The influence of foreign vs. North American emissions on surface ozone in the US

As part of the Hemispheric Transport of Air Pollution (HTAP; < a href='http://www.htap.org' target='_blank'> http:// www.htap.org ) project, we analyze results from 15 global and 1 hemispheric chemical transport models and compare these to Clean Air Status and Trends Network (CASTNet) observations in the United States (US) for 2001. Using the policy-relevant maximum daily 8-h average ozone (MDA8 O-3) statistic, the multi-model ensemble represents the observations well (mean r(2)=0.57, ensemble bias = +4.1 ppbv for all US regions and all seasons) despite a wide range in the individual model results. Correlations are strongest in the northeastern US during spring and fall (r(2)=0.68); and weakest in the midwestern US in summer (r(2)=0.46). However, large positive mean biases exist during summer for all eastern US regions, ranging from 10-20 ppbv, and a smaller negative bias is present in the western US during spring (similar to 3 ppbv). In nearly all other regions and seasons, the biases of the model ensemble simulations are < 5 ppbv. Sensitivity simulations in which anthropogenic O-3-precursor emissions (NOx + NMVOC + CO + aerosols) were decreased by 20% in four source regions: East Asia (EA), South Asia (SA), Europe (EU) and North America (NA) show that the greatest response of MDA8 O-3 to the summed foreign emissions reductions occurs during spring in the West (0.9 ppbv reduction due to 20% emissions reductions from EA + SA + EU). East Asia is the largest contributor to MDA8 O-3 at all ranges of the O-3 distribution for most regions (typically similar to 0.45 ppbv) followed closely by Europe. The exception is in the northeastern US where emissions reductions in EU had a slightly greater influence than EA emissions, particularly in the middle of the MDA8 O-3 distribution (response of similar to 0.35 ppbv between 35-55 ppbv). EA and EU influences are both far greater (about 4x) than that from SA in all regions and seasons. In all regions and seasons O-3-precursor emissions reductions of 20% in the NA source region decrease MDA8 O-3 the most - by a factor of 2 to nearly 10 relative to foreign emissions reductions. The O-3 response to anthropogenic NA emissions is greatest in the eastern US during summer at the high end of the O-3 distribution (5-6 ppbv for 20% reductions). While the impact of foreign emissions on surface O-3 in the US is not negligible - and is of increasing concern given the recent growth in Asian emissions - domestic emissions reductions remain a far more effective means of decreasing MDA8 O-3 values, particularly those above 75 ppb (the current US standard).

Multimodel estimates of intercontinental source-receptor relationships for ozone pollution

Isabelle Bey, Songmei Wu

Understanding the surface O-3 response over a "receptor" region to emission changes over a foreign "source" region is key to evaluating the potential gains from an international approach to abate ozone (O-3) pollution. We apply an ensemble of 21 global and hemispheric chemical transport models to estimate the spatial average surface O-3 response over east Asia (EA), Europe (EU), North America (NA), and south Asia (SA) to 20% decreases in anthropogenic emissions of the O-3 precursors, NOx, NMVOC, and CO (individually and combined), from each of these regions. We find that the ensemble mean surface O-3 concentrations in the base case (year 2001) simulation matches available observations throughout the year over EU but overestimates them by > 10 ppb during summer and early fall over the eastern United States and Japan. The sum of the O-3 responses to NOx, CO, and NMVOC decreases separately is approximately equal to that from a simultaneous reduction of all precursors. We define a continental-scale "import sensitivity" as the ratio of the O-3 response to the 20% reductions in foreign versus "domestic" (i.e., over the source region itself) emissions. For example, the combined reduction of emissions from the three foreign regions produces an ensemble spatial mean decrease of 0.6 ppb over EU (0.4 ppb from NA), less than the 0.8 ppb from the reduction of EU emissions, leading to an import sensitivity ratio of 0.7. The ensemble mean surface O-3 response to foreign emissions is largest in spring and late fall (0.7-0.9 ppb decrease in all regions from the combined precursor reductions in the three foreign regions), with import sensitivities ranging from 0.5 to 1.1 (responses to domestic emission reductions are 0.8-1.6 ppb). High O-3 values are much more sensitive to domestic emissions than to foreign emissions, as indicated by lower import sensitivities of 0.2 to 0.3 during July in EA, EU, and NA when O-3 levels are typically highest and by the weaker relative response of annual incidences of daily maximum 8-h average O-3 above 60 ppb to emission reductions in a foreign region(< 10-20% of that to domestic) as compared to the annual mean response (up to 50% of that to domestic). Applying the ensemble annual mean results to changes in anthropogenic emissions from 1996 to 2002, we estimate a Northern Hemispheric increase in background surface O-3 of about 0.1 ppb a(-1), at the low end of the 0.1-0.5 ppb a(-1) derived from observations. From an additional simulation in which global atmospheric methane was reduced, we infer that 20% reductions in anthropogenic methane emissions from a foreign source region would yield an O-3 response in a receptor region that roughly equals that produced by combined 20% reductions of anthropogenic NOx, NMVOC, and CO emissions from the foreign source

2009

Une première mesure lidar combinée d'ozone et de vent, à partir d'une instrumentation et d'une méthodologie coup par coup

During these last decades, air pollution has drawn the attention of scientists because of the deterioration of the human environment that it has caused. Unfortunately, the study of this dynamic phenomenon is very complex and requires the use of models that compute the evolution of the physico-chemical parameters of the atmosphere. Moreover, the predictions of the numerical simulations have to be validated by range- and time-resolved measurements, carried out continuously up to the top of the planetary boundary layer. Only the optical radar or lidar satisfies these specifications: for this reason the Laboratory for Air and Soil Pollution (LPAS) of the Swiss Federal Institute of Technology (EPFL) has developed such a system in order to provide the modellers with information complementary to that given by the ground measurements. This instrument, after mounting on a mobile platform, has determined the concentration of the key molecule ozone during several field campaigns, demonstrating its reliability and precision. Moreover, the EPFL system is a shot per shot lidar, able to record each detected signal and not only its average in a time interval. This feature is innovative to lidar determinations of tropospheric ozone and allows one to measure accurately the statistical error, to correct for the effect of systematic biases and to observe the dynamic behaviour of the atmosphere: the measurement of the statistical error has been used to build a model of the signal and of its noise, useful in the design of future lidar systems and for the comparison of the various data processing algorithms. the correction of the bias caused by the artificial deformation of the statistical distribution of the signal at long distance has led to a considerable increase of the range of the retrieved ozone profiles, the observation of the dynamic behaviour of the atmosphere has resulted in the first simultaneous measurement of a pollutant concentration and of the wind velocity with the same data set recorded by a lidar.

EPFL1996

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