Improved data on biosphere-atmosphere exchange are fundamental to understanding the production and fate of ammonia (NH3) in the atmosphere. The GRAMINAE Integrated Experiment combined novel... Show moreImproved data on biosphere-atmosphere exchange are fundamental to understanding the production and fate of ammonia (NH3) in the atmosphere. The GRAMINAE Integrated Experiment combined novel measurement and modelling approaches to provide the most comprehensive analysis of the interactions to date. Major inter-comparisons of micrometeorological parameters and NH3 flux measurements using the aerodynamic gradient method and relaxed eddy accumulation (REA) were conducted. These showed close agreement, though the REA systems proved insufficiently precise to investigate vertical flux divergence. Grassland management had a large effect on fluxes: emissions increased after grass cutting (-50 to 700 ng m(-2) s(-1) NH3) and after N-fertilization (0 to 3800 ng m(-2) s(-1)) compared with before the cut (-60 to 40 ng m(-2) s(-1)).Effects of advection and air chemistry were investigated using horizontal NH3 profiles, acid gas and particle flux measurements. Inverse modelling of NH3 emission from an experimental farm agreed closely with inventory estimates, while advection errors were used to correct measured grassland fluxes. Advection effects were caused both by the farm and by emissions from the field, with an inverse dispersion-deposition model providing a reliable new approach to estimate net NH3 fluxes. Effects of aerosol chemistry on net NH3 fluxes were small, while the measurements allowed NH3-induced particle growth rates to be calculated and aerosol fluxes to be corrected.Bioassays estimated the emission potential I" = [NH4+]/[H+] for different plant pools, with the apoplast having the smallest values (30-1000). The main within-canopy sources of NH3 emission appeared to be leaf litter and the soil surface, with I" up to 3 million and 300 000, respectively. Cuvette and within-canopy analyses confirmed the role of leaf litter NH3 emission, which, prior to cutting, was mostly recaptured within the canopy.Measured ammonia fluxes were compared with three models: an ecosystem model (PaSim), a soil vegetation atmosphere transfer model (SURFATM-NH3) and a dynamic leaf chemistry model (DCC model). The different models each reproduced the main temporal dynamics in the flux, highlighting the importance of canopy temperature dynamics (Surfatm-NH3), interactions with ecosystem nitrogen cycling (PaSim) and the role of leaf surface chemistry (DCC model). Overall, net above-canopy fluxes were mostly determined by stomatal and cuticular uptake (before the cut), leaf litter emissions (after the cut) and fertilizer and litter emissions (after fertilization). The dynamics of ammonia emission from leaf litter are identified as a priority for future research. Show less
Burkhardt, J.; Flechard, C.R.; Gresens, F.; Mattsson, M.; Jongejan, P.A.C.; Erisman, J.W.; ... ; Sutton, M.A. 2009
Ammonia exchange fluxes between grassland and the atmosphere were modelled on the basis of stomatal compensation points and leaf surface chemistry, and compared with measured fluxes during the... Show moreAmmonia exchange fluxes between grassland and the atmosphere were modelled on the basis of stomatal compensation points and leaf surface chemistry, and compared with measured fluxes during the GRAMINAE intensive measurement campaign in spring 2000 near Braunschweig, Germany. Leaf wetness and dew chemistry in grassland were measured together with ammonia fluxes and apoplastic NH4+ and H+ concentration, and the data were used to apply, validate and further develop an existing model of leaf surface chemistry and ammonia exchange. Foliar leaf wetness which is known to affect ammonia fluxes may be persistent after the end of rainfall, or sustained by recondensation of water vapour originating from the ground or leaf transpiration, so measured leaf wetness values were included in the model. pH and ammonium concentrations of dew samples collected from grass were compared to modelled values.The measurement period was divided into three phases: a relatively wet phase followed by a dry phase in the first week before the grass was cut, and a second drier week after the cut. While the first two phases were mainly characterised by ammonia deposition and occasional short emission events, regular events of strong ammonia emissions were observed during the post-cut period. A single-layer resistance model including dynamic cuticular and stomatal exchange could describe the fluxes well before the cut, but after the cut the stomatal compensation points needed to numerically match measured fluxes were much higher than the ones measured by bioassays, suggesting another source of ammonia fluxes. Considerably better agreement both in the direction and the size range of fluxes were obtained when a second layer was introduced into the model, to account for the large additional ammonia source inherent in the leaf litter at the bottom of the grass canopy. Therefore, this was found to be a useful extension of the mechanistic dynamic chemistry model by keeping the advantage of requiring relatively little site-specific information. Show less