Estimating sources, sinks and fluxes of reactive atmospheric compounds within a forest canopy

While few dispute the significance of within-canopy sources or sinks of reactive gaseous and particulate compounds, their estimation continues to be the subject of active research and debate. Reactive species undergo turbulent dispersion within an inhomogeneous flow field, and may be subjected to chemical, biological and/or physical deposition, emissions or transformations on leaves, woody elements, and the forest floor. This system involves chemical reactions and biological processes with multiple time scales and represents the terrestrial ecosystem's exposure to nutrient and acid deposition and atmospheric oxidants. The quantification of these processes is a first step in better understanding the ecological impact of air pollution and feedback to atmospheric composition. Hence, it follows that direct measurements of sources or sinks is difficult to conduct in the presence of all these processes. However, mean scalar concentration profiles measured within the canopy can be used to infer the profile distribution of effective sinks and sources if the flow field is known. This is commonly referred to as the 'inverse problem'. In-canopy and above-canopy multi-level concentration measurements of reactive nitrogen compounds (ammonia, nitric acid, nitrous acid), as well as other compounds that are highly reactive to ammonia and its secondary products (hydrochloric acid and sulfur dioxide), are presented within a deciduous second-growth 180 year old oak-hickory forest situated within the Southeastern U.S. Two different approaches are used to solve for the source-sink distribution from the measured mean scalar concentration profiles: (1) an Eulerian high-order closure model that solves the scalar flux budget equation and (2) a new Lagrangian stochastic model that estimates the dispersion matrix. As each of these methods is subject to different assumptions, the combination of the two can be used to constrain the solution to the inverse problem and permit inference on the fate of reactive compounds within forested vegetation.