To simulate global mercury (Hg) dynamics in chemical transport models (CTMs), surface-atmosphere exchange of gaseous elemental mercury, Hg 0 , is often parameterized based on resistance-based dry deposition schemes coupled with a re-emission function, mainly from soils. Despite extensive use of this approach, direct evaluations of this implementation against field observations of net Hg 0 exchange are lacking. In this study, we evaluate an existing net exchange parameterization (referred to here as the base model) by comparing modeled fluxes of Hg 0 to fluxes measured in the field using micrometeorological techniques. Comparisons were performed in two terrestrial ecosystems: a grassland site in Switzerland and an Arctic tundra site in Alaska, U.S., each including summer and winter seasons. The base model included the dry deposition and soil re-emission parameterizations from Zhang et al. (2003) and the global CTM GEOS-Chem, respectively. Comparisons of modeled and measured Hg 0 fluxes showed large discrepancies, particularly in the summer months when the base model overestimated daytime net deposition by approximately 9 and 2 ng m −2 h −1 at the grassland and tundra sites, respectively. In addition, the base model was unable to capture a measured nighttime net Hg 0 deposition and wintertime deposition. We conducted a series of sensitivity analyses and recommend that Hg simulations using CTMs: (i) reduce stomatal uptake of Hg 0 over grassland and tundra in models by a factor 5–7; (ii) increase nighttime net Hg 0 deposition, e.g. , by increasing ground and cuticular uptake by reducing the respective resistance terms by factors of 3–4 and 2–4, respectively; and (iii) implement a new soil re-emission parameterization to produce larger daytime emissions and lower nighttime emissions. We also compared leaf Hg 0 uptake over the growing season estimated by the dry deposition model against foliar Hg measurements, which revealed good agreement with the measured leaf Hg concentrations after adjusting the base model as suggested above. We conclude that the use of resistance-based models combined with the new soil re-emission flux parameterization is able to reproduce observed diel and seasonal patterns of Hg 0 exchange in these ecosystems. This approach can be used to improve model parameterizations for other ecosystems if flux measurements become available.
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Ozone dry deposition through plant stomata: multi-model comparison with flux observations and the role of water stress as part of AQMEII4 Activity 2
Abstract. A substantial portion of tropospheric O3 dry deposition occurs after diffusion of O3 through plant stomata. Simulating stomatal uptake of O3 in 3D atmospheric chemistry models is important in the face of increasing drought-induced declines in stomatal conductance and enhanced ambient O3. Here, we present a comparison of the stomatal component of O3 dry deposition (egs) from chemical transport models and estimates of egs from observed CO2, latent heat, and O3 flux. The dry deposition schemes were configured as single-point models forced with data collected at flux towers. We conducted sensitivity analyses to study the impact of model parameters that control stomatal moisture stress on modeled egs. Examining six sites around the Northern Hemisphere, we find that the seasonality of observed flux-based egs agrees with the seasonality of simulated egs at times during the growing season, with disagreements occurring during the later part of the growing season at some sites. We find that modeled water stress effects are too strong in a temperate–boreal transition forest. Some single-point models overestimate summertime egs in a seasonally water-limited Mediterranean shrubland. At all sites examined, modeled egs was sensitive to parameters that control the vapor pressure deficit stress. At specific sites that experienced substantial declines in soil moisture, the simulation of egs was highly sensitive to parameters that control the soil moisture stress. The findings demonstrate the challenges in accurately representing the effects of moisture stress on the stomatal sink of O3 during observed increases in dryness due to ecosystem-specific plant–resource interactions.
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- PAR ID:
- 10664860
- Author(s) / Creator(s):
- ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more »
- Publisher / Repository:
- Copernicus Publications
- Date Published:
- Journal Name:
- Atmospheric Chemistry and Physics
- Volume:
- 25
- Issue:
- 15
- ISSN:
- 1680-7324
- Page Range / eLocation ID:
- 8613 to 8635
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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