scholarly journals Non-stomatal exchange in ammonia dry deposition models: comparison of two state-of-the-art approaches

2016 ◽  
Vol 16 (21) ◽  
pp. 13417-13430 ◽  
Author(s):  
Frederik Schrader ◽  
Christian Brümmer ◽  
Chris R. Flechard ◽  
Roy J. Wichink Kruit ◽  
Margreet C. van Zanten ◽  
...  

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.

2016 ◽  
Author(s):  
Frederik Schrader ◽  
Christian Brümmer ◽  
Chris R. Flechard ◽  
Roy J. Wichink Kruit ◽  
Margreet C. van Zanten ◽  
...  

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 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 (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 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 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 Rw and the temperature response parameter in the unidirectional model and to revisit the temperature dependent Γw parameterization of the bidirectional model.


2003 ◽  
Vol 3 (6) ◽  
pp. 2067-2082 ◽  
Author(s):  
L. Zhang ◽  
J. R. Brook ◽  
R. Vet

Abstract. A parameterization scheme for calculating gaseous dry deposition velocities in air-quality models is revised based on recent study results on non-stomatal uptake of O3 and SO2 over 5 different vegetation types. Non-stomatal resistance, which includes in-canopy aerodynamic, soil and cuticle resistances, for SO2 and O3 is parameterized as a function of friction velocity, relative humidity, leaf area index, and canopy wetness. Non-stomatal resistance for other chemical species is scaled to those of SO2 and O3 based on their chemical and physical characteristics. Stomatal resistance is calculated using a two-big-leaf stomatal resistance sub-model for all gaseous species of interest. The improvements in the present model compared to its earlier version include a newly developed non-stomatal resistance formulation, a realistic treatment of cuticle and ground resistance in winter, and the handling of seasonally-dependent input parameters. Model evaluation shows that the revised parameterization can provide more realistic deposition velocities for both O3 and SO2, especially for wet canopies. Example model output shows that the parameterization provides reasonable estimates of dry deposition velocities for different gaseous species, land types and diurnal and seasonal variations. Maximum deposition velocities from model output are close to reported measurement values for different land types. The current parameterization can be easily adopted into different air-quality models that require inclusion of dry deposition processes.


2003 ◽  
Vol 3 (2) ◽  
pp. 1777-1804 ◽  
Author(s):  
L. Zhang ◽  
J. R. Brook ◽  
R. Vet

Abstract. A parameterization scheme for calculating gaseous dry deposition velocities in air-quality models is revised based on recent study results on non-stomatal uptake of O3 and SO2 over 5 different vegetation types. Non-stomatal resistance, which includes in-canopy aerodynamic resistance, soil resistance and cuticle resistance, for SO2 and  O3 is parameterized as a function of friction velocity, relative humidity, leaf area index, and canopy wetness. Non-stomatal resistance for all other species is scaled to those of SO2 and  O3 based on their chemical and physical characteristics. Stomatal resistance is calculated using a leaf-stomatal-resistance model for all gaseous species of interest. The improvements in the present model compared to its earlier version include a newly developed non-stomatal resistance formulation, a realistic treatment of cuticle and ground resistance in winter and the handling of seasonally-dependent input parameters. Model evaluation shows that the revised parameterization can provide more realistic deposition velocities for both  O3 and SO2, especially for wet canopies. Example model output shows that the parameterization provides reasonable estimates of dry deposition velocities for different gaseous species, land types and diurnal and seasonal variations. Maximum deposition velocities from model output are close to reported measurement values for different land types. The current parameterization can be easily adopted into different air-quality models that require inclusion of dry deposition processes.


2014 ◽  
Vol 7 (3) ◽  
pp. 1001-1024 ◽  
Author(s):  
P. A. Makar ◽  
R. Nissen ◽  
A. Teakles ◽  
J. Zhang ◽  
Q. Zheng ◽  
...  

Abstract. The balance between turbulent transport and emissions is a key issue in understanding the formation of O3 and particulate matter with diameters less than 2.5 μm (PM2.5). Discrepancies between observed and simulated concentrations for these species have, in the past, been ascribed to insufficient turbulent mixing, particularly for atmospherically stable environments. This assumption may be simplistic – turbulent mixing deficiencies may explain only part of these discrepancies, and as turbulence parameterizations are improved, the timing of primary PM2.5 emissions may play a much more significant role in the further reduction of model error. In a study of these issues, two regional air-quality models, the Community Multi-scale Air Quality model (CMAQ, version 4.6) and A Unified Regional Air-quality Modelling System (AURAMS, version 1.4.2), were compared to observations for a domain in north-western North America. The air-quality models made use of the same emissions inventory, emissions processing system, meteorological driving model, and model domain, map projection and horizontal grid, eliminating these factors as potential sources of discrepancies between model predictions. The initial statistical comparison between the models and monitoring network data showed that AURAMS' O3 simulations outperformed those of this version of CMAQ4.6, while CMAQ4.6 outperformed AURAMS for most PM2.5 statistical measures. A process analysis of the models revealed that many of the differences between the models' results could be attributed to the strength of turbulent diffusion, via the choice of an a priori lower limit in the magnitude of vertical diffusion coefficients, with AURAMS using 0.1 m2 s−1 and CMAQ4.6 using 1.0 m2 s−1. The use of the larger CMAQ4.6 value for the lower limit of vertical diffusivity within AURAMS resulted in a similar performance for the two models (with AURAMS also showing improved PM2.5, yet degraded O3, and a similar time series as CMAQ4.6). The differences between model results were most noticeable at night, when the higher minimum turbulent diffusivity resulted in an erroneous secondary peak in predicted night-time O3. A spatially invariant and relatively high lower limit in diffusivity could not reduce errors in both O3 and PM2.5 fields, implying that other factors aside from the strength of turbulence might be responsible for the PM2.5 over-predictions. Further investigation showed that the magnitude, timing and spatial allocation of area source emissions could result in improvements to PM2.5 performance with minimal O3 performance degradation. AURAMS was then used to investigate a land-use-dependant lower limit in diffusivity of 1.0 m2 s−1 in urban regions, linearly scaling to 0.01 m2s−1 in rural areas, as employed in CMAQ5.0.1. This strategy was found to significantly improve mean statistics for PM2.5 throughout the day and mean O3 statistics at night, while significantly degrading (halving) midday PM2.5 correlation coefficients and slope of observed to model simulations. Time series of domain-wide model error statistics aggregated by local hour were shown to be a useful tool for performance analysis, with significant variations in performance occurring at different hours of the day. The use of the land-use-dependant lower limit in diffusivity was also shown to reduce the model's sensitivity to the temporal allocation of its emissions inputs. The modelling scenarios suggest that while turbulence plays a key role in O3 and PM2.5 formation in urban regions, and in their downwind transport, the spatial and temporal allocation of primary PM2.5 emissions also has a potentially significant impact on PM2.5 concentration levels. The results show the complex nature of the interactions between turbulence and emissions, and the potential of the strength of the former to mask the impact of changes in the latter.


2009 ◽  
Vol 61 (4) ◽  
pp. 1053-1064 ◽  
Author(s):  
Jin-Ho Kang ◽  
Feng Shi ◽  
A. Daniel Jones ◽  
M. David Marks ◽  
Gregg A. Howe

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