International audienceExisting descriptions of bi-directional ammonia (NH3) land-atmosphere exchange incorporate temperature and moisture controls, and are beginning to be used in regional chemical transport models. However, such models have typically applied simpler emission factors to upscale the main NH3 emission terms. While this approach has successfully simulated the main spatial patterns on local to global scales, it fails to address the environment- and climate-dependence of emissions. To handle these issues, we outline the basis for a new modelling paradigm where both NH3 emissions and deposition are calculated online according to diurnal, seasonal and spatial differences in meteorology. We show how measurements reveal a strong, but complex pattern of climatic dependence, which is increasingly being characterized using ground-based NH3 monitoring and satellite observations, while advances in process-based modelling are illustrated for agricultural and natural sources, including a global application for seabird colonies. A future architecture for NH3 emission-deposition modelling is proposed that integrates the spatio-temporal interactions, and provides the necessary foundation to assess the consequences of climate change. Based on available measurements, a first empirical estimate suggests that 5°C warming would increase emissions by 42 per cent (28-67%). Together with increased anthropogenic activity, global NH3 emissions may increase from 65 (45-85) Tg N in 2008 to reach 132 (89-179) Tg by 2100

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.A large shortcoming of current chemistry transport models (CTM) for simulating the fate of ammonia in the atmosphere is the lack of a description of the bi-directional surface-atmosphere exchange. In this paper, results of an update of the surface-atmosphere exchange module DEPAC, i.e. DEPosition of Acidifying Compounds, in the chemistry transport model LOTOS-EUROS are discussed. It is shown that with the new description, which includes bi-directional surface-atmosphere exchange, the modeled ammonia concentrations increase almost everywhere, in particular in agricultural source areas. The reason is that by using a compensation point the ammonia lifetime and transport distance is increased. As a consequence, deposition of ammonia and ammonium decreases in agricultural source areas, while it increases in large nature areas and remote regions especially in southern Scandinavia. The inclusion of a compensation point for water reduces the dry deposition over sea and allows reproducing the observed marine background concentrations at coastal locations to a better extent. A comparison with measurements shows that the model results better represent the measured ammonia concentrations. The concentrations in nature areas are slightly overestimated, while the concentrations in agricultural source areas are still underestimated. Although the introduction of the compensation point improves the model performance, the modeling of ammonia remains challenging. Important aspects are emission patterns in space and time as well as a proper approach to deal with the high concentration gradients in relation to model resolution. In short, the inclusion of a bi-directional surface-atmosphere exchange is a significant step forward for modeling ammonia.

[1] The annual amount of dew input to the water budget in the midlatitudes is mostly neglected, possibly because direct dew measurements are very difficult and timeconsuming. As the Netherlands has a very high frequency of dew events, a grassland area was selected to determine whether dew input could be significant. The study site is situated within the Wageningen University meteorological station. Dew measurement experiments were carried out in 2004. Data were used to verify a surface energy dew model, which was then applied to an 11-year data set. A mean annual dew amount of 37 mm was obtained with a standard deviation of 8 mm, while the mean annual precipitation was 830 mm with a standard deviation of 200 mm. Dew contributed about 4.5% of the mean annual precipitation. The average number of dew nights per year was 250 (70%) with a standard deviation of 25 nights. This frequency significantly affects leaf wetness and possible vegetation diseases.

Abstract. Global distributions of atmospheric ammonia (NH 3 ) measured with satellite instruments such as the Infrared Atmospheric Sounding Interferometer (IASI) contain valuable information on NH 3 concentrations and variability in regions not yet covered by ground-based instruments. Due to their large spatial coverage and (bi-)daily overpasses, the satellite observations have the potential to increase our knowledge of the distribution of NH 3 emissions and associated seasonal cycles. However the observations remain poorly validated, with only a handful of available studies often using only surface measurements without any vertical information. In this study, we present the first validation of the IASI-NH 3 product using ground-based Fourier transform infrared spectroscopy (FTIR) observations. Using a recently developed consistent retrieval strategy, NH 3 concentration profiles have been retrieved using observations from nine Network for the Detection of Atmospheric Composition Change (NDACC) stations around the world between 2008 and 2015. We demonstrate the importance of strict spatiotemporal collocation criteria for the comparison. Large differences in the regression results are observed for changing intervals of spatial criteria, mostly due to terrain characteristics and the short lifetime of NH 3 in the atmosphere. The seasonal variations of both datasets are consistent for most sites. Correlations are found to be high at sites in areas with considerable NH 3 levels, whereas correlations are lower at sites with low atmospheric NH 3 levels close to the detection limit of the IASI instrument. A combination of the observations Published by Copernicus Publications on behalf of the European Geosciences Union. These results give an improved estimate of the IASI-NH3 product performance compared to the previous upper-bound estimates (−50 to +100 %).

The spatial comparison reveals a good overall agreement of the NH 3 distributions not only in these source regions but also over remote areas and over sea when transport is observed. On average, the measured columns exceed the modeled ones, except for a few cases. Large discrepancies over several industrial areas in Eastern Europe and Russia point to underestimated emissions in the underlying inventories. The temporal analysis over the three hot spot areas reveals that the seasonality is well captured by the model when the lower sensitivity of the satellite measurements in the colder months is taken into account. Comparison of the daily time series indicates possible misrepresentations of the timing and magnitude of the emissions. Finally, specific attention to biomass burning events shows that modeled plumes are less spread out than the observed ones. This is confirmed for the 2010 Russian fires with a comparison using in situ observations.

Abstract. We present two Differential Optical Absorption Spectroscopy (DOAS) instruments built at RIVM: the RIVM DOAS and the miniDOAS. Both instruments provide virtually interference-free measurements of NH 3 concentrations in the atmosphere, since they measure over an open path, without suffering from inlet problems or interference problems by ammonium aerosols dissociating on tubes or filters. They measure concentrations up to at least 200 µg m −3 , have a fast response, low maintenance demands, and a high uptime. The RIVM DOAS has a high accuracy of typically 0.15 µg m −3 for ammonia for 5-min averages and over a total light path of 100 m. The miniDOAS has been developed for application in measurement networks such as the Dutch National Air Quality Monitoring Network (LML). Compared to the RIVM DOAS it has a similar accuracy, but is significantly reduced in size, costs, and handling complexity. The RIVM DOAS and miniDOAS results showed excellent agreement (R 2 = 0.996) during a field measurement campaign in Vredepeel, the Netherlands. This measurement site is located in an agricultural area and is characterized by highly variable, but on average high ammonia concentrations in the air. The RIVM-DOAS and miniDOAS results were compared to the results of the AMOR instrument, a continuous-flow wet denuder system, which is currently used in the LML. Averaged over longer time spans of typically a day, the (mini)DOAS and AMOR results agree reasonably well, although an offset of the AMOR values compared to the (mini)DOAS results exists. On short time scales, the (mini)DOAS shows a faster response and does not show the memory effects due to inlet tubing and transport of absorption fluids encountered by the AMOR. Due to its high accuracy, high uptime, low maintenance and its open path, the (mini)DOAS shows a good potential for flux measurements by using two (or more) systems in a gradient set-up and applying the aerodynamic gradient technique.

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