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A comprehensive characterisation of atmospheric aerosols in the subtropical eastern North Atlantic has been carried out using long-term ground-based Aerosol Robotic NETwork (AERONET) photometric observations over the period 2005–2020 from a unique network made up of four stations strategically located from sea level to 3555 m on the island of Tenerife. This site can be considered a sentinel for the passage of airmasses going to Europe from Africa, and therefore the aerosol characterisation performed here adds important information for analysing their evolution during their path toward Northern Europe. Two of these stations (Santa Cruz de Tenerife – SCO – at sea level and La Laguna – LLO – at 580 m a.s.l.) are located within the marine atmospheric boundary layer (MABL), and the other two (Izaña – IZO – at 2373 m a.s.l. and Teide Peak – TPO – at 3555 m a.s.l.) are high mountain stations within the free troposphere (FT). Monthly climatology of the aerosol optical depth (AOD), Ångström exponent (AE), aerosol concentration, size distribution and aerosol optical properties has been obtained for the MABL and FT. Measurements that are quite consistent across the four sites have been used to categorise the main atmospheric scenarios, and these measurements confirm an alternation between predominant background conditions and predominant dust-loaded Saharan air mass conditions caused by seasonal dust transport over the subtropical North Atlantic. Background conditions prevail in the MABL and FT for most of the year, while dust-laden conditions dominate in July and August. The MABL under background conditions appears as a well-mixed layer with a low aerosol concentration (the volume concentration, VolCon, ranges from 0.02 ± 0.01 to 0.04 ± 0.02 µm3 µm−2), a predominance of coarse-mode marine aerosols (the effective radius, Reff, changes from 1.60 ± 0.19 to 1.91 ± 0.34 µm), and a volume contribution of the fine-mode fraction Vf/Vt . The clean FT is characterised by remarkably low aerosol loading and a predominant impact of fine-mode aerosols throughout the year (Vf/Vt has a maximum value of 0.93 ± 0.13), with an average Reff of 0.16 ± 0.02 µm. However, under dust-laden conditions and mainly in summer, we observe a predominance of coarse-mode aerosols with maximum VolCon values of 0.26 ± 0.23 µm3 µm−2 for the MABL and 0.16 ± 0.12 (0.06 ± 0.05) µm3 µm−2 for IZO (TPO), and a similar and quite consistent fine-mode fraction of 0.12 ± 0.03 in the vertical within the MABL and FT. Similarities in micro-physical and optical intensive aerosol properties confirm that the Saharan Air Layer (SAL) is a well-mixed layer in terms of the particulate composition. An estimation of the difference in the aerosol loading in the 1 km layer between IZO and TPO (in terms of VolCon and AOD) is performed in this study, and this shows that aerosol loading at IZO is double that at TPO, but they have similar fine-mode fractions, effective radii and intensive optical properties. The long-term trend analysis at SCO shows a significant negative trend in the fine-mode AOD between 2005 and 2020 (−1.8 ± 0.5) × 10−5 yr−1, which might be linked to the large reduction in oil-refining SO2 emissions from the SCO refinery in 2012.

The La Palma 2021 volcanic eruption was the first subaerial eruption in a 50-year period in the Canary Islands (Spain), emitting ~1.8 Tg of sulphur dioxide (SO2) into the troposphere over nearly 3 months (19 September-13 December 2021), exceeding the total anthropogenic SO2 emitted from the 27 European Union countries in 2019. We conducted a comprehensive evaluation of the impact of the 2021 volcanic eruption on air quality (SO2, PM10 and PM2.5 concentrations) utilising a multidisciplinary approach, combining ground and satellite-based measurements with height-resolved aerosol and meteorological information. High concentrations of SO2, PM10 and PM2.5 were observed in La Palma (hourly mean SO2 up to ~2600 μg m−3 and also sporadically at ~140 km distance on the island of Tenerife (> 7700 μg m−3) in the free troposphere. PM10 and PM2.5 daily mean concentrations in La Palma peaked at ~380 and 60 μg m−3. Volcanic aerosols and desert dust both impacted the lower troposphere in a similar height range (~ 0–6 km) during the eruption, providing a unique opportunity to study the combined effect of both natural phenomena. The impact of the 2021 volcanic eruption on SO2 and PM concentrations was strongly influenced by the magnitude of the volcanic emissions, the injection height, the vertical stratification of the atmosphere and its seasonal dynamics. Mean daily SO2 concentrations increased during the eruption, from 38 μg m−3 (Phase I) to 92 μg m−3 (Phase II), showing an opposite temporal trend to mean daily SO2 emissions, which decreased from 34 kt (Phase I) to 7 kt (Phase II). The results of this study are relevant for emergency preparedness in all international areas at risk of volcanic eruptions; a multidisciplinary approach is key to understand the processes by which volcanic eruptions affect air quality and to mitigate and minimise impacts on the population., The authors gratefully acknowledge the extraordinary effort carried out by the AEMET staff (both in La Palma and in support of the activities in La Palma) during the volcanic eruption, from the Izaña Atmospheric Research Center and the Delegation of AEMET in the Canary Islands. We thank the CSIC deployment service during the eruption and its coordination by Manuel Nogales. We also gratefully acknowledge the dedication and information provided by the PEVOLCA Scientific Committee and all the support received from the insular and local governments (Cabildo Insular de La Palma and the Ayuntamientos de Tazacorte, Los Llanos de Aridane and El Paso). The authors would also like to thank the Canary Islands Government for data from their Air Quality Monitoring Network and the MPL Network (MPLNET) for their support to the lidar measurements used in this paper. The authors also acknowledge the support from ACTRIS and ACTRIS-Spain, the Spanish Ministry of Science and Innovation and the support from the European Union H2020 program through the following projects (PID2019-104205GB-C21/AEI/10.13039/501100011033, EQC2018-004686-P, PID2019-103886RB-I00/AEI/10.13039/501100011033 and PID2020- 521-118793GA-I00) and programs (GA No. 654109, 778349, 871115, 101008004 and 101086690). Research activities of the CSIC staff during the eruption were funded by CSIC through the CSIC-PIE project with ID numbers PIE20223PAL009 and PIE20223PAL013 (Real Decreto 1078/2021, de 7 de diciembre). Part of this study was performed within the framework of the project AERO-EXTREME (PID2021-125669NBI00) funded by the Spanish State Research Agency (AEI) and ERDF funds.

A comprehensive characterization of atmospheric aerosols in the Subtropical Eastern North Atlantic has been carried out using long-term ground-based Aerosol Robotic NETwork (AERONET) photometric observations from a unique network made up of four stations strategically located from the sea level to 3555 m height on the island of Tenerife over the period 2005–2020. This site is can be considered a sentinel of the passage of airmass going to Europe from Africa and therefore the aerosol characterization performed here adds important information to analyse their evolution during the path toward Northern Europe. Two of these stations (Santa Cruz de Tenerife –SCO- at sea level and La Laguna –LLO- at 580 m asl) are located within the Marine Boundary Layer 5 (MBL) and the other two (Izana –IZO- at 2373 m asl and Teide Peak –TPO- at 3555 m asl) are high mountain stations within the Free Troposphere (FT). Monthly climatology of Aerosol Optical Depth (AOD), Angstrom Exponent (AE), aerosol concentration, size distribution, and aerosol optical properties has been obtained for the MBL and FT. Quite consistent measurements at the four sites have been used to categorise the main atmospheric scenarios confirming the predominance of the alternating background to dust-loaded Saharan air mass conditions seasonally affecting the sites as a result of the seasonal dust transport over the Subtropical North Atlantic. Background conditions prevail in the MBL and FT most of the year while dust-laden conditions dominate in July and August. The MBL under background conditions appears as a well-mixed layer with low aerosol concentration (volume concentration, VolCon, ranging from 0.02±0.01 to 0.04±0.02 μm3 · μm−2) with a predominance of coarse mode marine aerosols (effective radius, Re ff, changing from 1.60±0.19 to 1.91±0.34 μm) and fine mode fraction < 0.35. The clean FT has been characterised by remarkably low aerosol loading and a predominant impact of fine mode aerosols throughout the year (V f / V t with a maximum value of 0.93±0.13) with an average Re ff of 0.16±0.02 μm. However, under dust-laden conditions, we observe the predominance of coarse mode aerosols, mainly in summer, with maximum VolCon values of 0.26±0.23 μm3 · μm−2 for MBL and 0.16±0.12 (0.06±0.05) μm3 · μm−2 for IZO (TPO) and a similar and quite consistent fine mode fraction of 0.120.03 in the vertical within MBL and FT. Similarities in micro-physical and optical intensive aerosol properties confirm the Saharan Air Layer (SAL) as a well-mixed layer in terms of the particulate composition. An estimation of the difference in the aerosol loading in the 1-km layer between IZO and TPO (in terms of VolCon and AOD) is performed in this study, showing that aerosol loading at IZO is double that of TPO but with similar fine mode fraction, effective radius and optical intensive properties. The long-term trend analysis at SCO shows a negative significant trend in the fine AOD mode between 2005 and 2020 (-1.8±0.5) ·10−5 yr−1, which might be linked to the large reduction of oil refining SO2 emissions at SCO refinery in 2012.

In this study the GAG model, a process-based ammonia (NH3) emission model for urine patches was extended and applied for the field scale. The new model (GAG_field) was tested over two modelling periods, for which micrometeorological NH3 flux data were available. Acknowledging uncertainties in the measurements, the model was able to simulate the main features of the observed fluxes. The temporal evolution of the simulated NH3 exchange flux was found to be dominated by NH3 emission from the urine patches, offset by simultaneous NH3 deposition to areas of the field not affected by urine. The simulations show how NH3 fluxes over a grazed field in a given day can be affected by urine patches deposited several days earlier, linked to the interaction of volatilization processes with soil pH dynamics. Sensitivity analysis showed that GAG_field was more sensitive to soil buffering capacity (β), field capacity (θfc) and permanent wilting point (θpwp) than the patch scale model. This can be explained by the different initial soil pH and physical characteristics which determine the maximum volume of urine that can be stored in the NH3 source layer. It was found that in the case of urine patches with a higher initial soil pH and higher initial soil water content, the sensitivity of NH3 exchange to β was stronger. Also, in the case of a higher initial soil water content, NH3 exchange was more sensitive to the changes in θfc and θpwp. The sensitivity analysis showed that the nitrogen content of urine (cN) is associated with high uncertainty in the simulated fluxes. However, model experiments based on cN values randomized from an estimated statistical distribution indicated that this uncertainty is considerably smaller in practice. Finally, GAG_field was tested with a constant soil pH of 7.5. The variation of NH3 fluxes simulated in this way showed a good agreement with those from the simulations with the original approach, accounting for a dynamically changing soil pH. These results suggest a way for model simplification when GAG_field is applied later for regional scale.

Agricultural livestock represents the main source of ammonia (NH3) in Europe. In recent years, reduction policies have been applied to reduce NH3 emissions. In order to estimate the impacts of these policies, robust estimates of the emissions from the main sources, i.e. livestock farms are needed. In this paper, the NH3 emissions were estimated from a naturally ventilated livestock farm in Braunschweig, Germany during a joint field experiment of the GRAMINAE European project. An inference method was used with a Gaussian-3-D plume model and a local-scale dispersion and deposition model (FIDES-2-D). NH3 concentrations downwind of the source were used together with micrometeorological data to estimate the source strength over time. Mobile NH3 concentration measurements provided information on the spatial distribution of source strength. The estimated emission strength ranged between 6.0±0.17 kg NH3 d−1 (FIDES-2-D model) and 9.2±0.7 kg NH3 d−1 (Gaussian model). These estimates were 94% and 63% of what was obtained using emission factors from the German national inventory (9.6 kg d−1 NH3. However, the FIDES-2-D approach was shown to be very sensitive to the source size, the roughness height and to whether deposition was taken into account downwind of the source. Accounting for deposition in FIDES-2-D gives a potential emission estimate of 11.7 kg NH3 d−1, showing that deposition can explain the observed difference. The daily pattern of the source was correlated with net radiation and with the temperature inside the animal houses. The daily pattern resulted from a combination of a temperature effect on the source concentration together with an effect of variations in free and forced convection of the building ventilation rate. Further development of the plume technique is especially relevant for naturally ventilated farms, since the variable ventilation rate makes other emission measurements difficult.

The exchange of ammonia (NH3) between the atmosphere and the land surface is controlled by both atmospheric and land surface processes and can thus be bi-directional. Whether emission or deposition occurs depends on the nitrogen (N) status of the ecosystem. Resistance models have been developed to represent this bi-directional pattern of NH3 exchange. Major pathways include exchange with leaf cuticles, plant tissues (via stomata) and with the soil surface. However, the parameters that quantify the emission potential of the foliage and ground surface, the NH3 stomatal compensation point, χs, and the soil surface NH3 concentration, χsoil, respectively, are entirely empirical in these models and do not consider the influence of the plant and soil N status. On the other side, grassland ecosystem models simulate the ecosystem N dynamics, but until now NH3 biosphere–atmosphere exchange was only treated in a very simple manner. A two-layer resistance model for NH3 exchange has thus been combined with the grassland ecosystem model PaSim in order to link NH3 exchange with the ecosystem N dynamics. For this purpose, the plant substrate N pool in previous versions of PaSim has been divided between apoplastic and symplastic compartments, and the apoplastic substrate N pool has been linked to the stomatal NH3 exchange. In addition, soil ammoniacal N (NHx) has been partitioned between the soil surface and several soil layers, and the soil surface NH3 exchange has been linked to the soil surface ammonium (NH4+). The new combined model has been parameterised and applied to an intensively managed grassland site in Southern Scotland. The comparison with micrometeorological measurements of NH3 fluxes has shown that the model can qualitatively reproduce the effects of cutting and fertilisation on the net NH3 exchange above the canopy. In particular, the model reproduces the expected strong coupling of the NH3 exchange with the dynamics of the apoplastic substrate N pool. However, peak NH3 emissions are underestimated, and it is postulated that this could be related to the representation of leaf litter emissions from the soil surface in the model, and to the simulated soil NHx dynamics. Nevertheless, this new version of PaSim is a valuable tool for investigating the influence of different management scenarios or of climate change on NH3 exchange.

The stomatal compensation point of ammonia (χs) is a major factor controlling the exchange of atmospheric ammonia (NH3) with vegetation. It is known to depend on the supply of nitrogen and to vary among plant species, but its seasonal variation has not yet been reported for grassland. In this study, we present the temporal variation of apoplastic NH4+ concentration ([NH4+]apo) and pH (pHapo) measured in leaves of Lolium perenne L. in a grassland, through two periods of cutting / fertilisation, followed by a livestock grazing period. The total free NH4+ concentration measured in foliage ([NH4+]fol), and soil mineral NH4+ and NO3− concentration are also presented. The value of [NH4+]apo varied from less than 0.01 mM to a maximum of 0.5 mM occurring just after fertilisation, whereas the apoplastic pH ranged from pH 6 to 6.5 for most of the time and increased up to pH 7.8, 9 days after the second fertilisation, when grazing started. [NH4+]fol varied between 20 and 50 μg N-NH4+ g−1 f.w. The compensation point at 20°C, ranged from 0.02 μg NH3 m−3 between the fertilisations to 10 μg NH3 m−3 just after the second fertilisation. The reasons for these seasonal changes are discussed, with respect to plant metabolism and the concentration of ammonium and nitrate in the soil.

Intensive field measurements of NH3 and CO2 exchange were made over a wet heathland in the vicinity ( 10%). Corrections were applied using a local-scale dispersion-exchange model. The analysis highlights how advection modifies the classical one-dimensional inferential resistance approach. It is concluded that ecosystems in the vicinity of agricultural land receive more dry deposition than would be estimated using NH3 concentration monitoring and standard inferential models. In the present study, this effect represented an overall increase in total NH3 deposition of 32%.

A new resistance model is described to interpret the biosphere-atmosphere exchange fluxes of ammonia (NH 3 ) with vegetation, and compared with previous modelling approaches for NH 3 . The new model constitutes an extension of an existing one-layer canopy compensation point model: in addition to bi-directional foliar stomatal exchange and deposition to leaf cuticles, the model treats NH 3 emission from a ground layer. This may originate from fertilizer evaporation, the soil or decomposing plant parts. The emission potentials of the foliage and ground Surface are given by the NH 3 gas concentrations at equilibrium with the ammonium (NH + 4 ) concentration in the apoplastic fluid or soil solution. From these concentrations, as well as the transfer resistances of the different exchange pathways, the net compensation point of the canopy (X c ) may be derived. The net flux is determined by the relative magnitude of X c and the NH 3 air concentration above the vegetation. The two-layer canopy compensation point is applied to: (i) an oilseed rape canopy, in which NH 3 emission from decomposing leaf litter at the ground surface presents a second major source; and (ii) a wheat stubble field, in which emission from the soil contributes significantly to the net exchange. For both canopies, the model performance is contrasted with the single-layer X c model, which is not able to reproduce the temporal patterns of exchange. The two-layer model is proposed as the optimum compromise between simplicity and accuracy, capable of describing bi-directional NH 3 exchange in atmospheric transport models over a very wide range of vegetation types.

Existing descriptions of bi-directional ammonia (NH 3 ) 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 NH 3 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 NH 3 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 NH 3 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 NH 3 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 NH 3 emissions may increase from 65 (45–85) Tg N in 2008 to reach 132 (89–179) Tg by 2100.

The net ecosystem carbon dioxide (CO2) exchange (NEE) of nine European mountain grassland ecosystems was measured during 2002–2004 using the eddy covariance method. Overall, the availability of photosynthetically active radiation (PPFD) was the single most important abiotic influence factor for NEE. Its role changed markedly during the course of the season, PPFD being a better predictor for NEE during periods favorable for CO2 uptake, which was spring and autumn for the sites characterized by summer droughts (southern sites) and (peak) summer for the Alpine and northern study sites. This general pattern was interrupted by grassland management practices, that is, mowing and grazing, when the variability in NEE explained by PPFD decreased in concert with the amount of aboveground biomass (BMag). Temperature was the abiotic influence factor that explained most of the variability in ecosystem respiration at the Alpine and northern study sites, but not at the southern sites characterized by a pronounced summer drought, where soil water availability and the amount of aboveground biomass were more or equally important. The amount of assimilating plant area was the single most important biotic variable determining the maximum ecosystem carbon uptake potential, that is, the NEE at saturating PPFD. Good correspondence, in terms of the magnitude of NEE, was observed with many (semi-) natural grasslands around the world, but not with grasslands sown on fertile soils in lowland locations, which exhibited higher maximum carbon gains at lower respiratory costs. It is concluded that, through triggering rapid changes in the amount and area of the aboveground plant matter, the timing and frequency of land management practices is crucial for the short-term sensitivity of the NEE of the investigated mountain grassland ecosystems to climatic drivers.

[1] Ammonia emissions were measured from two entire seabird colonies with contrasting species assemblages, to ascertain the ammonia volatilisation potentials among seabird species in relation to their nesting behaviour. Emissions were calculated from downwind plume measurements of ammonia concentration using both inverse dispersion and tracer ratio methods. Measured colony emissions ranged 1–90 kg NH3 hour−1, and equated to 16 and 36% volatilization of excreted nitrogen for colonies dominated by ground/burrow nesting and bare rock nesting birds, respectively. The results were applied in a bioenergetics model with a global seabird database. Seabird colonies are found to represent the largest point sources of ammonia globally (up to ∼6 Gg NH3 colony−1 year−1). Moreover the largest emissions occur mainly in remote environments with otherwise low NH3 emissions. These ammonia “hot spots” explain significant perturbations of the nitrogen cycle in these regions and add ∼20% to oceanic ammonia emissions south of latitude 45°S.

The MODDAS-2D model (MOdel of Dispersion and Deposition of Ammonia over the Short-range in two dimensions) is presented. This stationary model couples a two-dimensional Lagrangian stochastic model for short-range dispersion, with a leaf-scale bi-directional exchange model for ammonia (NH3), which includes cuticular uptake and a stomatal compensation point. The coupling is obtained by splitting the upward and downward components of the flux, which can be generalized for any trace gas, and hence provides a way of simply incorporating bi-directional exchanges in existing deposition velocity models. The leaf boundary-layer resistance is parametrized to account for mixed convection in the canopy, and the model incorporates a stability correction for the Lagrangian time-scale for vertical velocity, which tends to increase the Lagrangian time-scale in very stable conditions compared with usual parametrizations. The model is validated against three datasets, where concentrations of atmospheric NH3 were measured at several distances from a line source. Two datasets are over grassland and one is over maize, giving a range of canopy structure. The model correctly simulates the concentration in one situation, but consistently overestimates it at further distances or underestimates it at small distances in the two other situations. It is argued that these discrepancies are mainly due to the lack of length of one of the line sources and non-aligned winds. Analysis shows that the surface exchange parameters and the turbulent mixing at the source level are the predominant factors controlling short-range deposition of NH3. Copyright © 2006 Royal Meteorological Society

Exchange of atmospheric ammonia (NH 3 ) with vegetation is characterized by the juxtaposition of sources and sinks at a landscape level. Such situations lead to a large fraction of the landscape being exposed to local advection effects that if not accounted for, introduce errors in standard micrometeorological measurements of NH 3 exchange with the surface. In this study, a simplified dispersion - exchange model for NH 3 (Flux Interpretation by Dispersion and Exchange over Short Range, FIDES) is evaluated and used to assess the advection fluxes at 260 m downwind of an isolated pasture, grazed with sheep, using the measurements of a classical three-point NH 3 gradient system located on adjacent moorland. The method consists of fitting the measured and modeled concentration profile by adjusting at the same time the emission strength of the local source and the exchange rate of NH 3 to the moorland area downwind. A local dispersion and surface exchange model such as FIDES has proved to be a valuable tool to estimate advection corrections, given sound estimates of background NH 3 concentrations, source location, and standard meteorological parameters. According to the model results the advection fluxes at the moorland measurement site, at 1.0 m height and 260 m downwind of the grazed pasture, were positive. For 80% of the situations they ranged between 30% and 60% of the vertical fluxes. In stable conditions the advection fluxes were large and more sensitive to the surface exchange parameters. These results demonstrate that if not accounted for, advection fluxes may lead to a severe underestimate of the NH3 deposition to seminatural ecosystems, such as moorland, in the vicinity of ground level agricultural sources.