Advances in understanding, models and parameterizations of biosphere-atmosphere ammonia exchange

Abstract. Atmospheric ammonia (NH₃) dominates global emissions of total reactive nitrogen (N_r), while emissions from agricultural production systems contribute about two-thirds of global NH₃ emissions; the remaining third emanates from oceans, natural vegetation, humans, wild animals and biomass burning. On land, NH₃ emitted from the various sources eventually returns to the biosphere by dry deposition to sink areas, predominantly semi-natural vegetation, and by wet and dry deposition as ammonium (NH₄⁺) to all surfaces. However, the land/atmosphere exchange of gaseous NH₃ is in fact bi-directional over unfertilized as well as fertilized ecosystems, with periods and areas of emission and deposition alternating in time (diurnal, seasonal) and space (patchwork landscapes). The exchange is controlled by a range of environmental factors, including meteorology, surface layer turbulence, thermodynamics, air and surface heterogeneous-phase chemistry, canopy geometry, plant development stage, leaf age, organic matter decomposition, soil microbial turnover, and, in agricultural systems, by fertilizer application rate, fertilizer type, soil type, crop type, and agricultural management practices. We review the range of processes controlling NH₃ emission and uptake in the different parts of the soil-canopy-atmosphere continuum, with NH₃ emission potentials defined at the substrate and leaf levels by different [NH₄⁺] / [H⁺] ratios (Γ). Surface/atmosphere exchange models for NH₃ are necessary to compute the temporal and spatial patterns of emissions and deposition at the soil, plant, field, landscape, regional and global scales, in order to assess the multiple environmental impacts of airborne and deposited NH₃ and NH₄⁺. Models of soil/vegetation/atmosphere NH₃ exchange are reviewed from the substrate and leaf scales to the global scale. They range from simple steady-state, "big leaf" canopy resistance models, to dynamic, multi-layer, multi-process, multi-chemical species schemes. Their level of complexity depends on their purpose, the spatial scale at which they are applied, the current level of parameterization, and the availability of the input data they require. State-of-the-art solutions for determining the emission/sink Γ potentials through the soil/canopy system include coupled, interactive chemical transport models (CTM) and soil/ecosystem modelling at the regional scale. However, it remains a matter for debate to what extent realistic options for future regional and global models should be based on process-based mechanistic versus empirical and regression-type models. Further discussion is needed on the extent and timescale by which new approaches can be used, such as integration with ecosystem models and satellite observations.