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Jesse O. Bash and David R. Miller


A relaxed eddy accumulation (REA) system was designed to continuously measure total gaseous mercury (TGM) fluxes over a forest canopy. TGM concentration measurements were measured at 5-min intervals with a Tekran model 2537A mercury analyzer located above the forest canopy on a walk-up meteorological tower. Ten-minute averages for up- and downdraft mercury concentrations were used to calculate the flux. The multiresolution decomposition technique was used to determine day- and nighttime averaging periods for the turbulent statistics used in the REA technique. This paper documents the REA system for mercury flux measurements and its use over a forest canopy.

The REA system response to the averaging times for the turbulent statistics and corrections to up- and downdraft concentrations are major considerations when using the technique with the Tekran mercury analyzer over a forest canopy. TGM flux data collected from 18 August to 12 September 2005 are used here to demonstrate the capabilities of the REA system to measure both short- (1-h time periods) and long-term flux dynamics. During the demonstration period the TGM median flux was 21.9 ± 32.6 ng m−2 h−1 and the median atmospheric TGM concentrations were 1.34 ± 0.13 ng m−2 h−1. Maximum short-term TGM evasive fluxes occurred during the daylight hours with minimums during the nighttime. A consistent bimodal emission pattern was observed during the daytime emissions over the canopy. The first peak occurred immediately following the evaporation of the nighttime dew on the canopy and the second peak occurred in the late afternoon.

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Jesse O. Bash, Patricia Bresnahan, and David R. Miller


This paper presents a review of recent natural surface mercury exchange research in the context of a new modeling framework. The literature indicates that the mercury biogeochemical flux is more dynamic than the current models predict, with interacting multimedia storage and processes. Although several natural mercury emissions models have been created and incorporated into air quality models (AQMs), none are coupled with air quality models on a mass balance basis, and all lack the capacity to explain processes that involve the transport of mercury across atmosphere–surface media concentration gradients. Existing natural mercury emission models treat the surface as both an infinite source and infinite sink for emissions and deposition, respectively, and estimate emissions through the following three pathways: soil, vegetation, and surface waters. The use of these three transport pathways, but with compartmentalized surface storage in a surface–vegetation–atmosphere transport (SVAT) resistance model, is suggested. Surface water fluxes will be modeled using a two-film diffusion model coupled to a surface water photochemical model. This updated framework will allow both the parameterization of the transport of mercury across atmosphere–surface media concentration gradients and the accumulation/depletion of mercury in the surface media. However, several key parameters need further experimental verification before the proposed modeling framework can be implemented in an AQM. These include soil organic mercury interactions, bioavailability, cuticular transport of mercury, atmospheric surface compensation points for different vegetation species, and enhanced soil diffusion resulting from pressure perturbations.

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