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Numerical weather prediction (NWP) of urban aerosols is increasingly sophisticated and accurate. In the absence of large particles (e.g. rain, cloud droplets), information on atmospheric aerosols can be obtained from single wavelength automatic lidars and ceilometers (ALC) that measure profiles of attenuated backscatter (βo). To assess the suitability of ALC profile observations for forecast evaluation and data assimilation, a forward operator is required to convert model variables into the measured quantity. Here, an aerosol forward operator (aerFO) is developed and tested with Met Office NWP data (UKV 1.5 km) to obtain synthetic attenuated backscatter profiles (βm). aerFO requires as input the profiles of bulk aerosol mass mixing ratio and relative humidity to compute βm, plus air temperature and pressure to calculate the effect of water vapour absorption. Bulk aerosol characteristics (e.g. mean radius and number concentration) are used to estimate optical properties. ALC profile observations in London are used to assess βm. A wavelength-dependent extinction enhancement factor accounts for the change in optical properties due to aerosol swelling. Sensitivity studies show the aerFO unattenuated backscatter is very sensitive to the aerosol mass and relative humidity above ∼60–80%. The extinction efficiency is sensitive to the choice of aerosol constituents and to ALC wavelength. Given aerosol is a tracer for boundary layer dynamics, application of the aerFO has proven very useful to evaluate the performance of urban surface parameterisation schemes and their ability to drive growth of the mixing layer. Implications of changing the urban surface scheme within the UKV is explored using two spring cases. For the original scheme, morning βm is too high probably because of delayed vertical mixing. The new scheme reduced this persistence of high morning βm, demonstrating the importance of surface heating processes. Analysis of profiles at five sites on 12 clear-sky days shows a positive, statistically significant relation between the differences of modelled and measured near-surface attenuated backscatter [βm - βo] and near-surface aerosol mass. This suggests errors in near-surface attenuated backscatter can be attributed to errors in the amount of aerosol estimated by the NWP scheme. Correlation increases when cases of high relative humidity in the NWP model are excluded. Given the impact on aerosol optical properties demonstrated, results suggest the use of a fixed, bulk aerosol for urban areas in the UKV should be revisited and the lidar ratio should be constrained. As quality of the observed attenuated backscatter is demonstrated to be critical for performing model evaluation, careful sensor operation and data processing is vital to avoid false conclusions to be drawn about model performance.

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 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 inter-changeably for purposes of model evaluation, interpretation of surface air quality observations or initialisation of chemical transport models.

Numerical weather prediction (NWP) models often parameterise aerosols to reduce computational needs, while aiming to accurately capture their impact adequately. Increasingly, aerosols are monitored in-situ directly and/or indirectly (e.g. by automatic lidars and ceilometers, ALC). ALC measure the aerosol optical characteristic of attenuated backscatter. This can also be estimated using forward models that combine forecast aerosol and relative humidity to parameterise aerosol physical and optical characteristics. The aerFO is one such forward model, designed to use Met Office NWP model output and parameterisations from the MURK visibility scheme. Given the aerFO-MURK scheme link, assessing the aerFO and its output could therefore be used to inform future developments of the MURK scheme. To identify which parameterised physical and optical aerosol characteristics in the scheme are the most critical in urban settings, aerFO is driven with different in-situ aerosol observations at a background site in central London. Estimated attenuated backscatter is then assessed against ALC observations. It is shown that the original MURK scheme parameterisation underestimates the variance of both dry mean volume radius and total number concentration. Representing both the accumulation and coarse mode aerosols in the aerFO reduces the median bias error of estimated attenuated backscatter by 69.1 %. Providing more realistic temporal (monthly to hourly) variability of relative mass for different species leads to little improvement, compared to using monthly climatological means. Numerical experiments show that having more realistic estimates of number concentration is more important than providing more accurate values of the dry mean volume radius for the accumulation mode. Hence, improving the parameterisations for number concentration should be a main focus for further development of the MURK scheme. To estimate aerosol attenuated backscatter, the aerFO requires an extinction to backscatter ratio (i.e. the lidar ratio). In addition to forward modelling, the lidar ratio can also be used with ALC attenuated backscatter to calculate aerosol properties estimated in aerosol forecasts. Here, a model is developed that estimates the ratio using in-situ observations of the number size distribution and speciated aerosol masses. The values of lidar ratio derived at the London background site (14 – 80 sr across selected common lidar wavelengths) compare well to the literature. However, the modelled lidar ratio is unexpectedly correlated to relative humidity. Further, a stronger dependence exists at shorter wavelengths (355 and 532 nm) compared to longer wavelengths (905 and 1064 nm), and is due to the critical relation of lidar wavelength to aerosol size.\ud \ud Keywords: urban aerosols; lidar forward operator; automatic lidar and ceilometers; urban observation network; lidar ratio

Anthropogenic emissions of heat and exhaust gases play an important role in the atmospheric boundary layer, altering air quality, greenhouse gas concentrations and the transport of heat and moisture at various scales. This is particularly evident in urban areas where emission sources are integrated in the highly heterogeneous urban canopy layer and directly linked to human activities which exhibit significant temporal variability. It is common practice to use eddy covariance observations to estimate turbulent surface fluxes of latent heat, sensible heat and carbon dioxide, which can be attributed to a local scale source area. This study provides a method to assess the influence of micro-scale anthropogenic emissions on heat, moisture and carbon dioxide exchange in a highly urbanized environment for two sites in central London, UK. A new algorithm for the Identification of Micro-scale Anthropogenic Sources (IMAS) is presented, with two aims. Firstly, IMAS filters out the influence of micro-scale emissions and allows for the analysis of the turbulent fluxes representative of the local scale source area. Secondly, it is used to give a first order estimate of anthropogenic heat flux and carbon dioxide flux representative of the building scale. The algorithm is evaluated using directional and temporal analysis. The algorithm is then used at a second site which was not incorporated in its development. The spatial and temporal local scale patterns, as well as micro-scale fluxes, appear physically reasonable and can be incorporated in the analysis of long-term eddy covariance measurements at the sites in central London. In addition to the new IMAS-technique, further steps in quality control and quality assurance used for the flux processing are presented. The methods and results have implications for urban flux measurements in dense urbanised settings with significant sources of heat and greenhouse gases.