The exchange of Ammonia (NH3) between grassland and the atmosphere was determined using Relaxed Eddy Accumulation (REA) measurements. The use of REA is of special interest for NH3, since the... Show moreThe exchange of Ammonia (NH3) between grassland and the atmosphere was determined using Relaxed Eddy Accumulation (REA) measurements. The use of REA is of special interest for NH3, since the determination of fluxes at one height permits multiple systems to be deployed to quantify vertical flux divergence (either due to effects of chemical production or advection). During the Braunschweig integrated experiment four different continuous-sampling REA systems were operated during a period of about 10 days and were compared against a reference provided by independent application of the Aerodynamic Gradient Method (AGM). The experiment covered episodes before and after both cutting and fertilizing and provided a wide range of fluxes -60-3600 ng NH3 m(-2) s(-1) for testing the REA systems. The REA systems showed moderate to good correlation with the AGM estimates, with r(2) values for the linear regressions between 0.3 and 0.82. For the period immediately after fertilization, the REA systems showed average fluxes 20% to 70% lower than the reference. At periods with low fluxes REA and AGM can agree within a few %. Overall, the results show that the continuous REA technique can now be used to measure NH3 surface exchange fluxes. While REA requires greater analytical precision in NH3 measurement than the AGM, a key advantage of REA is that reference sampling periods can be introduced to remove bias between sampling inlets. However, while the data here indicate differences consistent with advection effects, significant improvements in sampling precision are essential to allow robust determination of flux divergence in future studies. Wet chemical techniques will be developed further since they use the adsorptive and reactive properties of NH3 that impedes development of cheaper optical systems. Show less
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... Show moreA 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. Show less
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
