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Tropospheric O3 remains a major air-quality issue in the Mediterranean region. The combination of large anthropogenic emissions of precursors, transboundary contributions, a warm and dry aestival climate, and topographical features results in severe cases of photochemical pollution. Chemical transport models (CTMs) are essential tools for studying O3 dynamics and for assessing mitigation measures, but they need to be evaluated specifically for each air basin. In this study, we present an optimisation of the LOTOS-EUROS CTM for the Madrid air basin. Five configurations using different meteorological datasets (from the European Centre for Medium-Range Weather Forecast, ECMWF; and the Weather Research and Forecasting Model, WRF), horizontal resolution and number of vertical levels were compared for July 2016. LOTOS-EUROS responded satisfactorily in the five configurations reproducing observations of surface O3 with notable correlation and reduced bias and errors. However, the best-fit simulations for surface O3 were obtained by increasing spatial resolution and using a large number of vertical levels to reproduce vertical transport phenomena and the formation of reservoir layers. Using the optimal configuration obtained in the evaluation, three characteristic events have been described: recirculation (REC) episodes and northern and southern advection (NAD and SAD, respectively) events. REC events were found to produce the highest O3 due to the reduced ventilation associated with low wind speeds and the contribution of reservoir layers formed by vertical transport of O3 formed near the surface in the previous days of the event. NAD events, usually associated with higher wind speeds, present the lowest ground-level O3 concentrations in the region. During SAD episodes, external contributions along with low wind speeds allow O3 to increase considerably but not as much as in REC events because steady southerly winds disperse local emissions and hinder the formation of reservoir layers. ; Funding text #1 1Centro Universitario de la Defensa (CUD) de Zaragoza, Academia General Militar, Ctra. de Huesca s/n, 50090 Zaragoza, Spain 2TNO, P.O. Box 80015, 3584 TA, Utrecht, the Netherlands 3Institute of Environmental Assessment and Water Research (IDAEA-CSIC), Jordi Girona 18-26, 08034 Barcelona, Spain 4Department of Chemical and Environmental Engineering, Technical University of Madrid (UPM), c/José Gutiérrez Abascal 2, 28006 Madrid, Spain 5Escuela Técnica Superior de Ingeniería de Bilbao, Departamento de Ingeniería Química y del Medio Ambiente, Universidad del País Vasco (UPV/EHU), Urkixo Zumarkalea, s/n, 48013 Bilbao, Spain Funding text #2 Acknowledgements. This work was funded by the Ministry of Economy, Industry and Competitiveness and FEDER funds through the project HOUSE (CGL2016-78594-R); the Ministry of Agriculture, Fishing, Food and Environment; the Madrid City Council; the Madrid Regional Government; and by the Department of Research, Innovation and University of the Aragón Regional Government and the European Social Fund (project E23_17D). The study was also partially supported by the scientific programme TECNAIRE-CM funded by the Directorate General for Universities and Research of the Greater Madrid Region (S2013/MAE-2972). The authors gratefully acknowledge air-quality data provision by the following entities: Ministry for the Ecological Transition (MITECO); Madrid City Council; AEMET; and the autonomous communities of Madrid, Castilla y León and Castilla–La Mancha. Miguel Escudero received a grant from the José Castillejo programme of the Ministry of Education and Science of Spain (ref. CAS17/00108) for a 6-month research visit at TNO.View less Funding text #3 Ministry of Economy, Industry and Competitiveness of Spain and FEDER (grant no. CGL2016-78594-R); the Department of Research, Innovation and University of the Aragón Regional Government and the European Social Fund (grant no. E23_17D); the Directorate General for Universities and Research of the Greater Madrid Region (grant no. S2013/MAE-2972); and the Ministry of Education and Science of Spain (grant no. CAS17/00108). ; Peer reviewed

Ground-level and vertical measurements (performed using tethered and non-tethered balloons), coupled with modelling, of ozone (O3), other gaseous pollutants (NO, NO2, CO, SO2) and aerosols were carried out in the plains (Vic Plain) and valleys of the northern region of the (BMA) in July 2015, an area typically recording the highest O3 episodes in Spain. Our results suggest that these very high O3 episodes were originated by three main contributions: (i) the surface fumigation from high O3 reservoir layers located at 1500-3000 mg-a.g.l. (according to modelling and non-tethered balloon measurements), and originated during the previous day(s) injections of polluted air masses at high altitude; (ii) local/regional photochemical production and transport (at lower heights) from the BMA and the surrounding coastal settlements, into the inland valleys; and (iii) external (to the study area) contributions of both O3 and precursors. These processes gave rise to maximal O3 levels in the inland plains and valleys northwards from the BMA when compared to the higher mountain sites. Thus, a maximum O3 concentration was observed within the lower tropospheric layer, characterised by an upward increase of O3 and black carbon (BC) up to around 100-200 m a.g.l. (reaching up to 300 μg mg-3 of O3 as a 10 s average), followed by a decrease of both pollutants at higher altitudes, where BC and O3 concentrations alternate in layers with parallel variations, probably as a consequence of the atmospheric transport from the BMA and the return flows (to the sea) of strata injected at certain heights the previous day(s). At the highest altitudes reached in this study with the tethered balloons (900-1000 m a.g.l.) during the campaign, BC and O3 were often anti-correlated or unrelated, possibly due to a prevailing regional or even hemispheric contribution of O3 at those altitudes. In the central hours of the days a homogeneous O3 distribution was evidenced for the lowest 1 km of the atmosphere, although probably important variations could be expected at higher levels, where the high O3 return strata are injected according to the modelling results and non-tethered balloon data. Relatively low concentrations of ultrafine particles (UFPs) were found during the study, and nucleation episodes were only detected in the boundary layer. Two types of O3 episodes were identified: type A with major exceedances of the O3 information threshold (180 μg mg-3 on an hourly basis) caused by a clear daily concatenation of local/regional production with accumulation (at upper levels), fumigation and direct transport from the BMA (closed circulation); and type B with regional O3 production without major recirculation (or fumigation) of the polluted BMA/regional air masses (open circulation), and relatively lower O3 levels, but still exceeding the 8 h averaged health target. To implement potential O3 control and abatement strategies two major key tasks are proposed: (i) meteorological forecasting, from June to August, to predict recirculation episodes so that NOx and VOC abatement measures can be applied before these episodes start; (ii) sensitivity analysis with high-resolution modelling to evaluate the effectiveness of these potential abatement measures of precursors for O3 reduction. © 2017 Author(s). ; The present work was supported by the Spanish Ministry of Economy and Competitiveness and FEDER funds under the project HOUSE (CGL2016-78594-R), by the Generalitat de Catalunya (AGAUR 2015 SGR33 and the DGQA). Part of this research was supported by the Korean Ministry of the Environment through "The Eco-Innovation project". The participation of University of Marseille and University of Birmingham was partially supported by two TNA actions projects carried out under the ACTRIS2 project (grant agreement No. 654109) financed by the European Union's Horizon 2020 research and innovation program. The support of the CUD of Zaragoza (project CUD 2013-18) is also acknowledged. We are very thankful to the Generalitat de Catalunya for supplying the air quality data from the XVPCA stations, to METEOCAT (the Meteorological Office of Catalonia) for providing meteorological data and to the IES J. Callís and the Meteorological Station from Vica (especially to Manel Dot) for allowing the performance of the vertical profiles and mobile unit measurements, respectively. In memoriam of Andrei Lyasota ; Peer reviewed

Various studies have reported that the photochemical nucleation of new ultrafine particles (UFPs) in urban environments within high insolation regions occurs simultaneously with high ground ozone (O3) levels. In this work, we evaluate the atmospheric dynamics leading to summer O3 episodes in the Madrid air basin (central Iberia) by means of measuring a 3-D distribution of concentrations for both pollutants. To this end, we obtained vertical profiles (up to 1200m above ground level) using tethered balloons and miniaturised instrumentation at a suburban site located to the SW of the Madrid Metropolitan Area (MMA), the Majadahonda site (MJDH), in July 2016. Simultaneously, measurements of an extensive number of air quality and meteorological parameters were carried out at three supersites across the MMA. Furthermore, data from O3 soundings and daily radio soundings were also used to interpret atmospheric dynamics. The results demonstrate the concatenation of venting and accumulation episodes, with relative lows (venting) and peaks (accumulation) in O3 surface levels. Regardless of the episode type, the fumigation of high-altitude O3 (arising from a variety of origins) contributes the major proportion of surface O3 concentrations. Accumulation episodes are characterised by a relatively thinner planetary boundary layer ( 2400ma.s.l.). This orographic-meteorological setting causes the vertical recirculation of air masses and enrichment of O3 in the lower tropospheric layers. When the highly polluted urban plume from Madrid is affected by these dynamics, the highest Ox (O3CNO2) concentrations are recorded in the MMA. Vertical O3 profiles during venting episodes, with strong synoptic winds and a deepening of the planetary boundary layer reaching > 2000ma.s.l., were characterised by an upward gradient in O3 levels, whereas a reverse situation with O3 concentration maxima at lower levels was found during the accumulation episodes due to local and/or regional production. The two contributions to O3 surface levels (fumigation from high-altitude strata, a high O3 background, and/or regional production) require very different approaches for policy actions. In contrast to O3 vertical top-down transfer, UFPs are formed in the planetary boundary layer (PBL) and are transferred upwards progressively with the increase in PBL growth. © Author(s) 2018. ; Acknowledgements. The present work was supported by the Spanish Ministry of Agriculture, Fishing, Food and Environment, the Madrid City Council and Madrid Regional Government, and by the Ministry of Economy, Industry and Competitiveness and FEDER funds under the project HOUSE (CGL2016-78594-R) and the Gen-eralitat de Catalunya (AGAUR 2017 SGR41). Part of this research was supported by the Korea Ministry of Environment through "The Eco-Innovation project". Support is also acknowledged from the CUD of Zaragoza (project CUD 2016-05), UPV/EHU (UFI 11/47, GIU 16/03), the project PROACLIM CGL2014-52877-R, the City Council of Majadahonda for logistic support, AEMET for providing surface meteorological data, and data from radio soundings and ozone free soundings. We thank Alava Ingenieros, TSI, Solma Environmental Solutions, and Airmodus for their support and María Díez for her computer support in the treatment of radiosonde data. Dr. Escudero has been awarded a José Castillejo grant from the Spanish Ministry of Education and Science (CAS17/00108). ; Peer reviewed