Abstract. Recent advances in laser spectrometry offer new opportunities to investigate ecosystem–atmosphere exchange of environmentally relevant trace gases. In this study, we demonstrate the applicability of a quantum cascade laser (QCL) absorption spectrometer to continuously measure ammonia concentrations at high time resolution and thus to quantify the net exchange between a seminatural peatland ecosystem and the atmosphere based on the eddy-covariance approach. Changing diurnal patterns of both ammonia concentration and fluxes were found during different periods of the campaign. We observed a clear tipping point in early spring with decreasing ammonia deposition velocities and increasingly bidirectional fluxes that occurred after the switch from dormant vegetation to CO2 uptake but was triggered by a significant weather change. While several biophysical parameters such as temperature, radiation, and surface wetness were identified to partially regulate ammonia exchange at the site, the seasonal concentration pattern was clearly dominated by agricultural practices in the surrounding area. Comparing the results of a compensation point model with our measurement-based flux estimates showed considerable differences in some periods of the campaign due to overestimation of non-stomatal resistances caused by low acid ratios. The total cumulative campaign exchange of ammonia after 9 weeks, however, differed only in a 6 % deviation with 911 and 857 g NH3-N ha−1 deposition being found by measurements and modeling, respectively. Extrapolating our findings to an entire year, ammonia deposition was lower than reported by Hurkuck et al. (2014) for the same site in previous years using denuder systems. This was likely due to a better representation of the emission component in the net signal of eddy-covariance fluxes as well as better adapted site-specific parameters in the model. Our study not only stresses the importance of high-quality measurements for studying and assessing land surface–atmosphere interactions but also demonstrates the potential of QCL spectrometers for continuous observation of reactive nitrogen species as important additional instruments within long-term monitoring research infrastructures such as ICOS or NEON at sites with strong nearby ammonia sources leading to relatively high mean background concentrations and fluxes.
Abstract. The accurate representation of bidirectional ammonia (NH3) biosphere–atmosphere exchange is an important part of modern air quality models. However, the cuticular (or external leaf surface) pathway, as well as other non-stomatal ecosystem surfaces, still pose a major challenge to translating our knowledge into models. Dynamic mechanistic models including complex leaf surface chemistry have been able to accurately reproduce measured bidirectional fluxes in the past, but their computational expense and challenging implementation into existing air quality models call for steady-state simplifications. Here we qualitatively compare two semi-empirical state-of-the-art parameterizations of a unidirectional non-stomatal resistance (Rw) model after Massad et al. (2010), and a quasi-bidirectional non-stomatal compensation-point (χw) model after Wichink Kruit et al. (2010), with NH3 flux measurements from five European sites. In addition, we tested the feasibility of using backward-looking moving averages of air NH3 concentrations as a proxy for prior NH3 uptake and as a driver of an alternative parameterization of non-stomatal emission potentials (Γw) for bidirectional non-stomatal exchange models. Results indicate that the Rw-only model has a tendency to underestimate fluxes, while the χw model mainly overestimates fluxes, although systematic underestimations can occur under certain conditions, depending on temperature and ambient NH3 concentrations at the site. The proposed Γw parameterization revealed a clear functional relationship between backward-looking moving averages of air NH3 concentrations and non-stomatal emission potentials, but further reduction of uncertainty is needed for it to be useful across different sites. As an interim solution for improving flux predictions, we recommend reducing the minimum allowed Rw and the temperature response parameter in the unidirectional model and revisiting the temperature-dependent Γw parameterization of the bidirectional model.
Long-term monitoring stations for atmospheric pollutants are often equipped with low-resolution concentration samplers. In this study, we analyse the errors associated with using monthly average ammonia concentrations as input variables for bidirectional biosphere-atmosphere exchange models, which are commonly used to estimate dry deposition fluxes. Previous studies often failed to account for a potential correlation between ammonia exchange velocities and ambient concentrations. We formally derive the exact magnitude of these errors from statistical considerations and propose a correction scheme based on parallel measurements using high-frequency analysers. In case studies using both modelled and measured ammonia concentrations and micrometeorological drivers from sites with varying pollution levels, we were able to substantially reduce bias in the predicted ammonia fluxes. Neglecting to account for these errors can, in some cases, lead to significantly biased deposition estimates compared to using high-frequency instrumentation or corrected averaging strategies. Our study presents a first step towards a unified correction scheme for data from nation-wide air pollutant monitoring networks to be used in chemical transport and air quality models.
<p><strong>Abstract.</strong> The accurate representation of bidirectional ammonia (NH<sub>3</sub>) biosphere-atmosphere exchange is an important part of modern air quality models. However, the cuticular (or external leaf surface) pathway, as well as other non-stomatal ecosystem surfaces, still pose a major challenge of translating our knowledge into models. Dynamic mechanistic models including complex leaf surface chemistry have been able to accurately reproduce measured bidirectional fluxes in the past, but their computational expense and challenging implementation into existing air quality models call for steady-state simplifications. We here qualitatively compare two semi-empirical state-of-the-art parameterizations of a unidirectional non-stomatal resistance (<i>R</i><sub>w</sub>) model after Massad et al. (2010), and a quasi-bidirectional non-stomatal compensation point (&#967;<sub>w</sub>) model after Wichink Kruit et al. (2010), with NH<sub>3</sub> flux measurements from five European sites. In addition, we tested the feasibility of using backward-looking moving averages of air NH<sub>3</sub> concentrations as a proxy for prior NH<sub>3</sub> uptake and driver of an alternative parameterization of non-stomatal emission potentials (&#915;<sub>w</sub>) for bidirectional non-stomatal exchange models. Results indicate that the <i>R</i><sub>w</sub>-only model has a tendency to underestimate fluxes, while the &#967;<sub>w</sub> model mainly overestimates fluxes, although systematic underestimations can occur under certain conditions, depending on temperature and ambient NH<sub>3</sub> concentrations at the site. The proposed &#915;<sub>w</sub> parameterization appears to have potential for improvement, but cannot be recommended for use in large scale simulations in its present state due to large uncertainties. As an interim solution for improving flux predictions, we recommend to reduce the minimum allowed <i>R</i><sub>w</sub> and the temperature response parameter in the unidirectional model and to revisit the temperature dependent &#915;<sub>w</sub> parameterization of the bidirectional model.</p>
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