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Wolff, V; Trebs, I; Moravek, A; Zhu, Z; Meixner, FX: Concentrations and fluxes of water-soluble reactive nitrogen gases and aerosol compounds above a forest canopy
Vortrag, AGU, San Francisco: 15.12.2008 - 19.12.2008

Abstract:
In summer 2007 we measured concentration gradients of NH3, HNO3, HONO and related aerosol species NH4+ and NO3- as well as SO2, and aerosol SO42- above a spruce canopy in south-east Germany (50°09’N, 11°52’E, 775m asl). Measurements were performed as part of an intensive observation period within the framework of the EGER (ExchanGE processes in mountainous Regions) project. NH3, HNO3, HONO, SO2, aerosol NH4+, aerosol NO3-, and aerosol SO42- were measured using the Gradient Analyzer for Aerosols and Gases, mounted on a tower. Water-soluble gases and aerosol species were collected simultaneously at two different heights by two rotating wet-annular denuders and two Steam-Jet Aerosol Collectors, respectively. Samples were analysed on-line via ion chromatography and flow injection analysis. To our knowledge this was the first time that these gas and aerosol species were measured simultaneously and with high time resolution (30 min) above a forest canopy. Data accuracy and precision is provided by a rigorous data screening, including the use of an internal standard, careful error estimation and repeated in-field blanks. Gradient precision of the measurements are derived from extended periods of side-by-side sampling of the sample boxes (n = 257). NH3 mixing ratios reached their maximum in the late afternoon with 2 to 3 ppb and their minimum in morning hours with 0.25 ppb, whereas aerosol NH4+ mirrored this behaviour with maximum values late night and early morning with 4 up to 8 ppb and minimum values in the afternoon, around 0.5 ppb and less. HNO3 and aerosol NO3- diel cycles also mirrored each other, HNO3 maxima during late afternoon ( above 1 ppb) and minimum during night and early morning with less than 0.2 ppb and aerosol NO3- maxima during night ( around 2 ppb, up to 6 ppb) and minima during afternoons with 0.5 ppb. Patterns of aerosol NH4+ and aerosol NO3- in the time series are apparently closely related. NH3 gradients indicate bidirectional fluxes, whereas HNO3 gradients are indicating net deposition. These gradients may be biased by micrometeorology and chemistry. For example, gradients in NH3 and HNO3 may be product of a phase change in the thermodynamic equilibrium between NH3, HNO3 and particulate NH4NO3, induced by a temperature and/or humidity gradient above the forest canopy. The equilibrium will be investigated for the pure NH3-HNO3-NH4NO3 triad as well as for more complex inorganic aerosol mixtures and chemical timescales will be compared to turbulent timescales, to estimate the potential of chemical interferences affecting the gradient. If compounds react sufficiently slow and may therefore be treated as passive tracers, prerequisites for the application of micrometeorological methods to derive fluxes from gradients will be investigated.

Letzte Änderung 31.10.2008