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The PAES (French acronym for synoptic scale atmospheric pollution) network focuses on the chemical composition (ozone, CO, NO<sub>x/y</sub> and aerosols) of the lower troposphere (0–3000 m). Its high-altitude surface stations located in different mountainous areas in France complete the low-altitude rural MERA stations (the French contribution to the european program EMEP, European Monitoring and Evaluation Program). They are representative of pollution at the scale of the French territory because they are away from any major source of pollution. <br><br> This study deals with ozone observations between 2001 and 2004 at 11 stations from PAES and MERA, in addition to 16 elevated stations located in mountainous areas of Switzerland, Germany, Austria, Italy and Spain. The set of stations covers a range of altitudes between 115 and 3550 m. The comparison between recent ozone mixing ratios to those of the last decade at Pic du Midi (2877 m), as well as trends calculated over 14-year data series at three high-altitude sites in the Alps (Jungfraujoch, Sonnblick and Zugspitze) reveal that ozone is still increasing but at a slower rate than in the 1980s and 1990s. <br><br> The 2001–2004 mean levels of ozone from surface stations capture the ozone stratification revealed by climatological profiles from the airborne observation system MOZAIC (Measurement of OZone and water vapour by Airbus In-service airCraft) and from ozone soundings above Payerne (Switzerland). In particular all data evidence a clear transition at about 1000–1200 m a.s.l. between a sharp gradient below (of the order of +30 ppb/km) and a gentler gradient (+3 ppb/km) above. The same altitude (1200 m) is also found to be a threshold regarding how well the ozone levels at the surface stations agree with the free-tropospheric reference (MOZAIC or soundings). Below the departure can be as large as 40%, but suddenly drops within 15% above. For stations above 2000 m, the departure is even less than 8%. Ozone variability also reveals a clear transition between boundary-layer and free-tropospheric regimes around 1000 m a.s.l. Below, diurnal photochemistry accounts for about the third of the variability in summer, but less than 20% above – and at all levels in winter – where ozone variability is mostly due to day-to-day changes (linked to weather conditions or synoptic transport). In summary, the altitude range 1000–1200 m clearly turns out in our study to be an upper limit below which specific surface effects dominate the ozone content. <br><br> Monthly-mean ozone mixing-ratios show at all levels a minimum in winter and the classical summer broad maximum in spring and summer – which is actually the superposition of the tropospheric spring maximum (April–May) and regional pollution episodes linked to persistent anticyclonic conditions that may occur from June to September. To complement this classical result it is shown that summer maxima are associated with considerably more variability than the spring maximum. This ensemble of findings support the relevance of mountain station networks such as PAES for the long-term observation of free-tropospheric ozone over Europe.
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During springtime in the polar regions, unique photochemistry converts inert halide salt ions (e.g. Br<sup>−</sup>) into reactive halogen species (e.g. Br atoms and BrO) that deplete ozone in the boundary layer to near zero levels. Since their discovery in the late 1980s, research on ozone depletion events (ODEs) has made great advances; however many key processes remain poorly understood. In this article we review the history, chemistry, dependence on environmental conditions, and impacts of ODEs. This research has shown the central role of bromine photochemistry, but how salts are transported from the ocean and are oxidized to become reactive halogen species in the air is still not fully understood. Halogens other than bromine (chlorine and iodine) are also activated through incompletely understood mechanisms that are probably coupled to bromine chemistry. The main consequence of halogen activation is chemical destruction of ozone, which removes the primary precursor of atmospheric oxidation, and generation of reactive halogen atoms/oxides that become the primary oxidizing species. The different reactivity of halogens as compared to OH and ozone has broad impacts on atmospheric chemistry, including near complete removal and deposition of mercury, alteration of oxidation fates for organic gases, and export of bromine into the free troposphere. Recent changes in the climate of the Arctic and state of the Arctic sea ice cover are likely to have strong effects on halogen activation and ODEs; however, more research is needed to make meaningful predictions of these changes.
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We developed a new emission inventory for Asia (Regional Emission inventory in ASia (REAS) Version 1.1) for the period 1980–2020. REAS is the first inventory to integrate historical, present, and future emissions in Asia on the basis of a consistent methodology. We present here emissions in 2000, historical emissions for 1980–2003, and projected emissions for 2010 and 2020 of SO<sub>2</sub>, NO<sub>x</sub>, CO, NMVOC, black carbon (BC), and organic carbon (OC) from fuel combustion and industrial sources. Total energy consumption in Asia more than doubled between 1980 and 2003, causing a rapid growth in Asian emissions, by 28% for BC, 30% for OC, 64% for CO, 108% for NMVOC, 119% for SO<sub>2</sub>, and 176% for NO<sub>x</sub>. In particular, Chinese NO<sub>x</sub> emissions showed a marked increase of 280% over 1980 levels, and growth in emissions since 2000 has been extremely high. These increases in China were mainly caused by increases in coal combustion in the power plants and industrial sectors. NMVOC emissions also rapidly increased because of growth in the use of automobiles, solvents, and paints. By contrast, BC, OC, and CO emissions in China showed decreasing trends from 1996 to 2000 because of a reduction in the use of biofuels and coal in the domestic and industry sectors. However, since 2000, Chinese emissions of these species have begun to increase. Thus, the emissions of air pollutants in Asian countries (especially China) showed large temporal variations from 1980–2003. Future emissions in 2010 and 2020 in Asian countries were projected by emission scenarios and from emissions in 2000. For China, we developed three emission scenarios: PSC (policy success case), REF (reference case), and PFC (policy failure case). In the 2020 REF scenario, Asian total emissions of SO<sub>2</sub>, NO<sub>x</sub>, and NMVOC were projected to increase substantially by 22%, 44%, and 99%, respectively, over 2000 levels. The 2020 REF scenario showed a modest increase in CO (12%), a lesser increase in BC (1%), and a slight decrease in OC (−5%) compared with 2000 levels. However, it should be noted that Asian total emissions are strongly influenced by the emission scenarios for China.
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The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) has been operating since March 2002 onboard of the ENVIronmental SATellite of the European Space Agency (ESA). The high resolution (0.035 cm<sup>−1</sup> full width half maximum, unapodized) limb-emission measurements acquired by MIPAS in the first two years of operation have very good geographical and temporal coverage and have been re-processed by ESA with the most recent versions (4.61 and 4.62) of the inversion algorithms. The products of this processing chain are pressures at the tangent points and geolocated profiles of temperature and of the volume mixing ratios of six key atmospheric constituents: H<sub>2</sub>O, O<sub>3</sub>, HNO<sub>3</sub>, CH<sub>4</sub>, N<sub>2</sub>O and NO<sub>2</sub>. As for all the measurements made with innovative instruments and techniques, this data set requires a thorough validation. In this paper we present a geophysical validation of the temperature profiles derived from MIPAS measurements by the ESA retrieval algorithm. The validation is carried-out by comparing MIPAS temperature with correlative measurements made by radiosondes, lidars, in-situ and remote sensors operated either from the ground or stratospheric balloons. <br><br> The results of the intercomparison indicate that the bias of the MIPAS profiles is generally smaller than 1 or 2 K depending on altitude. Furthermore we find that, especially at the edges of the altitude range covered by the MIPAS scan, the random error estimated from the intercomparison is larger (typically by a factor of two to three) than the corresponding estimate derived on the basis of error propagation. <br><br> In this work we also characterize the discrepancies between MIPAS temperature and the temperature fields resulting from the analyses of the European Centre for Medium-range Weather Forecasts (ECMWF). The bias and the standard deviation of these discrepancies are consistent with those obtained when comparing MIPAS to correlative measurements; however, in this case the detected bias has a peculiar behavior as a function of altitude. This behavior is very similar to that observed in previous studies and is suspected to be due to vertical oscillations in the ECMWF temperature. The current understanding is that, at least in the upper stratosphere (above ≈10 hPa), these oscillations are caused by a discrepancy between model biases and biases of assimilated radiances from primarily nadir sounders.
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The effects of unified aerosol sources on global aerosol fields simulated by different models are examined in this paper. We compare results from two AeroCom experiments, one with different (ExpA) and one with unified emissions, injection heights, and particle sizes at the source (ExpB). Surprisingly, harmonization of aerosol sources has only a small impact on the simulated inter-model diversity of the global aerosol burden, and consequently global optical properties, as the results are largely controlled by model-specific transport, removal, chemistry (leading to the formation of secondary aerosols) and parameterizations of aerosol microphysics (e.g., the split between deposition pathways) and to a lesser extent by the spatial and temporal distributions of the (precursor) emissions. <br><br> The burdens of black carbon and especially sea salt become more coherent in ExpB only, because the large ExpA diversities for these two species were caused by a few outliers. The experiment also showed that despite prescribing emission fluxes and size distributions, ambiguities in the implementation in individual models can lead to substantial differences. <br><br> These results indicate the need for a better understanding of aerosol life cycles at process level (including spatial dispersal and interaction with meteorological parameters) in order to obtain more reliable results from global aerosol simulations. This is particularly important as such model results are used to assess the consequences of specific air pollution abatement strategies.
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The characteristics of planetary wave energy propagation are being compared based on NCEP reanalysis data from 1958 to 2002 between boreal winters after strong volcanic eruptions, non-volcanic winters and episodes of strong polar vortex lasting at least 30 days. It shows that in the volcanically disturbed winters much more planetary wave energy is produced in the troposphere, passes through the lowermost stratosphere and enters the upper stratosphere than in any other times. This is contradicting earlier interpretations and model simulations. Possibly the observed El Ninos coinciding with the three significant eruptions in the second half of the 20th century contributed to the planetary wave energy. In order to produce the observed robust climate anomaly patterns in the lower troposphere, these planetary waves are suggested to be reflected near the stratopause instead of breaking. While a strong polar vortex is observed after volcanic eruptions in the stratosphere and in the troposphere, specific episodes of strong polar vortex regime exhibit much stronger anomalies and different dynamics. Hence it is suggested that the climate effects of volcanic eruptions are not being explained by the excitation of inherent zonal mean variability modes such as Strong Polar Vortex or Northern Annular Mode, but rather is another mode that possibly reflects upon the North Atlantic Oscillation.
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Soils and forests in the boreal region of the Northern Hemisphere are recognised as having a large capacity for storing air-borne Persistent Organic Pollutants (POPs), such as the polychlorinated biphenyls (PCBs). Following reductions of primary emissions of various legacy POPs, there is an increasing interest and debate about the relative importance of secondary re-emissions on the atmospheric levels of POPs. In spring of 2006, biomass burning emissions from agricultural fires in Eastern Europe were transported to the Zeppelin station on Svalbard, where record-high levels of many air pollutants were recorded (Stohl et al., 2007). Here we report on the extremely high concentrations of PCBs that were also measured during this period. 21 out of 32 PCB congeners were enhanced by more than two standard deviations above the long-term mean concentrations. In July 2004, about 5.8 million hectare of boreal forest burned in North America, emitting a pollution plume which reached the Zeppelin station after a travel time of 3–4 weeks (Stohl et al., 2006). Again, 12 PCB congeners were elevated above the long-term mean by more than two standard deviations, with the less chlorinated congeners being most strongly affected. We propose that these abnormally high concentrations were caused by biomass burning emissions. Based on enhancement ratios with carbon monoxide and known emissions factors for this species, we estimate that 130 and 66 μg PCBs were released per kilogram dry matter burned, respectively. To our knowledge, this is the first study relating atmospheric PCB enhancements with biomass burning. The strong effects on observed concentrations far away from the sources, suggest that biomass burning is an important source of PCBs for the atmosphere.
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Equivalent effective stratospheric chlorine (EESC) is a convenient parameter to quantify the effects of halogens (chlorine and bromine) on ozone depletion in the stratosphere. We show, discuss, and analyze a new formulation of EESC that now includes the effects of age-of-air dependent fractional release values and an age-of-air spectrum. This EESC can be more appropriately applied to various parts of the stratosphere because of this dependence on mean age-of-air. This new formulation provides quantitative estimates of EESC that can be directly related to inorganic chlorine and bromine throughout the stratosphere. In this paper, we first provide a detailed description of the EESC calculation. We then use this EESC formulation to estimate that human-produced ozone depleting substances will recover to 1980 levels in 2041 in the midlatitudes, and 2067 over Antarctica. These recovery dates are based upon the assumption that the international agreements for regulating ozone-depleting substances are adhered to. In addition to recovery dates, we also estimate the uncertainties and possible problems in the estimated times of recovery. The midlatitude recovery of 2041 has a 95% confidence uncertainty from 2028 to 2049, while the 2067 Antarctic recovery has a 95% confidence uncertainty from 2056 to 2078. The principal uncertainties are from the estimated mean age-of-air and fractional release values, and the assumption that these quantities are time independent. Using other model estimates of age decrease due to climate change, we estimate that midlatitude recovery may be significantly accelerated.
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The simulation of convection, lightning and consequent NO<sub>x</sub> emissions with global atmospheric chemistry models is associated with large uncertainties since these processes are heavily parameterised. Each parameterisation by itself has deficiencies and the combination of these substantially increases the uncertainties compared to the individual parameterisations. In this study several combinations of state-of-the-art convection and lightning parameterisations are used in simulations with the global atmospheric chemistry general circulation model ECHAM5/MESSy, and are evaluated against lightning observations. A wide range in the spatial and temporal variability of the simulated flash densities is found, attributed to both types of parameterisations. Some combinations perform well, whereas others are hardly applicable. In addition to resolution dependent rescaling parameters, each combination of lightning and convection schemes requires individual scaling to reproduce the observed flash frequencies. The resulting NO<sub>x</sub> profiles are inter-compared, however definite conclusions about the most realistic profiles can currently not be drawn.
