We present a comparison of tropospheric NO₂ from OMI measurements to the median of an ensemble of Regional Air Quality (RAQ) models, and an intercomparison of the contributing RAQ models and two global models for the period July 2008–June 2009 over Europe. The model forecasts were produced routinely on a daily basis in the context of the European GEMS ("Global and regional Earth-system (atmosphere) Monitoring using Satellite and in-situ data") project. The tropospheric vertical column of the RAQ ensemble median shows a spatial distribution which agrees well with the OMI NO₂ observations, with a correlation r=0.8. This is higher than the correlations from any one of the individual RAQ models, which supports the use of a model ensemble approach for regional air pollution forecasting. The global models show high correlations compared to OMI, but with significantly less spatial detail, due to their coarser resolution. Deviations in the tropospheric NO₂ columns of individual RAQ models from the mean were in the range of 20–34% in winter and 40–62% in summer, suggesting that the RAQ ensemble prediction is relatively more uncertain in the summer months. The ensemble median shows a stronger seasonal cycle of NO₂ columns than OMI, and the ensemble is on average 50% below the OMI observations in summer, whereas in winter the bias is small. On the other hand the ensemble median shows a somewhat weaker seasonal cycle than NO₂ surface observations from the Dutch Air Quality Network, and on average a negative bias of 14%. Full profile information was available for two RAQ models and for the global models. For these models the retrieval averaging kernel was applied. Minor differences are found for area-averaged model columns with and without applying the kernel, which shows that the impact of replacing the a priori profiles by the RAQ model profiles is on average small. However, the contrast between major hotspots and rural areas is stronger for the direct modeled vertical columns than the columns where the averaging kernels are applied, related to a larger relative contribution of the free troposphere and the coarse horizontal resolution in the a priori profiles compared to the RAQ models. In line with validation results reported in the literature, summertime concentrations in the lowermost boundary layer in the a priori profiles from the DOMINO product are significantly larger than the RAQ model concentrations and surface observations over the Netherlands. This affects the profile shape, and contributes to a high bias in OMI tropospheric columns over polluted regions. The global models indicate that the upper troposphere may contribute significantly to the total column and it is important to account for this in comparisons with RAQ models. A combination of upper troposphere model biases, the a priori profile effects and DOMINO product retrieval issues could explain the discrepancy observed between the OMI observations and the ensemble median in summer.

We discuss the capability of current state-of-the-art chemistry and transport models to reproduce air quality trends and interannual variability. Documenting these strengths and weaknesses on the basis of historical simulations is essential before the models are used to investigate future air quality projections. To achieve this, a coordinated modelling exercise was performed in the framework of the CityZEN European Project. It involved six regional and global chemistry-transport models (BOLCHEM, CHIMERE, EMEP, EURAD, OSLOCTM2 and MOZART) simulating air quality over the past decade in the Western European anthropogenic emissions hotspots. Comparisons between models and observations allow assessing the skills of the models to capture the trends in basic atmospheric constituents (NO₂, O₃, and PM₁₀). We find that the trends of primary constituents are well reproduced (except in some countries – owing to their sensitivity to the emission inventory) although capturing the more moderate trends of secondary species such as O₃ is more challenging. Apart from the long term trend, the modelled monthly variability is consistent with the observations but the year-to-year variability is generally underestimated. A comparison of simulations where anthropogenic emissions are kept constant is also investigated. We find that the magnitude of the emission-driven trend exceeds the natural variability for primary compounds. We can thus conclude that emission management strategies have had a significant impact over the past 10 yr, hence supporting further emission reductions.

The EURODELTA III exercise has facilitated a comprehensive intercomparison and evaluation of chemistry transport model performances. Participating models performed calculations for four 1-month periods in different seasons in the years 2006 to 2009, allowing the influence of different meteorological conditions on model performances to be evaluated. The exercise was performed with strict requirements for the input data, with few exceptions. As a consequence, most of differences in the outputs will be attributed to the differences in model formulations of chemical and physical processes. The models were evaluated mainly for background rural stations in Europe. The performance was assessed in terms of bias, root mean square error and correlation with respect to the concentrations of air pollutants (NO₂, O₃, SO₂, PM₁₀ and PM_2.5), as well as key meteorological variables. Though most of meteorological parameters were prescribed, some variables like the planetary boundary layer (PBL) height and the vertical diffusion coefficient were derived in the model preprocessors and can partly explain the spread in model results. In general, the daytime PBL height is underestimated by all models. The largest variability of predicted PBL is observed over the ocean and seas. For ozone, this study shows the importance of proper boundary conditions for accurate model calculations and then on the regime of the gas and particle chemistry. The models show similar and quite good performance for nitrogen dioxide, whereas they struggle to accurately reproduce measured sulfur dioxide concentrations (for which the agreement with observations is the poorest). In general, the models provide a close-to-observations map of particulate matter (PM_2.5 and PM₁₀) concentrations over Europe rather with correlations in the range 0.4–0.7 and a systematic underestimation reaching −10 µg m⁻³ for PM₁₀. The highest concentrations are much more underestimated, particularly in wintertime. Further evaluation of the mean diurnal cycles of PM reveals a general model tendency to overestimate the effect of the PBL height rise on PM levels in the morning, while the intensity of afternoon chemistry leads formation of secondary species to be underestimated. This results in larger modelled PM diurnal variations than the observations for all seasons. The models tend to be too sensitive to the daily variation of the PBL. All in all, in most cases model performances are more influenced by the model setup than the season. The good representation of temporal evolution of wind speed is the most responsible for models' skillfulness in reproducing the daily variability of pollutant concentrations (e.g. the development of peak episodes), while the reconstruction of the PBL diurnal cycle seems to play a larger role in driving the corresponding pollutant diurnal cycle and hence determines the presence of systematic positive and negative biases detectable on daily basis.

Key apriori information used in 4D‐Var is the knowledge of the system's evolution equations. In this article we propose a method for taking full advantage of the knowledge of the system's dynamical instabilities in order to improve the quality of the analysis. We present an algorithm for four‐dimensional variational assimilation in the unstable subspace (4D‐Var – AUS), which consists of confining in this subspace the increment of the control variable. The existence of an optimal subspace dimension for this confinement is hypothesized. Theoretical arguments in favour of the present approach are supported by numerical experiments in a simple perfect nonlinear model scenario. It is found that the RMS analysis error is a function of the dimension N of the subspace where the analysis is confined and is a minimum for N approximately equal to the dimension of the unstable and neutral manifold. For all assimilation windows, from 1 to 5 d, 4D‐Var – AUS performs better than standard 4D‐Var. In the presence of observational noise, the 4D‐Var solution, while being closer to the observations, is farther away from the truth. The implementation of 4D‐Var – AUS does not require the adjoint integration. Copyright © 2010 Royal Meteorological Society