scholarly journals An evaluation of European nitrogen and sulfur wet deposition and their trends estimated by six chemistry transport models for the period 1990–2010

2019 ◽  
Vol 19 (1) ◽  
pp. 379-405 ◽  
Author(s):  
Mark R. Theobald ◽  
Marta G. Vivanco ◽  
Wenche Aas ◽  
Camilla Andersson ◽  
Giancarlo Ciarelli ◽  
...  

Abstract. The wet deposition of nitrogen and sulfur in Europe for the period 1990–2010 was estimated by six atmospheric chemistry transport models (CHIMERE, CMAQ, EMEP MSC-W, LOTOS-EUROS, MATCH and MINNI) within the framework of the EURODELTA-Trends model intercomparison. The simulated wet deposition and its trends for two 11-year periods (1990–2000 and 2000–2010) were evaluated using data from observations from the EMEP European monitoring network. For annual wet deposition of oxidised nitrogen (WNOx), model bias was within 30 % of the average of the observations for most models. There was a tendency for most models to underestimate annual wet deposition of reduced nitrogen (WNHx), although the model bias was within 40 % of the average of the observations. Model bias for WNHx was inversely correlated with model bias for atmospheric concentrations of NH3+NH4+, suggesting that an underestimation of wet deposition partially contributed to an overestimation of atmospheric concentrations. Model bias was also within about 40 % of the average of the observations for the annual wet deposition of sulfur (WSOx) for most models. Decreasing trends in WNOx were observed at most sites for both 11-year periods, with larger trends, on average, for the second period. The models also estimated predominantly decreasing trends at the monitoring sites and all but one of the models estimated larger trends, on average, for the second period. Decreasing trends were also observed at most sites for WNHx, although larger trends, on average, were observed for the first period. This pattern was not reproduced by the models, which estimated smaller decreasing trends, on average, than those observed or even small increasing trends. The largest observed trends were for WSOx, with decreasing trends at more than 80 % of the sites. On average, the observed trends were larger for the first period. All models were able to reproduce this pattern, although some models underestimated the trends (by up to a factor of 4) and others overestimated them (by up to 40 %), on average. These biases in modelled trends were directly related to the tendency of the models to under- or overestimate annual wet deposition and were smaller for the relative trends (expressed as % yr−1 relative to the deposition at the start of the period). The fact that model biases were fairly constant throughout the time series makes it possible to improve the predictions of wet deposition for future scenarios by adjusting the model estimates using a bias correction calculated from past observations. An analysis of the contributions of various factors to the modelled trends suggests that the predominantly decreasing trends in wet deposition are mostly due to reductions in emissions of the precursors NOx, NH3 and SOx. However, changes in meteorology (e.g. precipitation) and other (non-linear) interactions partially offset the decreasing trends due to emission reductions during the first period but not the second. This suggests that the emission reduction measures had a relatively larger effect on wet deposition during the second period, at least for the sites with observations.

2018 ◽  
Author(s):  
Mark R. Theobald ◽  
Marta G. Vivanco ◽  
Wenche Aas ◽  
Camilla Andersson ◽  
Giancarlo Ciarelli ◽  
...  

Abstract. The wet deposition of nitrogen and sulfur in Europe for the period 1990–2010 was estimated by six atmospheric chemistry transport models (CHIMERE, CMAQ, EMEP MSC-W, LOTOS-EUROS, MATCH and MINNI) within the framework of the EURODELTA-Trends model intercomparison. The simulated wet deposition and its trends for two eleven-year periods (1990–2000 and 2000–2010) were evaluated using data from observations from the EMEP European monitoring network. For annual wet deposition of oxidised nitrogen (WNOx), model bias was within 30 % of the average of the observations for most models. There was a tendency for most models to underestimate annual wet deposition of reduced nitrogen (WNHx) although model bias was within 40 % of the average of the observations. Model bias for WNHx was inversely correlated with model bias for atmospheric concentrations of NH3 + NH4+, suggesting that an underestimation of wet deposition partially contributed to an overestimation of atmospheric concentrations. Model bias was also within about 40 % of the average of the observations for the annual wet deposition of sulfur (WSOx) for most models. Decreasing trends in WNOx were observed at most sites for both eleven-year periods, with larger trends, on average, for the second period. The models also estimated predominantly decreasing trends at the monitoring sites and all but one of the models estimated larger trends, on average, for the second period. Decreasing trends were also observed at most sites for WNHx, although larger trends, on average, were observed for the first period. This pattern was not reproduced by the models, which estimated smaller decreasing trends, on average, than those observed or even small increasing trends. The largest observed trends were for WSOx, with decreasing trends at more than 80 % of the sites. On average, the observed trends were larger for the first period. All models were able to reproduce this pattern although some models underestimated the trends (by up to a factor of four) and others overestimated them (by up to 40 %), on average. These biases in modelled trends were directly related to the tendency of the models to under- or overestimate annual wet deposition and were smaller for the relative trends (expressed as % yr−1 relative to the deposition at the start of the period). The fact that model biases were fairly constant throughout the time series makes it possible to improve the predictions of wet deposition for future scenarios by adjusting the model estimates using a bias correction calculated from past observations. An analysis of the contributions of various factors to the modelled trends suggests that the predominantly decreasing trends in wet deposition are mostly due to reductions in emissions of the precursors NOx, NH3 and SOx. However, changes in meteorology (e.g. precipitation) and other (non-linear) interactions partially offset the decreasing trends due to emission reductions during the first period, but not the second. This suggests that the emission reduction measures had a larger effect on wet deposition during the second period, at least for the sites with observations.


2019 ◽  
Author(s):  
Daiwen Kang ◽  
Kristen Foley ◽  
Rohit Mathur ◽  
Shawn Roselle ◽  
Kenneth Pickering ◽  
...  

Abstract. This study assesses the impact of the lightning NOX (LNOX) production schemes in the CMAQ model (Kang et al., 2019) on ground-level air quality as well as aloft atmospheric chemistry through detailed evaluation of model predictions of nitrogen oxides (NOx) and ozone (O3) with corresponding observations for the U.S. For ground-level evaluations, hourly O3 and NOx from the US EPA's AQS monitoring network are used to assess the impact of different LNOx schemes on model prediction of these species in time and space. Vertical evaluations are performed using ozonesonde and P-3B aircraft measurements during the DISCOVER-AQ campaign conducted in the Baltimore/Washington region during July 2011. The impact on wet deposition of nitrate is assessed using measurements from the National Atmospheric Deposition Program's National Trends Network (NADP/NTN). Compared with the base model (without LNOx), the impact of LNOx on surface O3 varies from region to region depending on the base model conditions. Overall statistics suggest that for regions where surface O3 mixing ratios are already overestimated, the incorporation of additional NOx from lightning generally increased model overestimation of mean daily maximum 8-hr (DM8HR) O3 by 1–2 ppb. In regions where surface O3 is underestimated by the base model, LNOx can significantly reduce the underestimation and bring model predictions close to observations. Analysis of vertical profiles reveals that LNOx can significantly improve the vertical structure of modeled O3 distributions by reducing underestimation aloft, and to a lesser degree decreasing overestimation near the surface. Since the base model underestimates the wet deposition of nitrate in most regions across the modeling domain except the Pacific Coast, the inclusion of LNOx leads to reduction in biases and errors and an increase in correlation coefficients at almost all the NADP/NTN sites. Among the three LNOx schemes described in Kang et al. (2019), the hNLDN scheme, which is implemented using hourly observed lightning flash data from National Lightning Detection Network (NLDN), performs best for the ground-level, vertical profiles, and wet deposition comparisons except that for the accumulated wet deposition of nitrate, the mNLDN scheme (the monthly NLDN-based scheme) performed slightly better. However, when observed lightning flash data are not available, the linear regression-based parameterization scheme, pNLDN, provides an improved estimate for LNOx compared to the base simulation that does not include LNOx.


2016 ◽  
Author(s):  
Oleg Travnikov ◽  
Hélène Angot ◽  
Paulo Artaxo ◽  
Mariantonia Bencardino ◽  
Johannes Bieser ◽  
...  

Abstract. Current understanding of mercury (Hg) behaviour in the atmosphere contains significant gaps. Some key characteristics of Hg processes including anthropogenic and geogenic emissions, atmospheric chemistry, and air-surface exchange are still poorly known. This study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measurement data from ground-based sites and simulation results of chemical transport models. A variety of long-term measurements of gaseous elemental Hg (GEM) and reactive Hg (RM) concentration as well as Hg wet deposition flux has been compiled from different global and regional monitoring networks. Four contemporary global-scale transport models for Hg were applied both in their state-of-the-art configurations and for a number of numerical experiments aimed at evaluation of particular processes. Results of the model simulation were evaluated against measurements. As it follows from the analysis the inter-hemispheric gradient of GEM is largely formed by the spatial distribution of anthropogenic emissions which prevail in the Northern Hemisphere. Contribution of natural and secondary emissions enhances the south-to-north gradient but their effect is less significant. The atmospheric chemistry does not affect considerably both spatial distribution and temporal variation of GEM concentration in the surface air. On the other hand, RM air concentration and wet deposition are largely defined by oxidation chemistry. The Br oxidation mechanism allows successfully reproducing observed seasonal variation of the RM / GEM ratio in the near-surface layer, whereas it predicts maximum in wet deposition in spring instead of summer as observed at monitoring sites located in North America and Europe. Model runs with the OH chemistry correctly simulate both the periods of maximum and minimum values and the amplitude of observed seasonal variation but lead to shifting the maximum RM / GEM ratios from spring to summer. The O3 chemistry does not provide significant seasonal variation of Hg oxidation. Thus, performance of the considered Hg oxidation mechanisms differs in reproduction of different observed parameters that can imply possibility of more complex chemistry and multiple pathways of Hg oxidation occurring concurrently in various parts of the atmosphere.


2013 ◽  
Vol 13 (2) ◽  
pp. 4221-4287 ◽  
Author(s):  
A. T. Brown ◽  
C. M. Volk ◽  
M. R. Schoeberl ◽  
C. D. Boone ◽  
P. F. Bernath

Abstract. Long lived halogen-containing compounds are important atmospheric constituents since they can act both as a source of chlorine radicals, which go on to catalyse ozone loss, and as powerful greenhouse gases. The long term impact of these species on the ozone layer is dependent on their stratospheric lifetimes. Using observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) we present calculations of the stratospheric lifetimes of CFC-12, CCl4, CH4, CH3Cl and N2O. The lifetimes were calculated using the slope of the tracer-tracer correlation of these species with CFC-11 at the tropopause. The correlation slopes were corrected for the changing atmospheric concentrations of each species based on age of air and CFC-11 measurements from samples taken aboard the Geophysica aircraft – along with the effective linear trend of the VMR from tropical ground-based AGAGE sites. Stratospheric lifetimes were calculated using a CFC-11 lifetime of 45 yr. These calculations produced values of 113 + (−) 26 (18) yr (CFC-12), 35 + (−) 11 (7) yr (CCl4), 195 + (−) 75 (42) yr (CH4), 69 + (−) 65 (23) yr (CH3Cl) and 123 + (−) 53 (28) yr (N2O). The errors on these values are the weighted 1-σ non-systematic errors. The stratospheric lifetime of CH3Cl represents the first calculations of the stratospheric lifetime of CH3Cl using data from a space based instrument.


2017 ◽  
Vol 17 (8) ◽  
pp. 5271-5295 ◽  
Author(s):  
Oleg Travnikov ◽  
Hélène Angot ◽  
Paulo Artaxo ◽  
Mariantonia Bencardino ◽  
Johannes Bieser ◽  
...  

Abstract. Current understanding of mercury (Hg) behavior in the atmosphere contains significant gaps. Some key characteristics of Hg processes, including anthropogenic and geogenic emissions, atmospheric chemistry, and air–surface exchange, are still poorly known. This study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measured data from ground-based sites and simulation results from chemical transport models. A variety of long-term measurements of gaseous elemental Hg (GEM) and reactive Hg (RM) concentration as well as Hg wet deposition flux have been compiled from different global and regional monitoring networks. Four contemporary global-scale transport models for Hg were used, both in their state-of-the-art configurations and for a number of numerical experiments to evaluate particular processes. Results of the model simulations were evaluated against measurements. As follows from the analysis, the interhemispheric GEM gradient is largely formed by the prevailing spatial distribution of anthropogenic emissions in the Northern Hemisphere. The contributions of natural and secondary emissions enhance the south-to-north gradient, but their effect is less significant. Atmospheric chemistry has a limited effect on the spatial distribution and temporal variation of GEM concentration in surface air. In contrast, RM air concentration and wet deposition are largely defined by oxidation chemistry. The Br oxidation mechanism can reproduce successfully the observed seasonal variation of the RM ∕ GEM ratio in the near-surface layer, but it predicts a wet deposition maximum in spring instead of in summer as observed at monitoring sites in North America and Europe. Model runs with OH chemistry correctly simulate both the periods of maximum and minimum values and the amplitude of observed seasonal variation but shift the maximum RM ∕ GEM ratios from spring to summer. O3 chemistry does not predict significant seasonal variation of Hg oxidation. Hence, the performance of the Hg oxidation mechanisms under study differs in the extent to which they can reproduce the various observed parameters. This variation implies possibility of more complex chemistry and multiple Hg oxidation pathways occurring concurrently in various parts of the atmosphere.


2008 ◽  
Vol 8 (20) ◽  
pp. 6037-6050 ◽  
Author(s):  
M. G. Lawrence ◽  
M. Salzmann

Abstract. Global chemistry-transport models (CTMs) and chemistry-GCMs (CGCMs) generally simulate vertical tracer transport by deep convection separately from the advective transport by the mean winds, even though a component of the mean transport, for instance in the Hadley and Walker cells, occurs in deep convective updrafts. This split treatment of vertical transport has various implications for CTM simulations. In particular, it has led to a misinterpretation of several sensitivity simulations in previous studies in which the parameterized convective transport of one or more tracers is neglected. We describe this issue in terms of simulated fluxes and fractions of these fluxes representing various physical and non-physical processes. We then show that there is a significant overlap between the convective and large-scale mean advective vertical air mass fluxes in the CTM MATCH, and discuss the implications which this has for interpreting previous and future sensitivity simulations, as well as briefly noting other related implications such as numerical diffusion.


2021 ◽  
Author(s):  
Alexey V. Eliseev ◽  
Rustam D. Gizatullin ◽  
Alexandr V. Timazhev

<p>A stationary, computationally efficient  scheme, ChAP-1.0 (Chemistry and Aerosol Processes, version 1.0) for the sulphur cycle in the troposphereis developed. This scheme is envisaged to be implemented into Earth system models of intermediate complexity (EMICs). The scheme accounts for sulphur dioxide emissions into the atmosphere, its deposition to the surface, oxidation to sulphates, and dry and wet deposition of sulphates on the surface.<br>The calculations with the scheme were performed with the anthropogenic emissions of sulphur compounds into the atmosphere for 1850-2000 according to the CMIP5 (Coupled Models Intercomparison Project, phase 5) 'historical' protocol, with the ERA-Interim meteorology, and assuming that natural sources of sulphur into the atmosphere remain unchanged during this period. The model reasonably reproduces characteristics of the tropospheric sulphur cycle known from observations and other simulations (e.g., in the Atmospheric Chemistry and Climate Model Intercomparison Project phase II (ACCMIP) simulations, Copernicus Atmosphere Monitoring Service (CAMS) reanalysis, and the Meteorological Synthesizing Centre–West of the European Monitoring and Evaluation Programme (EMEP MSC-W) data). In particular, in 1980's and 1990's, , when the global anthropogenic emission of sulphur, global atmospheric burdens of SO<sub>2</sub> and SO<sub>4</sub> account, correspondingly, 0.2 TgS and 0.4 TgS. In our scheme, about half of the emitted sulphur dioxide is deposited to the surface and the rest in oxidised into sulphates. The latter mostly removed from the atmosphere by wet deposition. The lifetime of the SO<sub>2</sub> and SO<sub>4</sub> in the atmosphere is, respectively, 1.0±0.1 days and 4.1±0.3 days.<br>Despite its simplicity, our scheme may be successfully used to simulate sulphur/sulphates pollution in the atmosphere at coarse spatial and time scales and an impact of this pollution to direct radiative effect of sulphates on climate, their respective indirect (cloud- and precipitation-related) effects, as well as an impact of sulphur compounds on the terrestrial carbon cycle.</p>


2021 ◽  
Vol 14 (11) ◽  
pp. 7021-7046
Author(s):  
Yao Ge ◽  
Mathew R. Heal ◽  
David S. Stevenson ◽  
Peter Wind ◽  
Massimo Vieno

Abstract. Atmospheric pollution has many profound effects on human health, ecosystems, and the climate. Of concern are high concentrations and deposition of reactive nitrogen (Nr) species, especially of reduced N (gaseous NH3, particulate NH4+). Atmospheric chemistry and transport models (ACTMs) are crucial to understanding sources and impacts of Nr chemistry and its potential mitigation. Here we undertake the first evaluation of the global version of the EMEP MSC-W ACTM driven by WRF meteorology (1∘×1∘ resolution), with a focus on surface concentrations and wet deposition of N and S species relevant to investigation of atmospheric Nr and secondary inorganic aerosol (SIA). The model–measurement comparison is conducted both spatially and temporally, covering 10 monitoring networks worldwide. Model simulations for 2010 compared use of both HTAP and ECLIPSEE (ECLIPSE annual total with EDGAR monthly profile) emissions inventories; those for 2015 used ECLIPSEE only. Simulations of primary pollutants are somewhat sensitive to the choice of inventory in places where regional differences in primary emissions between the two inventories are apparent (e.g. China) but are much less sensitive for secondary components. For example, the difference in modelled global annual mean surface NH3 concentration using the two 2010 inventories is 18 % (HTAP: 0.26 µg m−3; ECLIPSEE: 0.31 µg m−3) but is only 3.5 % for NH4+ (HTAP: 0.316 µg m−3; ECLIPSEE: 0.305 µg m−3). Comparisons of 2010 and 2015 surface concentrations between the model and measurements demonstrate that the model captures the overall spatial and seasonal variations well for the major inorganic pollutants NH3, NO2, SO2, HNO3, NH4+, NO3-, and SO42- and their wet deposition in East Asia, Southeast Asia, Europe, and North America. The model shows better correlations with annual average measurements for networks in Southeast Asia (mean R for seven species: R7‾=0.73), Europe (R7‾=0.67), and North America (R7‾=0.63) than in East Asia (R5‾=0.35) (data for 2015), which suggests potential issues with the measurements in the latter network. Temporally, both model and measurements agree on higher NH3 concentrations in spring and summer and lower concentrations in winter. The model slightly underestimates annual total precipitation measurements (by 13 %–45 %) but agrees well with the spatial variations in precipitation in all four world regions (0.65–0.94 R range). High correlations between measured and modelled NH4+ precipitation concentrations are also observed in all regions except East Asia. For annual total wet deposition of reduced N, the greatest consistency is in North America (0.75–0.82 R range), followed by Southeast Asia (R=0.68) and Europe (R=0.61). Model–measurement bias varies between species in different networks; for example, bias for NH4+ and NO3- is largest in Europe and North America and smallest in East Asia and Southeast Asia. The greater uniformity in spatial correlations than in biases suggests that the major driver of model–measurement discrepancies (aside from differing spatial representativeness and uncertainties and biases in measurements) are shortcomings in absolute emissions rather than in modelling the atmospheric processes. The comprehensive evaluations presented in this study support the application of this model framework for global analysis of current and potential future budgets and deposition of Nr and SIA.


2016 ◽  
Author(s):  
Andreas Ostler ◽  
Ralf Sussmann ◽  
Prabir K. Patra ◽  
Sander Houweling ◽  
Marko De Bruine ◽  
...  

Abstract. The distribution of methane (CH4) in the stratosphere can be a major driver of spatial variability in the dry-air column-averaged CH4 mixing ratio (XCH4), which is being measured increasingly for the assessment of CH4 surface emissions. Chemistry-transport models (CTMs) therefore need to simulate the tropospheric and stratospheric fractional columns of XCH4 accurately for estimating surface emissions from XCH4. Simulations from three CTMs are tested against XCH4 observations from the Total Carbon Column Network (TCCON). We analyze how the model-TCCON agreement in XCH4 depends on the model representation of stratospheric CH4 distributions. Model equivalents of TCCON XCH4 are computed with stratospheric CH4 fields from both the model simulations and from satellite-based CH4 distributions from MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) and MIPAS CH4 fields adjusted to ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer) observations. In comparison to simulated model fields we find an improved model-TCCON XCH4 agreement for all models with MIPAS-based stratospheric CH4 fields. For the Atmospheric Chemistry Transport Model (ACTM) the average XCH4 bias is significantly reduced from 38.1 ppb to 13.7 ppb, whereas small improvements are found for the models TM5 (Transport Model, version 5; from 8.7 ppb to 4.3 ppb), and LMDz (Laboratoire de Météorologie Dynamique model with Zooming capability; from 6.8 ppb to 4.3 ppb), respectively. MIPAS stratospheric CH4 fields adjusted to ACE-FTS reduce the average XCH4 bias for ACTM (3.3 ppb), but increase the average XCH4 bias for TM5 (10.8 ppb) and LMDz (20.0 ppb). These findings imply that the range of satellite-based stratospheric CH4 is insufficient to resolve a possible stratospheric contribution to differences in total column CH4 between TCCON and TM5 or LMDz. Applying transport diagnostics to the models indicates that model-to-model differences in the simulation of stratospheric transport, notably the age of stratospheric air, can largely explain the inter-model spread in stratospheric CH4 and, hence, its contribution to XCH4. This implies that there is a need to better understand the impact of individual model transport components (e.g., physical parameterization, meteorological data sets, model horizontal/vertical resolution) on modeled stratospheric CH4.


2007 ◽  
Vol 7 (4) ◽  
pp. 10323-10342 ◽  
Author(s):  
S. L. Gong ◽  
X. Y. Zhang

Abstract. An integrated sand and dust storm (SDS) forecasting system – CUACE/Dust (the Chinese Unified Atmospheric Chemistry Environment for Dust) has been developed, which consists of a comprehensive dust aerosol module with emission, dry/wet depositions and other atmospheric dynamic processes, and a data assimilation system (DAS) using observational data from the CMA (China Meteorological Administration) ground dust monitoring network and retrieved dust information from a Chinese geostationary satellite – FY-2C. This is the first time that a combination of surface network observations and satellite retrievals of the dust aerosol has been successfully used in the real time operational forecasts in East Asia through a DAS. During its application for the operational SDS forecasts in East Asia for spring 2006, this system captured the major 31 SDS episodes observed by both surface and satellite observations. Analysis shows that the seasonal mean threat score (TS) for 0–24 h forecast over the East Asia in spring 2006 increased from 0.22 to 0.31 by using the DAS, a 41% enhancement. The time series of the forecasted dust concentrations for a number of representative stations for the whole spring 2006 were also evaluated against the surface PM10 monitoring data, showing a very good agreement in terms of the SDS timing and magnitudes near source regions where dust aerosols dominate. This is a summary paper for a special issue of ACP featuring the development and results of the forecasting system.


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