanes, whereas severe problems in the simulation of alkenes and isoprene are present. For oxygenated compounds the results are ambiguous: The model results are in good agreement with observations of formaldehyde, but systematic biases are present for methanol and acetone. The discrepancies between the model results and the observations are explained (partly) by means of sensitivity studies

Global cloud and precipitation chemistry and wet deposition: tropospheric model simulations with ECHAM5/MESSy1

International audienceThe representation of cloud and precipitation chemistry and subsequent wet deposition of trace constituents in global atmospheric chemistry models is associated with large uncertainties. To improve the simulated trace gas distributions we apply the new submodel SCAV, which includes detailed cloud and precipitation chemistry and present results of the atmospheric chemistry general circulation model ECHAM5/MESSy1. A good agreement with observed wet deposition fluxes for species causing acid rain is obtained. The new scheme enables prognostic calculations of the pH of clouds and precipitation, and these results are also in accordance with observations. We address the influence of detailed cloud and precipitation chemistry on trace constituents based on sensitivity simulations. The results confirm previous results from regional scale and box models, and we extend the analysis to the role of aqueous phase chemistry on the global scale. Some species are directly affected through multiphase removal processes, and many also indirectly through changes in oxidant concentrations, which in turn have an impact on the species lifetime. While the overall effect on tropospheric ozone is relatively small (3 can reach ?20%, and several important compounds (e.g., H2O2, HCHO) are substantially depleted by clouds and precipitation