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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 (< 1500m at midday, lower in altitude than the orographic features), light synoptic winds, and the development of mountain breezes along the slopes of the Guadarrama Mountain Range (located W and NW of the MMA, with a maximum elevation of > 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).

We collected ground-based and aircraft vertical profile measurements of meteorological parameters during a 2-week intensive campaign over the Valencia basin, in order to understand how mesoscale circulations develop over complex terrain and affect the atmospheric transport of tracers. A high-resolution version of the RAMS model was run to simulate the campaign and characterize the diurnal patterns of the flow regime: night-time katabatic drainage, morning sea-breeze development and its subsequent coupling with mountain up-slopes, and evening flow-veering under larger-scale interactions. An application of this mesoscale model to the transport of CO2 is given in a companion paper. A careful evaluation of the model performances against diverse meteorological observations is carried out. Despite the complexity of the processes interacting with each other, and the uncertainties on modeled soil moisture boundary conditions and turbulence parameterizations, we show that it is possible to simulate faithfully the contrasted flow regimes during the course of one day, especially the inland progression and organization of the sea breeze. This gives confidence with respect to future applicability of mesoscale models to establish a reliable link between surface sources of tracers and their atmospheric concentration signals over complex terrain.

Vertical profiles of CO2 concentration were collected during an intensive summer campaign in a coastal complex-terrain region within the frame of the European Project RECAB (Regional Assessment and Modelling of the Carbon Balance in Europe). The region presents marked diurnal mesoscale circulation patterns. These circulations result in a specific coupling between atmospherically transported CO2 and its surface fluxes. To understand the effects of this interaction on the spatial variability of the observed CO2 concentrations, we applied a high-resolution transport simulation to an idealized model of land biotic fluxes. The regional Net Ecosystem Exchange fluxes were extrapolated for different land-use classes by using a set of eddy-covariance measurements. The atmospheric transport model is a Lagrangian particle dispersion model, driven by a simulation of the RAMS mesoscale model. Our simulations were able to successfully reproduce some of the processes controlling the mesoscale transport of CO2. A semi-quantitative comparison between simulations and data allowed us to characterize how the coupling between mesoscale transport and surface fluxes produced CO2 spatial gradients in the domain. Temporal averages in the simulated CO2 field show a covariance between flux and transport consisting of: 1) horizontally, a CO2 deficit over land, mirrored by a CO2 excess over the sea and 2) vertically, the prevalence of a mean CO2 depletion between 500 and 2000 m, and a permanent build-up of CO2 in the lower levels.