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

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Lichens were recorded on Quercus petraea trunks and twigs near ammonia recording stations in ‘continental’ Norfolk, and ‘oceanic’ Devon in order to test indicator values developed for epiphytic lichens in areas of high atmospheric ammonia in the Netherlands. Lichens on trunks in Norfolk showed a similar correlation of nitrophyte indices with ammonia concentration and bark pH as those in Holland, whereas in Devon there was no correlation with nitrophyte indices on trunks and a negative correlation with acidophyte indices. Results on twigs in both sites suggest that lichens on twigs respond more rapidly to recent changes in ammonia concentrations while trunks may maintain relict lichen communities due to either a legacy of previous acidification or ecological continuity. The results suggest that loss of acidophytes is taking place prior to the establishment of nitrophytes indicating the importance of establishing levels of ammonia at which sensitive communities are at risk.

Abstract. The exchange of ammonia between crop canopies and the atmosphere depends on a range of plant parameters and climatic conditions. However, little is known about effects of management factors. We have here investigated the stomatal ammonia compensation point in response to cutting and fertilization of a grass sward dominated by Lolium perenne. Tall grass had a very low NH 3 compensation point (around 1 nmol mol −1 ), reflecting the fact that leaf nitrogen (N) concentration was very low. During re-growth after cutting, leaf tissue concentrations of NO concentration of the newly emerging leaves to increase dramatically. The NH 3 compensation point peaked between 15 and 25 nmol mol −1 the day after the fertiliser was applied and thereafter decreased over the following 10 days until reaching the same level as before fertilisation. Ammonium concentrations in leaf apoplast, bulk tissue and litter were positively correlated (P=0.001) throughout the experimental period. Bulk tissue NH

[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 NH 3 hour À1 , 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 NH 3 colony À1 year À1 ). Moreover the largest emissions occur mainly in remote environments with otherwise low NH 3 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.

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Abstract. A major international experiment on ammonia (NH3) biosphere-atmosphere exchange was conducted over intensively managed grassland at Braunschweig, Germany. The experimental strategy was developed to allow an integrated analysis of different features of NH3 exchange including: a) quantification of nearby emissions and advection effects, b) estimation of net NH3 fluxes with the canopy by a range of micrometeorological measurements, c) analysis of the sources and sinks of NH3 within the plant canopy, including soils and bioassay measurements, d) comparison of the effects of grassland management options on NH3 fluxes and e) assessment of the interactions of NH3 fluxes with aerosol exchange processes. Additional technical objectives included the inter-comparison of different estimates of sensible and latent heat fluxes, as well as continuous-gradient and Relaxed Eddy Accumulation (REA) systems for NH3 fluxes. The prior analysis established the spatial and temporal design of the experiment, allowing significant synergy between these objectives. The measurements were made at 7 measurement locations, thereby quantifying horizontal and vertical profiles, and covered three phases: a) tall grass canopy prior to cutting (7 days), b) short grass after cutting (7 days) and c) re-growing sward following fertilization with ammonium nitrate (10 days). The sequential management treatments allowed comparison of sources-sinks, advection and aerosol interactions under a wide range of NH3 fluxes. This paper describes the experimental strategy and reports the grassland management history, soils, environmental conditions and air chemistry during the experiment, finally summarizing how the results are coordinated in the accompanying series of papers.

Abstract. Quantification of ammonia (NH3) land-atmosphere exchange is required for atmospheric modelling and assessment of nitrogen deposition, yet flux measurement methods remain highly uncertain. To address this issue, a major inter-comparison of ammonia fluxes over intensively managed grassland was conducted during the GRAMINAE Integrated Experiment held in Braunschweig, Germany. In order to provide a robust dataset of ammonia exchange with the vegetation, four independent continuous flux gradient systems were operated. Three independently operated continuous wet denuders systems (AMANDA) were compared with a Wet Effluent Diffusion Denuder (mini-WEDD) system. Measurements were made at two distances from an adjacent livestock farm, allowing effects of advection to be quantified in a real landscape setting. Data treatment included filtering for instrument failure, disturbed wind sectors and unsuitable micrometeorological conditions, with corrections made for storage and advection errors. The inter-comparison demonstrated good agreement in measured ammonia concentrations and fluxes (<20% difference) for some periods, although the performance of the ammonia analyzers was variable, with much poorer agreement on particular days. However, by using four systems, the inter-comparison was able to provide a robust mean estimate of continuous ammonia fluxes through the experiment. The observed fluxes were: a) small bi-directional fluxes prior to cutting (−64 to 42 ng NH3 m−2 s−1), b) larger diurnally-varying emissions following cutting (−49 to 703 ng NH3 m−2 s−1) and c) much larger emissions following fertilizer application (0 to 3820 ng NH3 m−2 s−1). The results are a salutary reminder of the uncertainty in unreplicated ammonia flux measurements, while the replication of the present study provides a uniquely robust dataset for the evaluation of ammonia exchange processes. It is clear that consistently reliable determination of ammonia concentrations remains the major measurement challenge.