Effects of aerosol dynamics and gas–particle conversion on dry deposition of inorganic reactive nitrogen in a temperate forest

摘要

Dry deposition has an impact on nitrogen status in forest environments. However, the mechanism for the high dry-deposition rates of fine nitrate particles (NO3-) observed in forests remains unknown and is thus a potential source of error in chemical transport models (CTMs). Here, we modified and applied a multilayer land surface model coupled with dry-deposition and aerosol dynamic processes for a temperate mixed forest in Japan. This represents the first application of such a model to ammonium nitrate (NH4NO3) gas–particle conversion (gpc) and the aerosol water uptake of reactive nitrogen compounds. Thermodynamics, kinetics, and dry deposition for mixed inorganic particles are modeled by a triple-moment modal method. Data for inorganic mass and size-resolved total number concentrations measured by a filter pack and electrical low-pressure impactor in autumn were used for model inputs and subsequent numerical analysis. The model successfully reproduces turbulent fluxes observed above the canopy and vertical micrometeorological profiles noted in our previous studies. The sensitivity tests with and without gpc demonstrated clear changes in the inorganic mass and size-resolved total number concentrations within the canopy. The results also revealed that within-canopy evaporation of NH4NO3 under dry conditions significantly enhances the deposition flux of fine-NO3- and fine-NH4+ particles, while reducing the deposition flux of nitric acid gas (HNO3). As a result of the evaporation of particulate NH4NO3, the calculated daytime mass flux of fine NO3- over the canopy was 15 times higher in the scenario of “gpc” than in the scenario of “no gpc”. This increase caused high contributions from particle deposition flux (NO3- and NH4+) to total nitrogen flux over the forest ecosystem (～39%), although the contribution of NH3 was still considerable. A dry-deposition scheme coupled with aerosol dynamics may be required to improve the predictive accuracy of chemical transport models for the surface concentration of inorganic reactive nitrogen.