Abstract.A new sea spray source function (SSSF), termed Oceanflux Sea Spray Aerosol or OSSA, was derived based on in-situ sea spray aerosol measurements along with meteorological/physical parameters. Submicron sea spray aerosol fluxes derived from particle number concentration measurements at the Mace Head coastal station, on the west coast of Ireland, were used together with open-ocean eddy correlation flux measurements from the Eastern Atlantic Sea Spray, Gas Flux, and Whitecap (SEASAW) project cruise. In the overlapping size range, the data for Mace Head and SEASAW were found to be in a good agreement, which allowed deriving the new SSSF from the combined dataset spanning the dry diameter range from 15 nm to 6 µm. The OSSA source function has been parameterized in terms of five lognormal modes and the Reynolds number instead of the more commonly used wind speed, thereby encapsulating important influences of wave height, wind history, friction velocity, and viscosity. This formulation accounts for the different flux relationships associated with rising and waning wind speeds since these are included in the Reynolds number. Furthermore, the Reynolds number incorporates the kinematic viscosity of water, thus the SSSF inherently includes dependences on sea surface temperature and salinity. The temperature dependence of the resulting SSSF is similar to that of other in-situ derived source functions and results in lower production fluxes for cold waters and enhanced fluxes from warm waters as compared with SSSF formulations that do not include temperature effects.

Abstract. The development and application of chemistry transport models has a long tradition. Within the Netherlands the LOTOS-EUROS model has been developed by a consortium of institutes, after combining its independently developed predecessors in 2005. Recently, version 2.0 of the model was released as an open-source version. This paper presents the curriculum vitae of the model system, describing the model's history, model philosophy, basic features and a validation with EMEP stations for the new benchmark year 2012, and presents cases with the model's most recent and key developments. By setting the model developments in context and providing an outlook for directions for further development, the paper goes beyond the common model description.With an origin in ozone and sulfur modelling for the models LOTOS and EUROS, the application areas were gradually extended with persistent organic pollutants, reactive nitrogen, and primary and secondary particulate matter. After the combination of the models to LOTOS-EUROS in 2005, the model was further developed to include new source parametrizations (e.g. road resuspension, desert dust, wildfires), applied for operational smog forecasts in the Netherlands and Europe, and has been used for emission scenarios, source apportionment, and long-term hindcast and climate change scenarios. LOTOS-EUROS has been a front-runner in data assimilation of ground-based and satellite observations and has participated in many model intercomparison studies. The model is no longer confined to applications over Europe but is also applied to other regions of the world, e.g. China. The increasing interaction with emission experts has also contributed to the improvement of the model's performance. The philosophy for model development has always been to use knowledge that is state of the art and proven, to keep a good balance in the level of detail of process description and accuracy of input and output, and to keep a good record on the effect of model changes using benchmarking and validation. The performance of v2.0 with respect to EMEP observations is good, with spatial correlations around 0.8 or higher for concentrations and wet deposition. Temporal correlations are around 0.5 or higher. Recent innovative applications include source apportionment and data assimilation, particle number modelling, and energy transition scenarios including corresponding land use changes as well as Saharan dust forecasting. Future developments would enable more flexibility with respect to model horizontal and vertical resolution and further detailing of model input data.Published by Copernicus Publications on behalf of the European Geosciences Union.

Abstract. 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 PM2.5), 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 (PM2.5 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.

Through the comparison of several regional-scale chemistry transport modeling systems that simulate meteorology and air quality over the European and North American continents, this study aims at (i) apportioning error to the responsible processes using timescale analysis, (ii) helping to detect causes of model error, and (iii) identifying the processes and temporal scales most urgently requiring dedicated investigations. The analysis is conducted within the framework of the third phase of the Air Quality Model Evaluation International Initiative (AQMEII) and tackles model performance gauging through measurement-to-model comparison, error decomposition, and time series analysis of the models biases for several fields (ozone, CO, SO, NO, NO, PM, PM, wind speed, and temperature). The operational metrics (magnitude of the error, sign of the bias, associativity) provide an overallsense of model strengths and deficiencies, while apportioning the error to its constituent parts (bias, variance, and covariance) can help assess the nature and quality of the error. Each of the error components is analyzed independently and apportioned to specific processes based on the corresponding timescale (long scale, synoptic, diurnal, and intraday) using the error apportionment technique devised in the former phases of AQMEII. The application of the error apportionment method to the AQMEII Phase 3 simulations provides several key insights. In addition to reaffirming the strong impact of model inputs (emission and boundary conditions) and poor representation of the stable boundary layer on model bias, results also highlighted the high interdependencies among meteorological and chemical variables, as well as among their errors. This indicates that the evaluation of air quality model performance for individual pollutants needs to be supported by complementary analysis of meteorological fields and chemical precursors to provide results that are more insightful from a model development perspective. This will require evaluaion methods that are able to frame the impact on error of processes, conditions, and fluxes at the surface. For example, error due to emission and boundary conditions is dominant for primary species (CO, particulate matter (PM)), while errors due to meteorology and chemistry are most relevant to secondary species, such as ozone. Some further aspects emerged whose interpretation requires additional consideration, such as the uniformity of the synoptic error being region- and model-independent, observed for several pollutants; the source of unexplained variance for the diurnal component; and the type of error caused by deposition and at which scale.

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Inertial waves in a homogeneous rotating fluid travel along rays that are inclined with respect to the rotation axis. The angle of inclination depends solely on the ratio of the wave frequency and twice the angular frequency. Because of this fixed angle, the waves can become focused when reflected at a sloping wall. In an infinitely long channel with a sloping wall, the repeated action of focusing may lead to the approach to a limit cycle, the so-called wave attractor, where the energy is concentrated. This effect is studied in the laboratory in a rectangular tank with one sloping wall, placed excentrically on a rotating table. The waves are excited by modulation of the background rotation. Several frequency ratios are used to study different wave attractors and one standing wave. The observations consist mainly of particle image velocimetry data in horizontal and vertical cross-sections in one half of the basin. The attractors are observed in the vertical cross-sections. They show continuous phase propagation, which distinguishes them from the standing wave where the phase changes at the same time over the whole cross-section. However, particle motion of inertial waves is three-dimensional and the actual basin is not an ideal two-dimensional channel but is of finite length. This implies that the waves must adapt to the vertical endwalls, although a prediction of the nature of these adaptations and the structure of the three-dimensional wave field is at present lacking. For critical waves, whose rays are parallel to the slope, clear three-dimensional behaviour is observed. The location of most intense motion along this critical slope attractor changes in the horizontal direction and horizontal phase propagation is observed, with a wavelength between 1/5 and 1/4 of the basin length. For the other attractors there is little evidence of phase propagation in the horizontal direction. The motion along the attractor is however stronger near the vertical endwalls for attractors with wave rays of slopes close to 1 or larger. The standing wave and the other attractors are more clearly visible near 1/5 of the tank length.

Abstract. In this study the sensitivity of the model performance of the chemistry transport model (CTM) LOTOS-EUROS to the description of the temporal variability of emissions was investigated. Currently the temporal release of anthropogenic emissions is described by European average diurnal, weekly and seasonal time profiles per sector. These default time profiles largely neglect the variation of emission strength with activity patterns, region, species, emission process and meteorology. The three sources dealt with in this study are combustion in energy and transformation industries (SNAP1), nonindustrial combustion (SNAP2) and road transport (SNAP7). First of all, the impact of neglecting the temporal emission profiles for these SNAP categories on simulated concentrations was explored. In a second step, we constructed more detailed emission time profiles for the three categories and quantified their impact on the model performance both separately as well as combined. The performance in comparison to observations for Germany was quantified for the pollutants NO 2 , SO 2 and PM 10 and compared to a simulation using the default LOTOS-EUROS emission time profiles. The LOTOS-EUROS simulations were performed for the year 2006 with a temporal resolution of 1 h and a horizontal resolution of approximately 25 × 25km 2 .In general the largest impact on the model performance was found when neglecting the default time profiles for the three categories. The daily average correlation coefficient for instance decreased by 0.04 (NO 2 ), 0.11 (SO 2 ) and 0.01 (PM 10 ) at German urban background stations compared to the default simulation. A systematic increase in the correlation coefficient is found when using the new time profiles. The size of the increase depends on the source category, component and station. Using national profiles for road transport showed important improvements in the explained variability over the weekdays as well as the diurnal cycle for NO 2 . The largest impact of the SNAP1 and 2 profiles were found for SO 2 . When using all new time profiles simultaneously in one simulation, the daily average correlation coefficient increased by 0.05 (NO 2 ), 0.07 (SO 2 ) and 0.03 (PM 10 ) at urban background stations in Germany. This exercise showed that to improve the performance of a CTM, a better representation of the distribution of anthropogenic emission in time is recommendable. This can be done by developing a dynamical emission model that takes into account regional specific factors and meteorology.

Climate change may have an impact on air quality (ozone, particulate matter) due to the strong dependency of air quality on meteorology. The effect is often studied using a global climate model (GCM) to produce meteorological fields that are subsequently used by chemical transport models. However, climate models themselves are subject to large uncertainties and fail to reproduce the present-day climate adequately. The present study illustrates the impact of these uncertainties on air quality. To this end, output from the SRES-A1B constraint transient runs with two GCMs, i.e. ECHAM5 and MIROC-hires, has been dynamically downscaled with the regional climate model RACMO2 and used to force a constant emission run with the chemistry transport model LOTOS-EUROS in a one-way coupled run covering the period 1970–2060. <br><br> Results from the two climate simulations have been compared with a RACMO2-LOTOS-EUROS (RLE) simulation forced by the ERA-Interim reanalysis for the period 1989–2009. Both RLE_ECHAM and RLE_MIROC showed considerable deviations from RLE_ERA for daily maximum temperature, precipitation and wind speed. Moreover, sign and magnitude of these deviations depended on the region. The differences in average present-day concentrations between the simulations were equal to (RLE_MIROC) or even larger than (RLE_ECHAM) the differences in concentrations between present-day and future climate (2041–2060). The climate simulations agreed on a future increase in average summer ozone daily maximum concentrations of 5–10 μg m⁻³ in parts of Southern Europe and a smaller increase in Western and Central Europe. Annual average PM₁₀ concentrations increased 0.5–1.0 μg m⁻³ in North-West Europe and the Po Valley, but these numbers are rather uncertain: overall, changes for PM₁₀ were small, both positive and negative changes were found, and for many locations the two climate runs did not agree on the sign of the change. This illustrates that results from individual climate runs can at best indicate tendencies and should therefore be interpreted with great care