scholarly journals Technical note: How are NH<sub>3</sub> dry deposition estimates affected by combining the LOTOS-EUROS model with IASI-NH<sub>3</sub> satellite observations?

2018 ◽  
Vol 18 (17) ◽  
pp. 13173-13196 ◽  
Author(s):  
Shelley C. van der Graaf ◽  
Enrico Dammers ◽  
Martijn Schaap ◽  
Jan Willem Erisman

Abstract. Atmospheric levels of reactive nitrogen have increased substantially during the last century resulting in increased nitrogen deposition to ecosystems, causing harmful effects such as soil acidification, reduction in plant biodiversity and eutrophication in lakes and the ocean. Recent developments in the use of atmospheric remote sensing enabled us to resolve concentration fields of NH3 with larger spatial coverage. These observations may be used to improve the quantification of NH3 deposition. In this paper, we use a relatively simple, data-driven method to derive dry deposition fluxes and surface concentrations of NH3 for Europe and for the Netherlands. The aim of this paper is to determine the applicability and the limitations of this method for NH3. Space-born observations of the Infrared Atmospheric Sounding Interferometer (IASI) and the LOTOS-EUROS atmospheric transport model are used. The original modelled dry NH3 deposition flux from LOTOS-EUROS and the flux inferred from IASI are compared to indicate areas with large discrepancies between the two. In these areas, potential model or emission improvements are needed. The largest differences in derived dry deposition fluxes occur in large parts of central Europe, where the satellite-observed NH3 concentrations are higher than the modelled ones, and in Switzerland, northern Italy (Po Valley) and southern Turkey, where the modelled NH3 concentrations are higher than the satellite-observed ones. A sensitivity analysis of eight model input parameters important for NH3 dry deposition modelling showed that the IASI-derived dry NH3 deposition fluxes may vary from ∼ 20 % up to ∼50 % throughout Europe. Variations in the NH3 dry deposition velocity led to the largest deviations in the IASI-derived dry NH3 deposition flux and should be focused on in the future. A comparison of NH3 surface concentrations with in situ measurements of several established networks – the European Monitoring and Evaluation Programme (EMEP), Meetnet Ammoniak in Natuurgebieden (MAN) and Landelijk Meetnet Luchtkwaliteit (LML) – showed no significant or consistent improvement in the IASI-derived NH3 surface concentrations compared to the originally modelled NH3 surface concentrations from LOTOS-EUROS. It is concluded that the IASI-derived NH3 deposition fluxes do not show strong improvements compared to modelled NH3 deposition fluxes and there is a future need for better, more robust, methods to derive NH3 dry deposition fluxes.

2018 ◽  
Author(s):  
Shelley C. van der Graaf ◽  
Enrico Dammers ◽  
Martijn Schaap ◽  
Jan Willem Erisman

Abstract. Atmospheric levels of reactive nitrogen have substantially increased during the last century resulting in increased nitrogen deposition to ecosystems, causing harmful effects such as soil acidification, reduction in plant biodiversity and eutrophication in lakes and the ocean. Recent developments in the use of atmospheric remote sensing enabled us to resolve concentration fields of NH3 with larger spatial coverage and these observations may be used to improve the quantification of NH3 deposition. In this paper we use a relatively simple, data-driven method to derive dry deposition fluxes and surface concentrations of NH3 for Europe and for the Netherlands. The aim of this paper is to determine for the applicability and the limitations of this method for NH3 using space-born observations of the Infrared Atmospheric Sounding Interferometer (IASI) and the LOTOS-EUROS atmospheric transport model. The original modelled dry NH3 deposition flux from LOTOS-EUROS and the flux inferred from IASI are compared to indicate areas with large discrepancies between the two and where potential model improvements are needed. The largest differences in derived dry deposition fluxes occur in large parts of Central Europe, where the satellite-observed NH3 concentrations are higher than the modelled ones, and in Switzerland, northern Italy (Po Valley) and southern Turkey, where the modelled NH3 concentrations are higher than the satellite-observed ones. A sensitivity analysis of 8 model input parameters important for NH3 dry deposition modelling showed that the IASI-derived dry NH3 deposition fluxes may vary from ~ 20 % up to ~ 50 % throughout Europe. Variations in the dry deposition velocity used for NH3 led to the largest deviations in the IASI-derived dry NH3 deposition flux and should be focused on in the future. A comparison of NH3 surface concentrations with in-situ measurements of several established networks (EMEP, MAN and LML) showed no significant, or consistent improvement in the IASI-derived NH3 surface concentrations compared to the originally modelled NH3 surface concentrations from LOTOS-EUROS. It is concluded that the IASI-derived NH3 deposition fluxes do not show strong improvements compared to modelled NH3 deposition fluxes and there is future need for better, more robust, methods to derive NH3 dry deposition fluxes.


2011 ◽  
Vol 11 (4) ◽  
pp. 1549-1564 ◽  
Author(s):  
A. K. Halse ◽  
M. Schlabach ◽  
S. Eckhardt ◽  
A. Sweetman ◽  
K. C. Jones ◽  
...  

Abstract. Passive air samplers (PAS) were deployed at 86 European background sites during summer 2006 in order (i) to gain further insight into spatial patterns of persistent organic pollutants (POPs) in European background air and, (ii) to evaluate PAS as an alternative sampling technique under EMEP (Co-operative programme for monitoring and evaluation of the long-range transmissions of air pollutants in Europe). The samples were analyzed for selected PCBs, HCHs, DDTs, HCB, PAHs and chlordanes, and air concentrations were calculated on the basis of losses of performance reference compounds. Air concentrations of PCBs were generally lowest in more remote areas of northern Europe with elevated levels in more densely populated areas. γ-HCH was found at elevated levels in more central parts of Europe, whereas α-HCH, β-HCH and DDTs showed higher concentrations in the south-eastern part. There was no clear spatial pattern in the concentrations for PAHs, indicative of influence by local sources, rather than long range atmospheric transport (LRAT). HCB was evenly distributed across Europe, while the concentrations of chlordanes were typically low or non-detectable. A comparison of results obtained on the basis of PAS and active air sampling (AAS) illustrated that coordinated PAS campaigns have the potential serve as useful inter-comparison exercises within and across existing monitoring networks. The results also highlighted limitations of the current EMEP measurement network with respect to spatial coverage. We finally adopted an existing Lagrangian transport model (FLEXPART) as recently modified to incorporate key processes relevant for POPs to evaluate potential source regions affecting observed concentrations at selected sites. Using PCB-28 as an example, the model predicted concentrations which agreed within a factor of 3 with PAS measurements for all except 1 out of the 17 sites selected for this analysis.


2020 ◽  
Vol 13 (3) ◽  
pp. 1137-1153 ◽  
Author(s):  
Yadong Lei ◽  
Xu Yue ◽  
Hong Liao ◽  
Cheng Gong ◽  
Lin Zhang

Abstract. The terrestrial biosphere and atmospheric chemistry interact through multiple feedbacks, but the models of vegetation and chemistry are developed separately. In this study, the Yale Interactive terrestrial Biosphere (YIBs) model, a dynamic vegetation model with biogeochemical processes, is implemented into the Chemical Transport Model GEOS-Chem (GC) version 12.0.0. Within this GC-YIBs framework, leaf area index (LAI) and canopy stomatal conductance dynamically predicted by YIBs are used for dry deposition calculation in GEOS-Chem. In turn, the simulated surface ozone (O3) by GEOS-Chem affect plant photosynthesis and biophysics in YIBs. The updated stomatal conductance and LAI improve the simulated O3 dry deposition velocity and its temporal variability for major tree species. For daytime dry deposition velocities, the model-to-observation correlation increases from 0.69 to 0.76, while the normalized mean error (NME) decreases from 30.5 % to 26.9 % using the GC-YIBs model. For the diurnal cycle, the NMEs decrease by 9.1 % for Amazon forests, 6.8 % for coniferous forests, and 7.9 % for deciduous forests using the GC-YIBs model. Furthermore, we quantify the damaging effects of O3 on vegetation and find a global reduction of annual gross primary productivity by 1.5 %–3.6 %, with regional extremes of 10.9 %–14.1 % in the eastern USA and eastern China. The online GC-YIBs model provides a useful tool for discerning the complex feedbacks between atmospheric chemistry and the terrestrial biosphere under global change.


2017 ◽  
Vol 17 (14) ◽  
pp. 8999-9017 ◽  
Author(s):  
Viral Shah ◽  
Lyatt Jaeglé

Abstract. Oxidized mercury (Hg(II)) is chemically produced in the atmosphere by oxidation of elemental mercury and is directly emitted by anthropogenic activities. We use the GEOS-Chem global chemical transport model with gaseous oxidation driven by Br atoms to quantify how surface deposition of Hg(II) is influenced by Hg(II) production at different atmospheric heights. We tag Hg(II) chemically produced in the lower (surface–750 hPa), middle (750–400 hPa), and upper troposphere (400 hPa–tropopause), in the stratosphere, as well as directly emitted Hg(II). We evaluate our 2-year simulation (2013–2014) against observations of Hg(II) wet deposition as well as surface and free-tropospheric observations of Hg(II), finding reasonable agreement. We find that Hg(II) produced in the upper and middle troposphere constitutes 91 % of the tropospheric mass of Hg(II) and 91 % of the annual Hg(II) wet deposition flux. This large global influence from the upper and middle troposphere is the result of strong chemical production coupled with a long lifetime of Hg(II) in these regions. Annually, 77–84 % of surface-level Hg(II) over the western US, South America, South Africa, and Australia is produced in the upper and middle troposphere, whereas 26–66 % of surface Hg(II) over the eastern US, Europe, and East Asia, and South Asia is directly emitted. The influence of directly emitted Hg(II) near emission sources is likely higher but cannot be quantified by our coarse-resolution global model (2° latitude  ×  2.5° longitude). Over the oceans, 72 % of surface Hg(II) is produced in the lower troposphere because of higher Br concentrations in the marine boundary layer. The global contribution of the upper and middle troposphere to the Hg(II) dry deposition flux is 52 %. It is lower compared to the contribution to wet deposition because dry deposition of Hg(II) produced aloft requires its entrainment into the boundary layer, while rain can scavenge Hg(II) from higher altitudes more readily. We find that 55 % of the spatial variation of Hg wet deposition flux observed at the Mercury Deposition Network sites is explained by the combined variation of precipitation and Hg(II) produced in the upper and middle troposphere. Our simulation points to a large role of the dry subtropical subsidence regions. Hg(II) present in these regions accounts for 74 % of Hg(II) at 500 hPa over the continental US and more than 60 % of the surface Hg(II) over high-altitude areas of the western US. Globally, it accounts for 78 % of the tropospheric Hg(II) mass and 61 % of the total Hg(II) deposition. During the Nitrogen, Oxidants, Mercury, and Aerosol Distributions, Sources, and Sinks (NOMADSS) aircraft campaign, the contribution of Hg(II) from the dry subtropical regions was found to be 75 % when measured Hg(II) exceeded 250 pg m−3. Hg(II) produced in the upper and middle troposphere subsides in the anticyclones, where the dry conditions inhibit the loss of Hg(II). Our results highlight the importance the subtropical anticyclones as the primary conduits for the production and export of Hg(II) to the global atmosphere.


2021 ◽  
Author(s):  
Katherine Hayden ◽  
Shao-Meng Li ◽  
Paul Makar ◽  
John Liggio ◽  
Samar G. Moussa ◽  
...  

Abstract. The atmospheric lifetimes of pollutants determine their impacts on human health, ecosystems and climate and yet pollutant lifetimes due to dry deposition over large regions have not been determined from measurements. Here, a new methodology based on aircraft observations is used to determine the lifetimes of oxidized sulfur and nitrogen due to dry deposition over (3–6) × 103 km2 of boreal forest in Canada. Dry deposition fluxes decreased exponentially with distance, resulting in lifetimes of 2.2–26 hours. Fluxes were 2–14 and 1–18 times higher than model estimates for oxidized sulfur and nitrogen, respectively, indicating dry deposition velocities which were 1.2–5.4 times higher than those computed for models. A Monte-Carlo analysis with five commonly used inferential dry deposition algorithms indicates that such model underestimates of dry deposition velocity are typical. These findings indicate that deposition to vegetation surfaces are likely under-estimated in regional and global chemical transport models regardless of the model algorithm used. The model-observation gaps may be reduced if surface pH, and quasi-laminar and aerodynamic resistances in algorithms are optimized as shown in the Monte-Carlo analysis. Assessing the air quality and climate impacts of atmospheric pollutants on regional and global scales requires improved measurement-based understanding of atmospheric lifetimes of these pollutants.


2013 ◽  
Vol 13 (5) ◽  
pp. 11689-11744 ◽  
Author(s):  
M. Adon ◽  
C. Galy-Lacaux ◽  
V. Yoboue ◽  
C. Delon ◽  
F. Solmon ◽  
...  

Abstract. This work is part of the IDAF program (IGAC-DEBITS-AFRICA) and is based on the long term monitoring of gas concentrations (1998–2007) established on seven remote sites representative of major African ecosystems. Dry deposition fluxes were estimated by the inferential method using on one hand surface measurements of gas concentrations (NO2, HNO3, NH3, SO2, and O3) and on the other hand simulated dry deposition velocities (Vd). Vd were calculated using the big-leaf model of Zhang et al. (2003b). In the model of deposition, surface and meteorological conditions specific to IDAF sites have been adapted in order to simulate Vd representative of major African ecosystems. The monthly, seasonal and annual mean variations of gaseous dry deposition fluxes (NO2, HNO3, NH3, O3, and SO2) are analyzed. Along the latitudinal transect of ecosystems, the annual mean dry deposition fluxes of nitrogen compounds range from 0.4 ± 0.0 to 0.8 ± 0.2 kg N ha−1 yr−1 for NO2, from 0.7 ± 0.1 to 1.0 ± 0.3 kg N ha−1 yr−1 for HNO3, and from 2.3 ± 0.8 to 10.5 ± 5.0 kg N ha−1 yr−1 for NH3 over the study period (1998–2007). The total nitrogen dry deposition flux (NO2+HNO3+NH3) is more important in forests (11.2–11.8 kg N ha−1 yr−1) than in wet and dry savannas (3.4–5.3 kg N ha−1 yr−1). NH3 dominated nitrogen dry deposition, representing 67–80% of the total. The annual mean dry deposition fluxes of ozone range between 11.3 ± 4.7 and 17.5 ± 3.0 kg ha−1 yr−1 in dry savannas, 17.5 ± 3.0 and 19.2 ± 2.9 kg ha−1 yr−1 in wet savannas, and 10.6 ± 2.0 and 13.2 ± 3.6 kg ha−1 yr−1 in forests. Lowest O3 dry deposition fluxes in forests are correlated to low measured O3 concentrations, lower of a factor of 2–3, compared to others ecosystems. Along the ecosystem transect, annual mean of SO2 dry deposition fluxes present low values and a small variability (0.5 to 1 kg S ha−1 yr−1). No specific trend in the interannual variability of these gaseous dry deposition fluxes is observed over the study period.


2020 ◽  
Author(s):  
Athanasios Nenes ◽  
Maria Kanakidou ◽  
Spyros Pandis ◽  
Armistead Russell ◽  
Shaojie Song ◽  
...  

&lt;p&gt;Nitrogen oxides (NOx) and ammonia (NH&lt;sub&gt;3&lt;/sub&gt;) from anthropogenic and biogenic emissions are central contributors to particulate matter (PM) concentrations worldwide. Ecosystem productivity can also be strongly modulated by the atmospheric deposition of this inorganic &quot;reactive nitrogen&quot; nutrient. The response of PM and nitrogen deposition to changes in the emissions of both compounds is typically studied on a case-by-case basis, owing in part to the complex thermodynamic interactions of these aerosol precursors with other PM constituents. In the absence of rain, much of the complexity of nitrogen deposition is driven by the large difference in dry deposition velocity when a nitrogen-containing molecule is in the gas or condensed phase.&lt;/p&gt;&lt;p&gt;Here we present a simple but thermodynamically consistent approach that expresses the chemical domains of sensitivity of aerosol particulate matter to NH&lt;sub&gt;3&lt;/sub&gt; and HNO&lt;sub&gt;3&lt;/sub&gt; availability in terms of aerosol pH and liquid water content. From our analysis, four policy-relevant regimes emerge in terms of sensitivity: i) NH&lt;sub&gt;3&lt;/sub&gt;-sensitive, ii) HNO&lt;sub&gt;3&lt;/sub&gt;-sensitive, iii) combined NH&lt;sub&gt;3&lt;/sub&gt; and HNO&lt;sub&gt;3&lt;/sub&gt; sensitive, and, iv) a domain where neither NH&lt;sub&gt;3&lt;/sub&gt; and HNO&lt;sub&gt;3&lt;/sub&gt; are important for PM levels (but only nonvolatile precursors such as NVCs and sulfate). When this framework is applied to ambient measurements or predictions of PM and gaseous precursors, the &amp;#8220;chemical regime&amp;#8221; of PM sensitivity to NH3 and HNO3 availability is directly determined.&amp;#160;&lt;/p&gt;&lt;p&gt;The same framework is then extended to consider the impact of gas-to-particle partitioning, on the deposition velocity of NH&lt;sub&gt;3&lt;/sub&gt; and HNO&lt;sub&gt;3&lt;/sub&gt; individually, and combined affects the dry deposition of inorganic reactive nitrogen. Four regimes of deposition velocity emerge: i) HNO&lt;sub&gt;3&lt;/sub&gt;-fast, NH&lt;sub&gt;3&lt;/sub&gt;-slow, ii) HNO&lt;sub&gt;3&lt;/sub&gt;-slow, NH&lt;sub&gt;3&lt;/sub&gt;-fast, iii) HNO&lt;sub&gt;3&lt;/sub&gt;-fast, NH&lt;sub&gt;3&lt;/sub&gt;-fast, and, iv) HNO&lt;sub&gt;3&lt;/sub&gt;-slow, NH&lt;sub&gt;3&lt;/sub&gt;-slow. Conditions that favor strong partitioning of species to the aerosol phase strongly delay the deposition of reactive nitrogen species and promotes their accumulation in the boundary layer and potential for long-range transport.&amp;#160;&lt;/p&gt;&lt;p&gt;The use of these regimes allows novel insights and is an important tool to evaluate chemical transport models. Most notably, we find that nitric acid displays considerable variability of dry deposition flux, with maximum deposition rates found in the Eastern US (close to gas-deposition rates) and minimum rates for North Europe and China. Strong reductions in deposition velocity lead to considerable accumulation of nitrate aerosol in the boundary layer &amp;#8211;up to 10-fold increases in PM2.5 nitrate aerosol, eventually being an important contributor to high PM2.5 levels observed during haze episodes. With this new understanding, aerosol pH and associated liquid water content can be understood as control parameters that drive PM formation and dry deposition flux and arguably can catalyze the accumulation of aerosol precursors that cause intense haze events throughout the globe.&lt;/p&gt;


2009 ◽  
Vol 9 (17) ◽  
pp. 6597-6610 ◽  
Author(s):  
S. Eckhardt ◽  
K. Breivik ◽  
Y. F. Li ◽  
S. Manø ◽  
A. Stohl

Abstract. A key feature of POPs (Persistent Organic Pollutants) is their potential for long-range atmospheric transport. In order to better understand and predict atmospheric source-receptor relationships of POPs, we have modified an existing Lagrangian transport model (FLEXPART) to include some of the key processes that control the atmospheric fate of POPs. We also present four years (2004–2007) of new atmospheric measurement data for polychlorinated biphenyls (PCBs) and hexachlorocyclohexanes (HCHs) obtained at Birkenes, an EMEP (European Monitoring and Evaluation Programme) site in southern Norway. The model overestimates measured PCB-28 and γ-HCH concentrations by factors of 2 and 8, respectively, which is most likely because the emissions used as input to the model are overestimated. FLEXPART captures the temporal variability in the measurements very well and, depending on season, explains 31–67% (14–62%) of the variance of measured PCB-28 (γ-HCH) concentrations. FLEXPART, run in a time-reversed (adjoint) mode, was used to identify the source regions responsible for the POP loading at the Birkenes station. Emissions in Central Europe and Eastern Europe contributed 32% and 24%, respectively, to PCB-28 at Birkenes, while Western Europe was found to be the dominant source (50%) for γ-HCH. Intercontinental transport from North America contributed 13% γ-HCH. While FLEXPART has no treatment of the partitioning of POPs between different surface media, it was found a very useful tool for studying atmospheric source-receptor relationships for POPs and POP-like chemicals that do not sorb strongly to atmospheric particles and whose atmospheric levels are believed to be mainly controlled by primary sources.


2008 ◽  
Vol 8 (2) ◽  
pp. 7755-7779
Author(s):  
A. M. Michalak

Abstract. Inverse modeling methods are now commonly used for estimating surface fluxes of carbon dioxide, using atmospheric mass fraction measurements combined with a numerical atmospheric transport model. The geostatistical approach to flux estimation takes advantage of the spatial and/or temporal correlation in fluxes and does not require prior flux estimates. In this work, a geostatistical implementation of a fixed-lag Kalman smoother is developed to improve the computational efficiency of the inverse problem. This method makes it feasible to perform multi-year inversions, at fine resolutions, and with large amounts of data. The new method is applied to the recovery of global gridscale carbon dioxide fluxes for 1997 to 2001 using pseudodata representative of a subset of the NOAA-ESRL Cooperative Air Sampling Network.


2019 ◽  

<p>This paper analysis the contents and variation of heavy metals in wet and dry deposition in Changji (Xinjiang, China) revealed their reducing regularity for heavy metals in atmosphere in arid area. Samples (including 84 dry deposition samples and 16 wet deposition samples) were collected from January 2016 to December 2016, and the contents of heavy metals (Ni, Cu, Cd and Pb) were analyzed by AA-7000 atomic absorption spectrophotometer. The dry deposition fluxes of Ni, Cu, Cd and Pb are 3.70 mg/( m2.a), 4.81 mg/( m2. a), 0.53 mg/( m2•a) and 22.74 mg/( m2•a), respectively; the wet deposition fluxes of Ni, Cu, Cd and Pb are 0.77mg/( m2•a), 3.25mg/( m2•a), 0.04mg/( m2•a) and 0.11mg/( m2•a), respectively. Each of the four heavy metals deposition fluxes during heating period was higher than non-heating period, especially for Pb and Cd, which is mainly due to the emission of coal combustion for heating. During sampling periods, the ratio of wet deposition flux to total for Ni, Cu, Cd and Pb are 17.21%, 40.33%, 7.67% and 0.48%, respectively; the wet deposition flux is far less than dry deposition, especially for Pb. The rate of dry deposition is lower than wet deposition, however dry deposition plays an important role in scavenging heavy metals in arid region. Arid region has a low intensity and frequency of rain event, heavy metals were mainly scavenging by dry deposition attribute to its continuous and dependable process. Dry deposition has much more environmental effect on heavy metal in arid region.</p>


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