The Clean Air for London (ClearfLo) project provides integrated measurements of the meteorology, composition, and particulate loading of the urban atmosphere in London, United Kingdom, to improve predictive capability for air quality. METEOROLOGY, AIR QUALITY, AND HEALTH IN LONDONThe ClearfLo Project Economic and Social Affairs 2013). Urban populations are exposed to stressful environmental conditions, such as local and nonlocal pollutants, that cause poor air quality and microclimates that exacerbate heat stress during heat waves. These are projected to increase in a warming climate. Our cities are therefore nexus points for several environmental health stresses that we currently face (Rydin et al. 2012) and the interacting issues around sustainability and human health.The purpose of this paper is to introduce the Clean Air for London (ClearfLo) project, which investigates the atmospheric science that underpins these health stresses, with a particular focus on the urban increment in atmospheric drivers. We focused on three atmospheric drivers of environmental health stress in cities, namely, heat, gas-phase pollutants, and particulate matter (PM). Health stresses from the urban atmospheric environment.Heat waves have an impact on human health. Populations typically display an optimal temperature range at which the (daily or weekly) mortality rate is lowest. Mortality rates rise as temperatures exceed this optimal range (e.g., Rydin et al. 2012). The 2003 European heat wave (Stedman 2004) in combination with air pollution was responsible for more than 2000 excess deaths in the United Kingdom (Johnson et al. 2005). Under a warming climate, the risks posed by heat stress are predicted to increase (Hacker et al. 2005). People living in urban environments are exposed to higher temperatures than in nonurban regions. Thus, heat-related deaths could be higher within urban areas (Mavrogianni et al. 2011). Hence, ClearfLo is concerned with measuring the factors controlling the urban atmospheric boundary layer, that is, the surface energy balance.The World Health Organization (WHO) reported (WHO 2006) that the strongest effects of air quality 779MAY 2015 AMERICAN METEOROLOGICAL SOCIETY | on health are attributable to PM, followed by ozone (O 3 ) and nitrogen dioxide (NO 2 ). A recent report (Guerreiro et al. 2013) indicates that in 2011 up to 88% of the urban population in Europe was exposed to concentrations exceeding the WHO air quality guidelines for PM 10 (defined as particles that pass through a size-selective inlet with a 50% efficiency cutoff at 10-µm aerodynamic diameter, representative of the inhalable fraction). It is estimated that a reduction of PM 10 to the WHO annual-mean guideline of 20 µg m −3 would reduce attributable deaths per year in Europe by 22,000. Further, this would lead to a substantial improvement in the quality of life for millions with a preexisting respiratory or cardiovascular disease (COMEAP 2010).Epidemiological studies consistently demonstrate an association between the PM mass concentr...

It has long been known that the urban surface energy balance is different to that of a rural surface, and that heating of the urban surface after sunset gives rise to the Urban Heat Island (UHI). Less well known is how flow and turbulence structure above the urban surface are changed during different phases of the urban boundary layer (UBL). This paper presents new observations above both an urban and rural surface and investigates how much UBL structure deviates from classical behaviour. A 5-day, low wind, cloudless, high pressure period over London, UK, was chosen for analysis, during which there was a strong UHI. Boundary layer evolution for both sites was determined by the diurnal cycle in sensible heat flux, with an extended decay period of approximately 4 h for the convective UBL. This is referred to as the "Urban Convective Island" as the surrounding rural area was already stable at this time. Mixing height magnitude depended on the combination of regional temperature profiles and surface temperature. Given the daytime UHI intensity of 1.5°C, combined with multiple inversions in the temperature profile, urban and rural mixing heights underwent opposite trends over the period, resulting in a factor of three height difference by the fifth day. Nocturnal jets undergoing inertial oscillations were observed aloft in the urban wind profile as soon as the rural boundary layer became stable: clear jet maxima over the urban surface only emerged once the UBL had become stable. This was due to mixing during the Urban Convective Island reducing shear. Analysis of turbulent moments (variance, skewness and kurtosis) showed "upside-down" boundary layer characteristics on some mornings during initial rapid growth of the convective UBL. During the "Urban Convective Island" phase, turbulence structure still resembled a classical convective boundary layer but with some influence from shear aloft, depending on jet strength. These results demonstrate that appropriate choice of Doppler lidar scan patterns can give detailed profiles of UBL flow. Insights drawn from the observations have implications for accuracy of boundary conditions when simulating urban flow and dispersion, as the UBL is clearly the result of processes driven not only by local surface conditions but also regional atmospheric structure.

Nine methods to determine local-scale aerodynamic roughness length (z 0 ) and zero-plane displacement (z d ) are compared at three sites (within 60 m of each other) in London, UK. Methods include three anemometric (single-level high frequency observations), six morphometric (surface geometry) and one reference-based approach (look-up tables). A footprint model is used with the morphometric methods in an iterative procedure. The results are insensitive to the initial z d and z 0 estimates. Across the three sites, z d varies between 5 and 45 m depending upon the method used. Morphometric methods that incorporate roughness-element height variability agree better with anemometric methods, indicating z d is consistently greater than the local mean building height. Depending upon method and wind direction, z 0 varies between 0.1 and 5 m with morphometric z 0 consistently being 2-3 m larger than the anemometric z 0 . No morphometric method consistently resembles the anemometric methods. Wind-speed profiles observed with Doppler lidar provide additional data with which to assess the methods. Locally determined roughness parameters are used to extrapolate wind-speed profiles to a height roughly 200 m above the canopy. Wind-speed profiles extrapolated based on morphometric methods that account for roughness-element height variability are most similar to observations. The extent of the modelled source area for measurements varies by up to a factor of three, depending upon the morphometric method used to determine z d and z 0 .

Abstract. Determining the contribution of wood smoke to air pollution in large cities such as London is becoming increasingly important due to the changing nature of domestic heating in urban areas. During winter, biomass burning emissions have been identified as a major cause of exceedances of European air quality limits. The aim of this work was to quantify the contribution of biomass burning in London to concentrations of PM2.5 and determine whether local emissions or regional contributions were the main source of biomass smoke. To achieve this, a number of biomass burning chemical tracers were analysed at a site within central London and two sites in surrounding rural areas. Concentrations of levoglucosan, elemental carbon (EC), organic carbon (OC) and K+ were generally well correlated across the three sites. At all the sites, biomass burning was found to be a source of OC and EC, with the largest contribution of EC from traffic emissions, while for OC the dominant fraction included contributions from secondary organic aerosols, primary biogenic and cooking sources. Source apportionment of the EC and OC was found to give reasonable estimation of the total carbon from non-fossil and fossil fuel sources based upon comparison with estimates derived from 14C analysis. Aethalometer-derived black carbon data were also apportioned into the contributions from biomass burning and traffic and showed trends similar to those observed for EC. Mean wood smoke mass at the sites was estimated to range from 0.78 to 1.0 μg m−3 during the campaign in January–February 2012. Measurements on a 160 m tower in London suggested a similar ratio of brown to black carbon (reflecting wood burning and traffic respectively) in regional and London air. Peaks in the levoglucosan and K+ concentrations were observed to coincide with low ambient temperature, consistent with domestic heating as a major contributing local source in London. Overall, the source of biomass smoke in London was concluded to be a background regional source overlaid by contributions from local domestic burning emissions. This could have implications when considering future emission control strategies during winter and may be the focus of future work in order to better determine the contributing local sources.

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Abstract. We report on more than 3 years of measurements of fluxes of methane (CH4), carbon monoxide (CO) and carbon dioxide (CO2) taken by eddy-covariance in central London, UK. Mean annual emissions of CO2 in the period 2012–2014 (39.1 ± 2.4 ktons km−2 yr−1) and CO (89 ± 16 tons km−2 yr−1) were consistent (within 1 and 5 % respectively) with values from the London Atmospheric Emissions Inventory, but measured CH4 emissions (72 ± 3 tons km−2 yr−1) were over two-fold larger than the inventory value. Seasonal variability was large for CO with a winter to summer reduction of 69 %, and monthly fluxes were strongly anti-correlated with mean air temperature. The winter increment in CO emissions was attributed mainly to vehicle cold starts and reduced fuel combustion efficiency. CO2 fluxes were 33 % higher in winter than in summer and anti-correlated with mean air temperature, albeit to a lesser extent than for CO. This was attributed to an increased demand for natural gas for heating during the winter. CH4 fluxes exhibited moderate seasonality (21 % larger in winter), and a spatially variable linear anti-correlation with air temperature. Differences in resident population within the flux footprint explained up to 90 % of the spatial variability of the annual CO2 fluxes and up to 99 % for CH4. Furthermore, we suggest that biogenic sources of CH4, such as wastewater, which is unaccounted for by the atmospheric emissions inventories, make a substantial contribution to the overall budget and that commuting dynamics in and out of central business districts could explain some of the spatial and temporal variability of CO2 and CH4 emissions. To our knowledge, this study is unique given the length of the data sets presented, especially for CO and CH4 fluxes. This study offers an independent assessment of "bottom-up" emissions inventories and demonstrates that the urban sources of CO and CO2 are well characterized in London. This is however not the case for CH4 emissions which are heavily underestimated by the inventory approach. Our results and others point to opportunities in the UK and abroad to identify and quantify the "missing" sources of urban methane, revise the methodologies of the emission inventories and devise emission reduction strategies for this potent greenhouse gas.

Abstract. Trace element measurements in PM10–2.5, PM2.5–1.0 and PM1.0–0.3 aerosol were performed with 2 h time resolution at kerbside, urban background and rural sites during the ClearfLo winter 2012 campaign in London. The environment-dependent variability of emissions was characterized using the Multilinear Engine implementation of the positive matrix factorization model, conducted on data sets comprising all three sites but segregated by size. Combining the sites enabled separation of sources with high temporal covariance but significant spatial variability. Separation of sizes improved source resolution by preventing sources occurring in only a single size fraction from having too small a contribution for the model to resolve. Anchor profiles were retrieved internally by analysing data subsets, and these profiles were used in the analyses of the complete data sets of all sites for enhanced source apportionment. A total of nine different factors were resolved (notable elements in brackets): in PM10–2.5, brake wear (Cu, Zr, Sb, Ba), other traffic-related (Fe), resuspended dust (Si, Ca), sea/road salt (Cl), aged sea salt (Na, Mg) and industrial (Cr, Ni); in PM2.5–1.0, brake wear, other traffic-related, resuspended dust, sea/road salt, aged sea salt and S-rich (S); and in PM1.0–0.3, traffic-related (Fe, Cu, Zr, Sb, Ba), resuspended dust, sea/road salt, aged sea salt, reacted Cl (Cl), S-rich and solid fuel (K, Pb). Human activities enhance the kerb-to-rural concentration gradients of coarse aged sea salt, typically considered to have a natural source, by 1.7–2.2. These site-dependent concentration differences reflect the effect of local resuspension processes in London. The anthropogenically influenced factors traffic (brake wear and other traffic-related processes), dust and sea/road salt provide further kerb-to-rural concentration enhancements by direct source emissions by a factor of 3.5–12.7. The traffic and dust factors are mainly emitted in PM10–2.5 and show strong diurnal variations with concentrations up to 4 times higher during rush hour than during night-time. Regionally influenced S-rich and solid fuel factors, occurring primarily in PM1.0–0.3, have negligible resuspension influences, and concentrations are similar throughout the day and across the regions.

With a number of operational centres looking forward to the possibilities of “city scale” NWP and climate modelling it is important to understand the behaviour of order 100 m models over cities. A key issue is how to handle the representation of partially resolved turbulence in these models. In this article we compare the representation of a clear convective boundary‐layer case in London in 100 and 50 m grid‐length versions of the Unified Model (MetUM) with observations. Comparison of Doppler lidar observations of the vertical velocity shows that convective overturning in the boundary layer is broadly well represented in terms of its depth and magnitude. The role of model resolution was investigated by comparing a 50 m grid‐length model with the 100 m one. It is found that, although going to 50 m grid length does not greatly change many of the bulk properties (mixing height, heat flux profiles, etc.) the spatial structure of the overturning is significantly different. This is confirmed with spectral analysis which shows that the 50 m model resolves significantly more of the energetic eddies, and a length‐scale analysis that shows the 50 and 100 m models produce convective structures 2–3 times larger than observed. We conclude that, for the MetUM, model grid‐lengths of order 100 m may well be sufficient for predicting many bulk and statistical properties of convective boundary layers; however, the details of the spatial structures around convective overturning in these situations are likely to be still under‐resolved. Spin‐up artefacts emanating from the inflow boundary of the model are investigated by comparing with a smaller 100 m grid‐length domain which is more dominated by such effects. These manifest themselves as along‐wind boundary‐layer rolls which produce a less realistic comparison with the lidar observations. A stability analysis is presented in order to better understand the formation of these rolls.