Abstract. An Analysis of Covariance (ANCOVA) was used to derive the influence of the meteorological variability on the daily maximum ozone concentrations at 12 low-elevation sites north of the Alps in Switzerland during the four seasons in the 1992-2002 period. The afternoon temperature and the morning global radiation were the variables that accounted for most of the meteorological variability in summer and spring, while other variables that can be related to vertical mixing and dilution of primary pollutants (afternoon global radiation, wind speed, stability or day of the week) were more significant in winter. In addition, the number of days after a frontal passage was important to account for ozone build-up in summer and ozone destruction in winter. The statistical model proved to be a robust tool for reducing the impact of the meteorological variability on the ozone concentrations. The explained variance of the model, averaged over all stations, ranged from 60.2% in winter to 71.9% in autumn. The year-to-year variability of the seasonal medians of daily ozone maxima was reduced by 85% in winter, 60% in summer, and 50% in autumn and spring after the meteorological adjustment. For most stations, no significantly negative trends (at the 95% confidence level) of the summer medians of daily O 3 or O x (O 3 +NO 2 ) maxima were found despite the significant reduction in the precursor emissions in Central Europe. However, significant downward trends in the summer 90th percentiles of daily O x maxima were observed at 6 sites in the region around Zürich (on average −0.73 ppb yr −1 for those sites). The lower effect of the titration by NO as a consequence of the reduced emissions could partially explain the significantly positive O 3 trends in the cold seasons (on average 0.69 ppb yr −1 in winter and 0.58 ppb yr −1 in autumn). The increase of O x found for most stations in autumn (on average 0.23 ppb yr −1 ) and winter (on average 0.39 ppb yr −1 ) could be due to increasing European background ozone levCorrespondence to: A. S. H. Prévôt (andre.prevot@psi.ch) els, in agreement with other studies. The statistical model was also able to explain the very high ozone concentrations in summer 2003, the warmest summer in Switzerland for at least ∼150 years. On average, the measured daily ozone maximum was 15 ppb (nearly 29%) higher than in the reference period summer 1992-2002, corresponding to an excess of 5 standard deviations of the summer means of daily ozone maxima in that period.
Abstract. Net vertical air mass export by thermally driven flows from the atmospheric boundary layer (ABL) to the free troposphere (FT) above deep Alpine valleys was investigated. The vertical export of pollutants above mountainous terrain is presently poorly represented in global chemistry transport models (GCTMs) and needs to be quantified. Air mass budgets were calculated using aircraft observations obtained in deep Alpine valleys. The results show that on average 3 times the valley air mass is exported vertically per day under fair weather conditions. During daytime the type of valleys investigated in this study can act as an efficient "air pump" that transports pollutants upward. The slope wind system within the valley plays an important role in redistributing pollutants. Nitrogen oxide emissions in mountainous regions are efficiently injected into the FT. This could enhance their ozone (O 3 ) production efficiency and thus influences tropospheric pollution budgets. Once lifted to the FT above the Alps pollutants are transported horizontally by the synoptic flow and are subject to European pollution export. Forward trajectory studies show that under fair weather conditions two major pathways for air masses above the Alps dominate. Air masses moving north are mixed throughout the whole tropospheric column and further transported eastward towards Asia. Air masses moving south descend within the subtropical high pressure system above the Mediterranean.
Atmospheric transport processes, relevant to high Alpine sites, were deduced from 2 sets of aerosol records: a 9‐year record from the Jungfraujoch (3454 m) on the northern side of the Swiss Alps and a 2.5‐year record from Colle Gnifetti (4452 m) on the southern side. A classification scheme for synoptic weather types was applied to separate the aerosol data into groups corresponding to different atmospheric transport conditions. For both sites, vertical aerosol transport by thermally driven convection, acting between late spring and late summer, was found to be the dominant transport process. In summer, the thermally driven aerosol transport to both sites caused an increase of the seasonally averaged aerosol concentration between 0800 and 1800 local standard time by a factor of two. Under anticyclonic conditions, when subsidence on a synoptic scale is present, the thermally driven aerosol transport is most pronounced. Therefore, the aerosol determining thermal transport takes place within a synoptic scale vertical motion of opposite direction. Under cyclonic conditions, when lifting on a synoptic scale is present, the thermally driven aerosol transport is nearly absent. In winter, thermally driven convection does not contribute to the aerosol concentrations at both sites. Nevertheless, also in winter statistically significant differences in aerosol concentration were found between cyclonic and anticyclonic weather conditions, which can be attributed to the vertical transport acting on the synoptic scale. These differences in aerosol concentration were small compared to the corresponding differences in summer. Within the weather types, which are dominated by horizontal advection in the Alpine region, the aerosol concentrations are more diffcult to interpret with respect to the effective transport process.
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