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It is well established that in Europe, high O3 concentrations are most pronounced in southern/Mediterranean countries due to the more favourable climatological conditions for its formation. However, the contribution of the different sources of precursors to O3 formation within each country relative to the imported (regional and hemispheric) O3 is poorly quantified. This lack of quantitative knowledge prevents local authorities from effectively designing plans that reduce the exceedances of the O3 target value set by the European air quality directive. O3 source attribution is a challenge because the concentration at each location and time results not only from local biogenic and anthropogenic precursors, but also from the transport of O3 and precursors from neighbouring regions, O3 regional and hemispheric transport and stratospheric O3 injections. The main goal of this study is to provide a first quantitative estimation of the contribution of the main anthropogenic activity sectors to peak O3 events in Spain relative to the contribution of imported (regional and hemispheric) O3. We also assess the potential of our source apportionment method to improve O3 modelling. Our study applies and thoroughly evaluates a countrywide O3 source apportionment method implemented in the CALIOPE air quality forecast system for Spain at high resolution (4 × 4 km 2) over a 10-day period characterized by typical summer conditions in the Iberian Peninsula (IP). The method tags both O3 and its gas precursor emissions from source sectors within one simulation, and each tagged species is subject to the typical physico-chemical processes (advection, vertical mixing, deposition, emission and chemistry) as the actual conditions remain unperturbed. We quantify the individual contributions of the largest NOx local sources to high O3 concentrations compared with the contribution of imported O3. We show, for the first time, that imported O3 is the largest input to the ground-level O3 concentration in the IP, accounting for 46 %–68 % of the daily mean O3 concentration during exceedances of the European target value. The hourly imported O3 increases during typical northwestern advections (70 %–90 %, 60–80 µ g m -3), and decreases during typical stagnant conditions (30 %–40 %, 30–60 µ g m -3) due to the local NO titration. During stagnant conditions, the local anthropogenic precursors control the O3 peaks in areas downwind of the main urban and industrial regions (up to 40 % in hourly peaks). We also show that ground-level O3 concentrations are strongly affected by vertical mixing of O3 -rich layers present in the free troposphere, which result from local/regional layering and accumulation, and continental/hemispheric transport. Indeed, vertical mixing largely explains the presence of imported O3 at ground level in the IP. Our results demonstrate the need for detailed quantification of the local and remote contributions to high O3 concentrations for local O3 management, and show O3 source apportionment to be an essential analysis prior to the design of O3 mitigation plans in any non-attainment area. Achieving the European O3 objectives in southern Europe requires not only ad hoc local actions but also decided national and European-wide strategies. [ABSTRACT FROM AUTHOR]

The origin of the daily exceedances of 50μg PM10m−3 (daily limit value or DLV of the EU air quality directive) and of an arbitrary daily value (DV) 35μg PM2. 5m−3 recorded in 2001–2003 in 13 regional background stations of the Iberian Peninsula were interpreted. This was carried out by means of back-trajectory analysis, available PM model outputs, satellite data and meteorological maps. This allows the detection of high PM episodes on a regional scale and the study of their seasonal and geographical variability. The number of exceedances of the PM10 DLV ranged in 2001–2003 from 6 to 41 depending on the monitoring site. For the selected PM2. 5DV, the range of daily exceedances was 0–10 in the study period. The majority of the PM10 (>70% in most stations) and PM2. 5 (17–55% in most stations) exceedances in regional background monitoring stations are caused by African dust outbreaks. These exceedances were less frequent in winter than in summer due to: (a) the frequent long range transport of dust in the warm seasons over Iberia, (b) the re-suspension associated with convective atmospheric dynamics, and (c) the relative low rainfall favouring re-suspension and high residence time of PM. Moreover, a regional contribution of secondary aerosols derived from the efficient photochemical transformation of gaseous precursors may coincide with African transport in summer. Episodes with lack of advective conditions caused 2–29% and 20–50% of the PM10 and PM2. 5 exceedances. These occurred mainly in summer due to poor renovation of air masses, increased convective re-suspension, dispersion of pollutants towards rural areas and regional re-circulation and aging of air masses which result in the proliferation of secondary inorganic species. Long-range transport of PM from continental Europe caused exceedances (9–40% and 18–38% of the PM10 and PM2. 5 exceedances, respectively), only in northern Iberia because, as the European air masses evolve towards the south, the pollutants suffer dispersion/dilution. Local exceedances are associated with the advection of the clean Atlantic air masses, which cannot increase PM levels to a great extent without the influence of a local source of PM. The proportion of local exceedances of PM10 and PM2. 5 ranged 6–33% and 17–40%, respectively. [Copyright &y& Elsevier]