Abstract. Road traffic emissions are often considered the main source of ultrafine particles (UFP, diameter smaller than 100 nm) in urban environments. However, recent studies worldwide have shown that – in high-insolation urban regions at least – new particle formation events can also contribute to UFP. In order to quantify such events we systematically studied three cities located in predominantly sunny environments: Barcelona (Spain), Madrid (Spain) and Brisbane (Australia). Three long-term data sets (1–2 years) of fine and ultrafine particle number size distributions (measured by SMPS, Scanning Mobility Particle Sizer) were analysed. Compared to total particle number concentrations, aerosol size distributions offer far more information on the type, origin and atmospheric evolution of the particles. By applying k-means clustering analysis, we categorized the collected aerosol size distributions into three main categories: "Traffic" (prevailing 44–63% of the time), "Nucleation" (14–19%) and "Background pollution and Specific cases" (7–22%). Measurements from Rome (Italy) and Los Angeles (USA) were also included to complement the study. The daily variation of the average UFP concentrations for a typical nucleation day at each site revealed a similar pattern for all cities, with three distinct particle bursts. A morning and an evening spike reflected traffic rush hours, whereas a third one at midday showed nucleation events. The photochemically nucleated particles' burst lasted 1–4 h, reaching sizes of 30–40 nm. On average, the occurrence of particle size spectra dominated by nucleation events was 16% of the time, showing the importance of this process as a source of UFP in urban environments exposed to high solar radiation. Nucleation events lasting for 2 h or more occurred on 55% of the days, this extending to > 4 h in 28% of the days, demonstrating that atmospheric conditions in urban environments are not favourable to the growth of photochemically nucleated particles. In summary, although traffic remains the main source of UFP in urban areas, in developed countries with high insolation urban nucleation events are also a main source of UFP. If traffic-related particle concentrations are reduced in the future, nucleation events will likely increase in urban areas, due to the reduced urban condensation sinks.

Access to detailed comparisons in air quality variations encountered when commuting through a city offers the urban traveller more informed choice on how to minimise personal exposure to inhalable pollutants. In this study we report on an experiment designed to compare atmospheric contaminants inhaled during bus, subway train, tram and walking journeys through the city of Barcelona. Average number concentrations of particles 10-300 nm in size, N, are lowest in the commute using subway trains (N<2.5×10(4) part. cm(-3)), higher during tram travel and suburban walking (2.5×10(4) cm(-3)5.0×10(4) cm(-3)), with extreme transient peaks at busy traffic crossings commonly exceeding 1.0×10(5) cm(-3) and accompanied by peaks in Black Carbon and CO. Subway particles are coarser (mode 90 nm) than in buses, trams or outdoors (<70 nm), and concentrations of fine particulate matter (PM2.5) and Black Carbon are lower in the tram when compared to both bus and subway. CO2 levels in public transport reflect passenger numbers, more than tripling from outdoor levels to >1200 ppm in crowded buses and trains. There are also striking differences in inhalable particle chemistry depending on the route chosen, ranging from aluminosiliceous at roadsides and near pavement works, ferruginous with enhanced Mn, Co, Zn, Sr and Ba in the subway environment, and higher levels of Sb and Cu inside the bus. We graphically display such chemical variations using a ternary diagram to emphasise how "air quality" in the city involves a consideration of both physical and chemical parameters, and is not simply a question of measuring particle number or mass.

International audienc

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