Volume for pollution dispersion: London’s atmospheric boundary layer during ClearfLo observed with two ground-based lidar types

In urban areas with high air pollution emissions, the boundary layer volume within which gases and particles are diluted is critical to air quality impacts. With advances in ground-based remote sensing technologies and data processing algorithms, observations of layers forming the atmospheric boundary layer (ABL) are becoming increasingly available at high temporal resolution. Here, mixing height (MH) estimates determined from turbulence measurements of Doppler lidars and aerosol derived mixed layer height (MLH) based on automatic lidar and ceilometer (ALC) observations within the centre of London are assessed. While MH uncertainty increases with shorter duration of vertical stare sampling within the Doppler lidar scan pattern, instrument-related noise of the ALC may result in large MLH errors due to the challenging task of layer attribution. However, when long time series are assessed most of the algorithm- and instrument-related uncertainties average out and therefore become less critical to overall climatological analyses. Systematic differences occur in nocturnal MH from two nearby (3-4 km) sites but MLH estimates at both sites generally agree with MH obtained at the denser urban setting. During daytime, most spatial variations in ABL structure induced by synoptic conditions or land cover heterogeneity at this scale do not exceed measurement uncertainty. Agreement between MH and MLH is clearly affected by ABL aerosol content and cloud 28 conditions. Discrepancies increase with cloud complexity. On average, MH rises ahead of MLH during the morning growth period and peaks earlier in the day. There is a faster afternoon decay of MLH so that MLH and MH converge again around sunset and often have similar nocturnal values. Results demonstrate that turbulence-derived MH and aerosol-derived MLH should not be used inter32 changeably for purposes of model evaluation, interpretation of surface air quality observations or 33 initialisation of chemical transport models

Ground-based aerosol optical depth trends at three high-altitude sites in Switzerland and Southern Germany from 1995–2010

Ground-based aerosol optical depth (AOD) climatologies at three high-altitude sites in Switzerland (Jungfraujoch and Davos) and Southern Germany (Hohenpeissenberg) are updated and re-calibrated for the period 1995 – 2010. In addition, AOD time-series are augmented with previously unreported data, and are homogenized for the first time. Trend analysis revealed weak AOD trends (λ = 500 nm) at Jungfraujoch (JFJ; +0.007 decade-1), Davos (DAV; +0.002 decade-1) and Hohenpeissenberg (HPB; -0.011 decade-1) where the JFJ and HPB trends were statistically significant at the 95% and 90% confidence levels. However, a linear trend for the JFJ 1995 – 2005 period was found to be more appropriate than for 1995 – 2010 due to the influence of stratospheric AOD which gave a trend -0.003 decade-1 (significant at 95% level). When correcting for a recently available stratospheric AOD time-series, accounting for Pinatubo (1991) and more recent volcanic eruptions, the 1995 – 2010 AOD trends decreased slightly at DAV and HPB but remained weak at +0.000 decade-1 and -0.013 decade-1 (significant at 95% level). The JFJ 1995 – 2005 AOD time-series similarly decreased to -0.003 decade-1 (significant at 95% level). We conclude that despite a more detailed re40 analysis of these three time-series, which have been extended by five years to the end of 2010, a significant decrease in AOD at these three high-altitude sites has still not been observed

Spatial and temporal variability of urban fluxes of methane, carbon monoxide and carbon dioxide above London, UK

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 bud- get 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

Field measurement of natural ventilation rate in an idealised full-scale building located in a staggered urban array: comparison between tracer gas and pressure-based methods

Currently, no clear standards exist for determining urban building natural ventilation rates, especially under varying realistic meteorological conditions. In this study, ventilation rates are determined using tracer gas decay and pressure-based measurements for a full-scale (6 m tall) cube. The cube was either isolated (2 months of observations) or sheltered within a staggered array (7 months), for both single-sided and cross ventilation (openings 0.4 x 1 m). Wind speeds at cube height ranged between 0.04 m s-1 and 13.1 m s-1. Errors for both ventilation methods are carefully assessed. There is no discernible linear relation between normalised ventilation rates from the two methods, except for cross ventilation in the array case. The ratio of tracer gas and pressure derived ventilation rates is assessed with wind direction. For single-sided (leeward opening) cases it approached 1. For cross ventilation the ratio was closer to 1 but with more scatter. One explanation is that agreement is better when internal mixing is less jet-dominated, i.e. for oblique directions in the isolated case and for all directions for unsteady array flows. Sheltering may reduce the flushing rate of the tracer gas from the cube relative to internal mixing rate. This new dataset provides an extensive range of conditions for numerical model evaluation and for understanding uncertainty of ventilation rates. Knowledge of the latter is critical in buildin

The impact of boundary layer height on air pollution concentrations in London – early results from the ClearfLo project.

The ClearfLo projects aims to understand the processes generating pollutants like ozone, NOx and particulate matter and their interaction with the urban atmospheric boundary layer. ClearfLo (www.clearflo.ac.uk) is a large multi-institution NERC-funded project that is establishing integrated measurements of the meteorology, composition and particulate loading of London’s urban atmosphere, complemented by an ambitious modeling programme. The project established a new long-term measurement infrastructure in London encompassing measurement capabilities at street level and at elevated sites. These measurements were accompanied by high resolution mod- eling with the UK Met Office Unified model and WRF. This combined measuring/modelling approach enables us to identify the seasonal cycle in the meteorology and composition, together with the controlling processes. Two intensive observation periods in January/February 2012 and during the Olympics in summer 2012 measured London’s atmosphere with higher level of detail. Data from these IOPs will enable us (i) to determine the vertical structure and evolution of the urban atmosphere (ii) to determine the chemical controls on ozone production, particularly the role of biogenic emissions and (iii) to determine the processes controlling the evolution of the size,distribution and composition of particulate matter. We present results from the wintertime IOP in London focusing on a wintertime pollution episode during January 2012. We compare measured concentrations from top of BT Tower in central London with rural background measurements and determine the processes leading to the urban increment in pollutant concentrations. Therefore, we combine high-resolution simulations with the Met Office Unified Model for London and mixing layer heights derived from lidar measurements with air quality measurements in central London in order to quantify the role the boundary layer depth plays for London’s concentrations

Sources and contributions of wood smoke during winter in London: assessing local and regional influences

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 KC 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

Advanced source apportionment of size-resolved trace elements at multiple sites in London during winter

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

Kerb and urban increment of highly time-resolved trace elements in PM10, PM2.5 and PM1.0 winter aerosol in London during ClearfLo 2012

Ambient concentrations of trace elements with 2 h time resolution were measured in PM10–2.5, PM2.5–1.0 and PM1.0–0.3 size ranges at kerbside, urban background and rural sites in London during winter 2012. Samples were collected using rotating drum impactors (RDIs) and subsequently analysed with synchrotron radiation-induced X-ray fluorescence spectrometry (SR-XRF). Quantification of kerb and urban increments (defined as kerb-to-urban and urban-to-rural concentration ratios, respectively), and assessment of diurnal and weekly variability provided insight into sources governing urban air quality and the effects of urban micro-environments on human exposure. Traffic-related elements yielded the highest kerb increments, with values in the range of 10.4 to 16.6 for SW winds (3.3–6.9 for NE) observed for elements influenced by brake wear (e.g. Cu, Sb, Ba) and 5.7 to 8.2 for SW (2.6–3.0 for NE) for other traffic-related processes (e.g. Cr, Fe, Zn). Kerb increments for these elements were highest in the PM10–2.5 mass fraction, roughly twice that of the PM1.0–0.3 fraction. These elements also showed the highest urban increments (~ 3.0), although no difference was observed between brake wear and other traffic-related elements. All elements influenced by traffic exhibited higher concentrations during morning and evening rush hours, and on weekdays compared to weekends, with the strongest trends observed at the kerbside site, and additionally enhanced by winds coming directly from the road, consistent with street canyon effects. Elements related to mineral dust (e.g. Al, Si, Ca, Sr) showed significant influences from traffic-induced resuspension, as evidenced by moderate kerb (3.4–5.4 for SW, 1.7–2.3 for NE) and urban (~ 2) increments and increased concentrations during peak traffic flow. Elements related to regional transport showed no significant enhancement at kerb or urban sites, with the exception of PM10–2.5 sea salt (factor of up to 2), which may be influenced by traffic-induced resuspension of sea and/or road salt. Heavy-duty vehicles appeared to have a larger effect than passenger vehicles on the concentrations of all elements influenced by resuspension (including sea salt) and wearing processes. Trace element concentrations in London were influenced by both local and regional sources, with coarse and intermediate fractions dominated by traffic-induced resuspension and wearing processes and fine particles influenced by regional transport

Urban heat mitigation by green and blue infrastructure: drivers, effectiveness, and future needs

The combination of urbanisation and global warming leads to urban overheating and compounds the frequency and intensity of extreme heat events due to climate change. Yet, the risk of urban overheating can be mitigated by urban green-blue-grey infrastructures (GBGI), such as parks, wetlands, and engineered greening, which have the potential to effectively reduce summer air temperatures. Despite many reviews, the evidence bases on quantified GBGI cooling benefits remains partial and the practical recommendations for implementation are unclear. This systematic literature review synthesises the evidence base for heat mitigation and related co-benefits, identifies knowledge gaps, and proposes recommendations for their implementation to maximise their benefits. After screening 27,486 papers, 202 were reviewed, based on 51 GBGI types categorised under 10 main divisions. Certain GBGI (green walls, parks, street trees) have been well-researched for their urban cooling capabilities. However, several other GBGI have received negligible (zoological garden, golf course, estuary) or minimal (private garden, allotment) attention. The most efficient air cooling was observed in botanical gardens (5.0±3.5°C), wetlands (4.9±3.2°C), green walls (4.1±4.2°C), street trees (3.8±3.1°C), and vegetated balconies (3.8±2.7°C). Under changing climate conditions (2070-2100) with consideration of RCP8.5, there is a shift in climate subtypes, either within the same climate zone (e.g., Dfa to Dfb and Cfb to Cfa) or across other climate zones (e.g., Dfb (continental warm-summer humid) to BSk (dry, cold semi-arid) and Cwa (temperate) to Am (tropical)). These shifts may result in lower efficiency for the current GBGI in the future. Given the importance of multiple services, it is crucial to balance their functionality, cooling performance, and other related co-benefits when planning for the future GBGI. This global GBGI heat mitigation inventory can assist policymakers and urban planners in prioritising effective interventions to reduce the risk of urban overheating, filling research gaps, and promoting community resilience

Evaluation of urban local-scale aerodynamic parameters: implications for the vertical profile of wind speed and for source areas

Nine methods to determine local-scale aerodynamic roughness length (z0) and zero-plane displacement (zd) 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 zd and z0 estimates. Across the three sites, zd varies between 5 – 45 m depending upon the method used. Morphometric methods that incorporate roughness-element height variability agree better with anemometric methods, indicating zd is consistently greater than the local mean building height. Depending upon method and wind direction, z0 varies between 0.1 and 5 m with morphometric z0 consistently being 2 – 3 m larger than the anemometric z0. 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 zd and z0