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Air quality networks in cities can be costly and inconsistent and typically monitor a few pollutants. Space-based instruments provide global coverage spanning more than a decade to determine trends in air quality, augmenting surface networks. Here we target cities in the UK (London and Birmingham) and India (Delhi and Kanpur) and use observations of nitrogen dioxide (NO2) from the Ozone Monitoring Instrument (OMI), ammonia (NH3) from the Infrared Atmospheric Sounding Interferometer (IASI), formaldehyde (HCHO) from OMI as a proxy for non-methane volatile organic compounds (NMVOCs), and aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) for PM2.5. We assess the skill of these products at reproducing monthly variability in surface concentrations of air pollutants where available. We find temporal consistency between column and surface NO2 in cities in the UK and India (R = 0.5–0.7) and NH3 at two of three rural sites in the UK (R = 0.5–0.7) but not between AOD and surface PM2.5 (R < 0.4). MODIS AOD is consistent with AERONET at sites in the UK and India (R ≥ 0.8) and reproduces a significant decline in surface PM2.5 in London (2.7 % a−1) and Birmingham (3.7 % a−1) since 2009. We derive long-term trends in the four cities for 2005–2018 from OMI and MODIS and for 2008–2018 from IASI. Trends of all pollutants are positive in Delhi, suggesting no air quality improvements there, despite the roll-out of controls on industrial and transport sectors. Kanpur, identified by the WHO as the most polluted city in the world in 2018, experiences a significant and substantial (3.1 % a−1) increase in PM2.5. The decline of NO2, NH3, and PM2.5 in London and Birmingham is likely due in large part to emissions controls on vehicles. Trends are significant only for NO2 and PM2.5. Reactive NMVOCs decline in Birmingham, but the trend is not significant. There is a recent (2012–2018) steep (> 9 % a−1) increase in reactive NMVOCs in London. The cause for this rapid increase is uncertain but may reflect the increased contribution of oxygenated volatile organic compounds (VOCs) from household products, the food and beverage industry, and domestic wood burning, with implications for the formation of ozone in a VOC-limited city.

The Atmospheric Pollution and Human Health in a Chinese Megacity (APHH-Beijing) programme is an international collaborative project focusing on understanding the sources, processes and health effects of air pollution in the Beijing megacity. APHH-Beijing brings together leading China and UK research groups, state-of-the-art infrastructure and air quality models to work on four research themes: (1) sources and emissions of air pollutants; (2) atmospheric processes affecting urban air pollution; (3) air pollution exposure and health impacts; and (4) interventions and solutions. Themes 1 and 2 are closely integrated and support Theme 3, while Themes 1–3 provide scientific data for Theme 4 to develop cost-effective air pollution mitigation solutions. This paper provides an introduction to (i) the rationale of the APHH-Beijing programme and (ii) the measurement and modelling activities performed as part of it. In addition, this paper introduces the meteorology and air quality conditions during two joint intensive field campaigns – a core integration activity in APHH-Beijing. The coordinated campaigns provided observations of the atmospheric chemistry and physics at two sites: (i) the Institute of Atmospheric Physics in central Beijing and (ii) Pinggu in rural Beijing during 10 November–10 December 2016 (winter) and 21 May–22 June 2017 (summer). The campaigns were complemented by numerical modelling and automatic air quality and low-cost sensor observations in the Beijing megacity. In summary, the paper provides background information on the APHH-Beijing programme and sets the scene for more focused papers addressing specific aspects, processes and effects of air pollution in Beijing.

The Pico Mountain Observatory, located at 2225 m a.s.l. in the Azores Islands, was established in 2001 to observe long-range transport from North America to the central North Atlantic. In previous research conducted at the observatory, ozone enhancement (> 55 ppbv) in North American outflows was observed, and efficient ozone production in these outflows was postulated. This study is focused on determining the causes for high d[O3] / d[CO] values (~1 ppbv ppbv−1) observed in the summers of 2009 and 2010. The folded retroplume technique, developed by Owen and Honrath (2009), was applied to combine upwind FLEXPART transport pathways with GEOS-Chem chemical fields. The folded result provides a semi-Lagrangian view of polluted North American outflow in terms of physical properties and chemical processes, including production/loss rate of ozone and NOx produced by lightning and thermal decomposition of peroxy acetyl nitrate (PAN). Two transport events from North America were identified for detailed analysis. High d[O3] / d[CO] was observed in both events, but due to differing transport mechanisms, ozone production tendency differed between the two. A layer of net ozone production was found at 2 km a.s.l. over the Azores in the first event plume, apparently driven by PAN decomposition during subsidence of air mass in the Azores–Bermuda High. In the second event, net ozone loss occurred during transport in the lower free troposphere, yet observed d[O3] / d[CO] was high. We estimate that in both events, CO loss through oxidation contributed significantly to d[O3] / d[CO] enhancement. Thus, it is not appropriate to use CO as a passive tracer of pollution in these events. In general, use of d[O3] / d[CO] as an indicator of net ozone production/loss may be invalid for any situation in which oxidants are elevated. Based on our analysis, use of d[O3] / d[CO] to diagnose ozone enhancement without verifying the assumption of negligible CO loss is not advisable.

In situ measurements of carbon monoxide (CO) and ozone (O3) at the Pico Mountain Observatory (PMO) located in the Azores, Portugal, are analyzed together with results from an atmospheric chemical transport model (GEOS-Chem) and satellite remote sensing data (AIRS (Atmospheric Infrared Sounder) for CO, and TES (Tropospheric Emission Spectrometer) for O3) to examine the evolution of free-troposphere CO and O3 over the North Atlantic for 2001–2011. GEOS-Chem captured the seasonal cycles for CO and O3 well but significantly underestimated the mixing ratios of CO, particularly in spring. Statistically significant (using a significance level of 0.05) decreasing trends were found for both CO and O3 based on harmonic regression analysis of the measurement data. The best estimates of the possible trends for CO and O3 measurements are −0.31 ± 0.30 (2-σ) ppbv yr−1 and −0.21 ± 0.11 (2-σ) ppbv yr−1, respectively. Similar decreasing trends for both species were obtained with GEOS-Chem simulation results. The most important factor contributing to the decreases in CO and O3 at PMO over the past decade is the decline in anthropogenic emissions from North America, which more than compensate for the impacts from increasing Asian emissions. It is likely that climate change in the past decade has also affected the intercontinental transport of O3.

Point source measurements of IO by laser induced fluorescence spectroscopy were made at a semi-polluted coastal location during the Reactive Halogens in the Marine Boundary Layer (RHaMBLe) campaign in September 2006. The site, on the NW French coast in Roscoff, was characterised by extensive intertidal macroalgae beds which were exposed at low tide. The closest known iodine active macroalgae beds were at least 300 m from the measurement point. From 20 days of measurements, IO was observed above the instrument limit of detection on 14 days, of which a clear diurnal profile was observed on 11 days. The maximum IO mixing ratio was 30.0 pptv (10 s integration period) during the day, amongst the highest concentrations ever observed in the atmosphere, and 1–2 pptv during the night. IO concentrations were strongly dependent on tidal height, the intensity of solar irradiation and meteorological conditions. An intercomparison of IO measurements made using point source and spatially averaged DOAS instruments confirms the presence of hot-spots of IO caused by an inhomogeneous distribution of macroalgae. The co-incident, point source measurement of IO and ultra fine particles (2.5 nm≥d≥10 nm) displayed a strong correlation, providing evidence that IO is involved in the production pathway of ultra fine particles at coastal locations. Finally, a modelling study shows that high IO concentrations which are likely to be produced in a macrolagae rich environment can significantly perturb the concentrations of OH and HO2 radicals. The effect of IO on HOx is reduced as NOx concentrations increase.