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We conduct the first 4D-Var inversion of NH3 accounting for NH3 bi-directional flux, using CrIS satellite NH3 observations over Europe in 2016. We find posterior NH3 emissions peak more in springtime than prior emissions at continental to national scales, and annually they are generally smaller than the prior emissions over central Europe, but larger over most of the rest of Europe. Annual posterior anthropogenic NH3 emissions for 25 European Union members (EU25) are 25% higher than the prior emissions and very close (3 fluxes as uni-directional emissions, while the monthly regional difference can be up to 34% (Switzerland in July). Compared to monthly mean in-situ observations, our posterior NH3 emissions from both schemes generally improve the magnitude and seasonality of simulated surface NH3 and bulk NHx wet deposition throughout most of Europe, whereas evaluation against hourly measurements at a background site shows the bi-directional scheme better captures observed diurnal variability of surface NH3. This contrast highlights the need for accurately simulating diurnal variability of NH3 in assimilation of sun-synchronous observations and also the potential value of future geostationary satellite observations. Overall, our top-down ammonia emissions can help to examine the effectiveness of air pollution control policies to facilitate future air pollution management, as well as helping us understand the uncertainty in top-down NH3 emissions estimates associated with treatment of NH3 surface exchange.

We conduct the first 4D-Var inversion of NH

Increased atmospheric nitrogen (N) deposition is driving nutrient imbalances, soil acidification, biodiversity losses and the long-term reduction in stability of sensitive ecosystems which previously had limited N. In this study, we analysed the concentrations of seven different N compounds in precipitation and in the air at 34 sites across Switzerland. We calculated the N deposition by precipitation (bulk deposition) and applied the inferential method to derive dry deposition (gases, aerosols) from air concentrations. We then quantified the total inorganic N deposition by adding together the bulk and dry deposition. Finally, the total inorganic N input into the sensitive ecosystems of the 34 sites was compared to the critical loads of these ecosystems. N deposition by precipitation was the main contributor to the total N load in 16 out of 34 sites, especially into open ecosystems such as alpine/subalpine grassland, mountain hay meadows, and raised bogs. Dry deposition of ammonia (NH3) was the second most important pathway, in particular for forests close to agricultural activities, due to high NH3 concentrations and the higher deposition velocity. The N deposition exceeded the lower limit of the Critical Load of Nitrogen (CLN) range at most sites, and at many sites even surpassed the upper limit of the CLN range. No, or minor, exceedances of the critical loads for N were found only at remote sites at higher elevation in the Central Alps. Annual inorganic N deposition between 2000 and 2017 revealed a significant decline in oxidised N compounds at four of five sites (−1.6–1.8% per year), but reduced compounds only decreased at two sites (−1% and −1.4% per year) and even increased at one site (+1.2% per year), despite adopted abatement strategies for agricultural practices. This emphasises that most sensitive ecosystems in Switzerland continue to be exposed to excessive N loads through atmospheric deposition, with detrimental consequences for the biodiversity and stability of these ecosystems.

We report the determination of ammonia (NH3) diffusive sampling rates for six different designs of commercial diffusive samplers (CEH ALPHA sampler, Gradko diffusion tube, Gradko DIFRAM-400, Passam ammonia sampler, and ICS Maugeri Radiello radial sampler (blue and white turbulence barriers)), together with the validation test results for a pumped sampler (CEH DELTA denuder). The devices were all exposed in the UK's National Physical Laboratory's (NPL) controlled atmosphere test facility (CATFAC). For each of the seven diffusive sampler exposure tests there were traceable concentrations of ammonia (in the range 3–25 μg m−3) generated under well-defined conditions of temperature, relative humidity and wind speed, which are applicable to a variety of ambient monitoring environments. The sampler exposure time at each concentration was 28 days, except for the radial devices, which were exposed for 14 days. The work relied on the dilution of newly developed stable Primary Standard Gas Mixtures (PSMs) prepared by gravimetry in passivated gas cylinders as a method of improving the metrological traceability of ammonia measurements. The exposed diffusive samplers were sent blind to the participants for analysis and the reported NH3 concentrations were then compared against the known reference concentration. From the results for each sampler type a diffusive sampling rate was calculated and compared against the rate used routinely by the participants. Some measurement results were in good agreement with the known traceable reference concentration (particularly for one diffusive sampler design (ALPHA)), while other devices exhibited over-reading and under-reading (each with a clear bias). The new diffusive sampling rates determined in the laboratory study were then applied to measurements in a field comparison campaign, and this was found to deliver an improvement in agreement between the different devices deployed.

Atmospheric nitrogen (N) deposition in terrestrial ecosystems is difficult to quantify, especially in forests. In this study, we compared three approaches for determining the wet and dry deposition of nitrogen (total deposition) at 17 intensively monitored forest sites in Switzerland. Specifically, we considered approaches based on: 1) measurements of bulk deposition and throughfall in 2014 (throughfall method); 2) measurements of bulk deposition and measurements of air concentrations of ammonia (NH3) and nitrogen dioxide (NO2), to which deposition velocities were applied, also in 2014 (inferential method); and 3) a model developed for Switzerland at a high spatial resolution, run for the five-year period 2013–2017 (emission based model). In addition, changes over two decades were assessed using continuous measurements of throughfall and bulk deposition. Further, air concentrations of NH3 and NO2 measured in 2014 were compared with concentrations measured in 2000 at 10 of the sites. The three approaches generally yielded comparable estimates of total deposition, with some notable differences at some sites. For both the model and the inferential method, uncertainties were related to the deposition velocities that were applied to air concentrations of N compounds, especially for NH3. The throughfall method provided a minimum estimate of the total N deposition in the forest, but the fraction of the deposited N that is directly taken up by the canopy remained difficult to quantify. Nitrogen deposition has decreased since the mid-1990s at the majority of the sites. However, deposition of the reduced forms of N seems to have stagnated at the local level. Furthermore, N deposition is still too high in comparison with the range of empirical critical loads of N (CLN). The minimum deposition estimated from throughfall exceeds the lower limit of CLN at all sites except those in the Central Alps. Deposition estimated with the model and the inferential method exceeds the lower limit of CLN at all sites and even exceeds the upper limit at several locations.

Gaseous ammonia (NH3) is an important form of N deposition to ecosystems, but it is not being routinely monitored in Switzerland. Therefore, a study was conducted to estimate annual means and seasonal patterns of NH3 concentrations for different site types in Switzerland, and to compare annual measured and modelled NH3 concentrations. NH3 concentrations were measured using the 'Zürcher' passive sampler, a Palmes type sampler with an acidic solution as absorbent. Twenty-four sampling sites were run for one year, and 17 for two years. The samplers were changed fortnightly or monthly. Spatial emission patterns were mapped by combining information on (1) the location of emission sources, (2) national statistics on NH3-emitting activities and (3) activity-specific emission factors. The spatial resolution was one hectare. The mean annual NH3 concentration in the ambient air of the 41 sites was 2.5+/-0.3 microg m(-3) (mean+/-standard error). It ranged from 0.4 to 7.5 microg m(-3). The site type and the season were the most important factors explaining the variation in the seasonal mean concentration. NH3 concentrations were highest in intensively used agricultural areas and in cities, and lowest in Alpine sites remote from emission sources. At 39 out of 41 sites, the NH3 concentrations were higher in summer (3.1+/-0.3 microg m(-3)) than in winter (2.0+/-0.3 microg m(-3)). Modelled NH3 concentrations did not systematically deviate from measured concentrations (r2 = 0.69). With the combined monitoring and modelling approach, it is now possible to obtain a reasonable and consolidated picture of the overall NH3 situation in Switzerland.

This study presents the results of the analyses of Cd, Pb, cations and anions present in precipitation and dust at a pre-alpine and a suburban site in Switzerland in the period from 1988 to 2003. The aim of these measurements was to monitor the success of measures taken to diminish pollutant emissions. No change was found for Ca2+, K+, Na+ and Mg2+ loads – in line with expectations, as no reducing measures had been taken. Statistically significant and largely decreasing values (50–90%) were found for Cl− and Cd (linked to the fitting of filters in incineration plants), Pb (unleaded petrol), \( {\text{SO}}^{{2 - }}_{4} \) (diminishing the use of mineral oil with high S content), and the proton (lower HCl and SO2 emissions). A smaller decrease (up to 30%) or none was registered for oxidised nitrogen components (fitting cars with catalytic converters, but an increase in numbers of cars and trucks). No significant change was found for NH3 as farming techniques had undergone no major changes. The long-term measurements show that the measures taken to reduce emissions were successful. A shorter monitoring period would have been misleading owing to data variability and temporary incidents e.g. amount of precipitation.

Ambient ammonia concentrations, mainly originating from agricultural activities, have increased in the last few decades in Europe. As a consequence, critical loads on oligotrophic ecosystems such as forests and mires are greatly exceeded. Monitoring of ambient ammonia concentrations is necessary in order to investigate source-receptor relationships. Measuring ambient ammonia concentrations continuously with high time resolution is very expensive and cost-efficient systems are required. Where time resolution is of minor importance, several cost-effective systems, mainly dry denuder and passive samplers, can be applied. In this paper the Zürcher passive sampler, a diffusive sampling system, is presented. It is a Palmes type sampler with an acidic solution as absorbent and is easy to handle. It was tested at 46 sites in Switzerland over one year. The average concentration in ambient air was 2.5 microg m(-3) +/- 0.4 microg m(-3). The average of the blank values were 0.21 microg m(-3). The detection limit (double the standard deviation of the blank values) was 0.36 microg m(-3). Three passive samplers were exposed at each site and each period. The mean standard deviation of these triplicate measurements was 9.5%. Compared with a discontinuous tubular denuder system and a continuous annular denuder system, the deviation was less than 10%. The Zürcher passive sampler is a useful and cost-efficient tool to determine long-term average ammonia concentrations (one- to four-week periods) in ambient air for mean concentrations above 1 microg m(-3).