Inverse modeling of European CH4 emissions: sensitivity to the observational network

Inverse modeling is widely employed to provide “top-down” emission estimates using atmospheric measurements. Here, we analyze the dependence of derived CH4 emissions on the sampling frequency and density of the observational surface network, using the TM5-4DVAR inverse modeling system and synthetic observations. This sensitivity study focuses on Europe. The synthetic observations are created by TM5 forward model simulations. The inversions of these synthetic observations are performed using virtually no knowledge on the a priori spatial and temporal distribution of emissions, i.e. the emissions are derived mainly from the atmospheric signal detected by the measurement network. Using the European network of stations for which continuous or weekly flask measurements are available for 2001, the synthetic experiments can retrieve the “true” annual total emissions for single countries such as France within 20%, and for all North West European countries together within ~5%. However, larger deviations are obtained for South and East European countries due to the scarcity of stations in the measurement network. Upgrading flask sites to stations with continuous measurements leads to an improvement for central Europe in emission estimates. For realistic emission estimates over the whole European domain, however, a major extension of the number of stations in the existing network is required. We demonstrate the potential of an extended network of a total of ~60 European stations to provide realistic emission estimates over the whole European domain

The impact of air pollutant and methane emission controls on tropospheric ozone and radiative forcing: CTM calculations for the period 1990-2030

To explore the relationship between tropospheric ozone and radiative forcing with changing emissions, we compiled two sets of global scenarios for the emissions of the ozone precursors methane (CH₄), carbon monoxide (CO), non-methane volatile organic compounds (NMVOC) and nitrogen oxides (NO_x) up to the year 2030 and implemented them in two global Chemistry Transport Models. The 'Current Legislation' (CLE) scenario reflects the current perspectives of individual countries on future economic development and takes the anticipated effects of presently decided emission control legislation in the individual countries into account. In addition, we developed a 'Maximum technically Feasible Reduction' (MFR) scenario that outlines the scope for emission reductions offered by full implementation of the presently available emission control technologies, while maintaining the projected levels of anthropogenic activities. Whereas the resulting projections of methane emissions lie within the range suggested by other greenhouse gas projections, the recent pollution control legislation of many Asian countries, requiring introduction of catalytic converters for vehicles, leads to significantly lower growth in emissions of the air pollutants NO_x, NMVOC and CO than was suggested by the widely used and more pessimistic IPCC (Intergovernmental Panel on Climate Change) SRES (Special Report on Emission Scenarios) scenarios (Nakicenovic et al., 2000), which made Business-as-Usual assumptions regarding emission control technology. With the TM3 and STOCHEM models we performed several long-term integrations (1990-2030) to assess global, hemispheric and regional changes in CH₄, CO, hydroxyl radicals, ozone and the radiative climate forcings resulting from these two emission scenarios. Both models reproduce broadly the observed trends in CO, and CH₄ concentrations from 1990 to 2002. <P style='line-height: 20px;'> For the 'current legislation' case, both models indicate an increase of the annual average ozone levels in the Northern Hemisphere by 5ppbv, and up to 15ppbv over the Indian sub-continent, comparing the 2020s (2020-2030) with the 1990s (1990-2000). The corresponding higher ozone and methane burdens in the atmosphere increase radiative forcing by approximately 0.2 Wm^-2. Full application of today's emissions control technologies, however, would bring down ozone below the levels experienced in the 1990s and would reduce the radiative forcing of ozone and methane to approximately -0.1 Wm^-2. This can be compared to the 0.14-0.47 Wm^-2 increase of methane and ozone radiative forcings associated with the SRES scenarios. While methane reductions lead to lower ozone burdens and to less radiative forcing, further reductions of the air pollutants NO_x and NMVOC result in lower ozone, but at the same time increase the lifetime of methane. Control of methane emissions appears an efficient option to reduce tropospheric ozone as well as radiative forcing

Influence of future air pollution mitigation strategies on total aerosol radiative forcing

We apply different aerosol and aerosol precursor emission scenarios reflecting possible future control strategies for air pollution in the ECHAM5-HAM model, and simulate the resulting effect on the Earth's radiation budget. We use two opposing future mitigation strategies for the year 2030: one in which emission reduction legislation decided in countries throughout the world are effectively implemented (current legislation; CLE 2030) and one in which all technical options for emission reductions are being implemented independent of their cost (maximum feasible reduction; MFR 2030). We consider the direct, semi-direct and indirect radiative effects of aerosols. The total anthropogenic aerosol radiative forcing defined as the difference in the top-of-the-atmosphere radiation between 2000 and pre-industrial times amounts to -2.00 W/m2. In the future this negative global annual mean aerosol radiative forcing will only slightly change (+0.02 W/m2) under the "current legislation" scenario. Regionally, the effects are much larger: e.g. over Eastern Europe radiative forcing would increase by +1.50 W/m2 because of successful aerosol reduction policies, whereas over South Asia it would decrease by -1.10 W/m2 because of further growth of emissions. A "maximum feasible reduction" of aerosols and their precursors would lead to an increase of the global annual mean aerosol radiative forcing by +1.13 W/m2. Hence, in the latter case, the present day negative anthropogenic aerosol forcing could be more than halved by 2030 because of aerosol reduction policies and climate change thereafter will be to a larger extent be controlled by greenhouse gas emissions. We combined these two opposing future mitigation strategies for a number of experiments focusing on different sectors and regions. In addition, we performed sensitivity studies to estimate the importance of future changes in oxidant concentrations and the importance of the aerosol microphysical coupling within the range of expected future changes. For changes in oxidant concentrations caused by future air pollution mitigation, we do not find a significant effect for the global annual mean radiative aerosol forcing. In the extreme case of only abating SO2 or carbonaceous emissions to a maximum feasible extent, we find deviations from additivity for the radiative forcing over anthropogenic source regions up to 10% compared to an experiment abating both at the same time

Formation of secondary organic aerosol from isoprene oxidation over Europe

The role of isoprene as a precursor to secondary organic aerosol (SOA) over Europe is studied with the two-way nested global chemistry transport model TM5. The inclusion of the formation of SOA from isoprene oxidation in our model almost doubles the atmospheric burden of SOA over Europe compared to SOA formation from terpenes and aromatics. The reference simulation, which considers SOA formation from isoprene, terpenes and aromatics, predicts a yearly European production rate of 1.0 Tg SOA yr&lt;sup&gt;&amp;minus;1&lt;/sup&gt; and an annual averaged atmospheric burden of about 50 Gg SOA over Europe. A fraction of 35% of the SOA produced in the boundary layer over Europe is transported to higher altitudes or to other world regions. Summertime measurements of organic matter (OM) during the extensive EMEP OC/EC campaign 2002/2003 are better reproduced when SOA formation from isoprene is taken into account, reflecting also the strong seasonality of isoprene and other biogenic volatile organic compounds (BVOC) emissions from vegetation. However, during winter, our model strongly underestimates OM, likely caused by missing wood burning in the emission inventories. Uncertainties in the parameterisation of isoprene SOA formation have been investigated. Maximum SOA production is found for irreversible sticking (non-equilibrium partitioning) of condensable vapours on particles, with tropospheric SOA production over Europe increased by a factor of 4 in summer compared to the reference case. Completely neglecting SOA formation from isoprene results in the lowest estimate (0.51 Tg SOA yr&lt;sup&gt;&amp;minus;1&lt;/sup&gt;). The amount and the nature of the absorbing matter are shown to be another key uncertainty when predicting SOA levels. Consequently, smog chamber experiments on SOA formation should be performed with different types of seed aerosols and without seed aerosols in order to derive an improved treatment of the absorption of SOA in the models. Consideration of a number of recent insights in isoprene SOA formation mechanisms reduces the tropospheric production of isoprene derived SOA over Europe from 0.4 Tg yr&lt;sup&gt;&amp;minus;1&lt;/sup&gt; in our reference simulation to 0.1 Tg yr&lt;sup&gt;&amp;minus;1&lt;/sup&gt;

Hydroxyl radicals maintain the self-cleansing capacity of the troposphere

International audienceBillions of tons natural and anthropogenic gases are released and subsequently removed from the troposphere each year. Photochemical reactions, initiated by hydroxyl (OH) radicals, oxidise most gases to products which are more easily removed by precipitation and dry deposition at the Earth's surface. Since human-induced pollution emissions strongly affect OH formation and loss, large global changes in OH concentrations are possible. The available evidence as reviewed here, however, indicates that global mean OH has changed relatively little in the past century. Depletion of OH by reactive carbon gases has been compensated by increased OH formation by nitrogen oxides, an act of "inadvertent geo-engineering". Analyses of global mean OH for the past 2.5 decades, however, partly based on methyl chloroform measurements, are ambiguous. Especially the OH trend in the 1990s based on these analyses is at odds with present understanding. Since the discrepancy is dominated by the uncertainty in methyl chloroform emission estimates, improvements of source inventories and model analyses, combined with continued high precision methyl chloroform measurements, will help resolve this problem

Atmospheric deposition of nutrients and excess N formation in the North Atlantic

Anthropogenic emissions of nitrogen (N) to the atmosphere have been strongly increasing during the last century, leading to greater atmospheric N deposition to the oceans. The North Atlantic subtropical gyre (NASTG) is particularly impacted. Here, upwind sources of anthropogenic N from North American and European sources have raised atmospheric N deposition to rates comparable with N2 fixation in the gyre. However, the biogeochemical fate of the deposited N is unclear because there is no detectable accumulation in the surface waters. Most likely, deposited N accumulates in the main thermocline instead, where there is a globally unique pool of N in excess of the canonical Redfield ratio of 16 N:1 phosphorus (P). To investigate this depth zone as a sink for atmospheric N, we used a biogeochemical ocean transport model and year 2000 nutrient deposition data. We examined the maximum effects of three mechanisms that may transport excess N from the ocean surface to the main thermocline: physical transport, preferential P remineralization of sinking particles, and nutrient uptake and export by phytoplankton at higher than Redfield N:P ratios. Our results indicate that atmospheric deposition may contribute 13-19% of the annual excess N input to the main thermocline. Modeled nutrient distributions in the NASTG were comparable to observations only when non-Redfield dynamics were invoked. Preferential P remineralization could not produce realistic results on its own; if it is an important contributor to ocean biogeochemistry, it must co-occur with N2 fixation. The results suggest that: 1) the main thermocline is an important sink for anthropogenic N deposition, 2) non-Redfield surface dynamics determine the biogeochemical fate of atmospherically deposited nutrients, and 3) atmospheric N accumulation in the main thermocline has long term impacts on surface ocean biology

A GCM study of future climate response to aerosol pollution reductions

We use the global atmospheric GCM aerosol model ECHAM5-HAM to asses possible impacts of future air pollution mitigation strategies on climate. Air quality control strategies focus on the reduction of aerosol emissions. Here we investigate the extreme case of a maximum feasible end-of-pipe abatement of aerosols in the near term future (2030) in combination with increasing greenhouse gas (GHG) concentrations. The temperature response of increasing GHG concentrations and reduced aerosol emissions leads to a global annual mean equilibrium temperature response of 2.18 K. When aerosols are maximally abated only in the Industry and Powerplant sector, while other sectors stay with currently enforced regulations, the temperature response is 1.89 K. A maximum feasible abatement applied in the Domestic and Transport sector, while other sectors remain with the current legislation, leads to a temperature response of 1.39 K. Increasing GHG concentrations alone lead to a temperature response of 1.20 K. We also simulate 2–5% increases in global mean precipitation among all scenarios considered, and the hydrological sensitivity is found to be significantly higher for aerosols than for GHGs. Our study, thus highlights the huge potential impact of future air pollution mitigation strategies on climate and supports the need for urgent GHG emission reductions. GHG and aerosol forcings are not independent as both affect and are influenced by changes in the hydrological cycle. However, within the given range of changes in aerosol emissions and GHG concentrations considered in this study, the climate response towards increasing GHG concentrations and decreasing aerosols emissions is additive

Threats for Global Food Supply of Increasing Surface Ozone - Spatial Assessment of Impacts and Adaptation Options

Surface ozone (O3) is a potent phytotoxic air pollutant and significantly reduces the productivity of important agricultural crops. Growing use of fossil fuel and changes in climate are increasing the global background surface ozone concentrations to levels that threaten regional and global food supply. We performed an integrated modeling study, considering biophysical and crop management factors, to identify the spatial pattern of ozone damage in lands suitable for crop cultivation and to assess the potential for adaptation for four key crops (wheat, maize, rice and soybean) under current and future air quality legislation. Results indicate that China, India and the United States are by far the most affected countries, bearing more than half of all global losses and threatened areas. Short-erm adaptive measures at farm level, such as shifting crop calendars (by changing sowing dates or using crop cultivars with different cycle lengths) can reduce ozone damage regionally but have only limited impact at the global level. Considering these limited benefits of adaptation, mitigation of O3 precursors remains the main option to secure regional and global food production