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The large-eddy simulation (LES) model uDALES is used to evaluate the predictive skill of the operational air quality model SIRANE. The use of LES in this study presents a novel approach to air quality model evaluation, avoiding sources of uncertainty and providing numerical control that permits systematic analysis of targeted parametrisations and assumptions.A case study is conducted over South Kensington, London with the morphology, emissions, meteorological conditions and boundary conditions carefully matched in both models. The dispersion of both inert (NOx) and reactive (NO, NO2 and O3) pollutants under neutral, steady-state conditions is simulated for a south-westerly and westerly wind direction. A quantitative comparison between the two models is performed using statistical indices (the fractional bias, FB, the normalised mean squared error, NMSE, and the fraction in a factor of 2, FAC2).SIRANE is shown to successfully capture the dominant trends with respect to canyon-averaged concentrations of inert NOx (FB = −0.08, NMSE = 0.08 and FAC2 = 1.0). The prediction of along-canyon velocities is shown to exhibit sources of systematic error dependant on the angle of incidence of the mean wind (FB = −0.18). The assumption of photostationarity within SIRANE (deviations from equilibrium of up to 170% exist close to busy roads) is also identified as a significant source of systematic bias resulting in over- and underpredictions of NO2 (FB = −0.18) and O3 (FB = 0.14) respectively. The validity of the assumed uniform in-canyon concentration is assessed by analysing the pedestrian, leeward and windward concentrations resolved in uDALES. The use of canyon-averaged concentrations to predict pedestrian level exposure is shown to result in significant underestimations. Linear regression is used to effectively capture the relationship between pedestrian- and canyon-averaged concentrations in uDALES. Correction factors are derived (m≈1.62 and R2=0.92 for inert NOx) that are capable of significantly improving SIRANE's ability to assess pedestrian level exposure for the conditions investigated in this study. The prevalence of intersections and advective nature of the shear layer are highlighted as important differences between modelling real heterogeneous urban morphology and idealised infinite canyons. Keywords: Urban air quality, Model evaluation, Large-eddy simulation, Street canyon modelling, Traffic emissions, Pollutant dispersion

Accurate instantaneous vehicle emissions models are vital for evaluating the impacts of road transport on air pollution at high temporal and spatial resolution. In this study, we apply machine learning techniques to a dataset of 70 diesel vehicles tested in real-world driving conditions to: (i) cluster vehicles with similar emissions performance, and (ii) model instantaneous emissions. The application of dynamic time warping and clustering analysis by NOx emissions resulted in 17 clusters capturing 88% of trips in the dataset. We show that clustering effectively groups vehicles with similar emissions profiles, however no significant correlation between emissions and vehicle characteristics (i.e. engine size, vehicle weight) were found. For each cluster, we evaluate three instantaneous emissions models: a look-up table (LT) approach, a non-linear regression (NLR) model and a neural network multi-layer perceptron (MLP) model. The NLR model provides accurate instantaneous NOx predictions, on par with the MLP: relative errors in prediction of emission factors are below 20% for both models, average fractional biases are −0.01 (s.d. 0.02) and −0.0003 (s.d. 0.04), and average normalised mean squared errors are 0.25 (s.d. 0.14) and 0.29 (s.d. 0.16), for the NLR and MLP models respectively. However, neural networks are better able to deal with vehicles not belonging to a specific cluster. The new models that we present rely on simple inputs of vehicle speed and acceleration, which could be extracted from existing sources including traffic cameras and vehicle tracking devices, and can therefore be deployed immediately to enable fast and accurate prediction of vehicle NOx emissions. The speed and the ease of use of these new models make them an ideal operational tool for policy makers aiming to build emission inventories or evaluate emissions mitigation strategies.