Dry Deposition Estimates Research Articles

Dry deposition of nitric acid gas by long-term measurement above and below a forest canopy

Reactive nitrogen negatively affects terrestrial ecosystems by excessive deposition. Nitric acid gas (HNO3), a component of reactive nitrogen, is readily deposited on ground surfaces due to its high reactivity. However, there have been recent cases in which suppressed deposition fluxes, including upward fluxes, were observed above forests. As the mechanisms of HNO3 dry deposition on forest surfaces are not fully understood, the accuracy of dry deposition estimates remains uncertain. To reduce uncertainties in the estimation, we investigated dry deposition of HNO3 by 1-year measurement in a forest. We measured the vertical profiles of HNO3, nitrate, and sulfate in PM2.5 in a deciduous forest in suburban Tokyo (FM Tama). We observed their concentrations above the forest canopy (30 m) and near the forest floor (2 and 0.2 m) using the denuder/filter pack from October 2020 to September 2021. The HNO3 concentration decreased significantly from 30 to 2 m. However, the decrease in HNO3 was not as significant, and occasionally, emission profiles were produced between 2 and 0.2 m. This was likely caused by HNO3 generated by the volatilization of NH4NO3 near the forest floor, which was warmed by sunlight during daytime in both leafy and leafless periods. Conversely, HNO3 concentrations at 30 m were much higher than those at 2 m and 0.2 m, indicating that the forest acted as a sink for HNO3 from a long-term perspective. It is presumed that HNO3, generated just above the forest canopy, could cause an upward flux if a temperature difference of several degrees occurs between 25 and 20 m.

A single-point modeling approach for the intercomparison and evaluation of ozone dry deposition across chemical transport models (Activity 2 of AQMEII4).

A primary sink of air pollutants and their precursors is dry deposition. Dry deposition estimates differ across chemical transport models, yet an understanding of the model spread is incomplete. Here, we introduce Activity 2 of the Air Quality Model Evaluation International Initiative Phase 4 (AQMEII4). We examine 18 dry deposition schemes from regional and global chemical transport models as well as standalone models used for impact assessments or process understanding. We configure the schemes as single-point models at eight Northern Hemisphere locations with observed ozone fluxes. Single-point models are driven by a common set of site-specific meteorological and environmental conditions. Five of eight sites have at least 3 years and up to 12 years of ozone fluxes. The interquartile range across models in multiyear mean ozone deposition velocities ranges from a factor of 1.2 to 1.9 annually across sites and tends to be highest during winter compared with summer. No model is within 50 % of observed multiyear averages across all sites and seasons, but some models perform well for some sites and seasons. For the first time, we demonstrate how contributions from depositional pathways vary across models. Models can disagree with respect to relative contributions from the pathways, even when they predict similar deposition velocities, or agree with respect to the relative contributions but predict different deposition velocities. Both stomatal and nonstomatal uptake contribute to the large model spread across sites. Our findings are the beginning of results from AQMEII4 Activity 2, which brings scientists who model air quality and dry deposition together with scientists who measure ozone fluxes to evaluate and improve dry deposition schemes in the chemical transport models used for research, planning, and regulatory purposes.

Atmospheric dry and wet deposition of total phosphorus to the Great Lakes

Quantifying atmospheric loadings of total phosphorus (TP) to freshwater environments is essential to improve understanding of its fate and transport, and to mitigate the effects of excessive levels in freshwater ecosystems. To date, atmospheric deposition of TP in the U.S. is poorly characterized due to the lack of long-term deposition observations. Here, we integrate several historical datasets to develop an estimate of dry and wet deposition to the Great Lakes region. For dry deposition, we use TP concentrations in fine particulate matter (PM2.5) samples from fourteen land-based IMPROVE sites (2013–2020) upwind of the Great Lakes to provide new fine particle phosphorus dry deposition estimates. For wet deposition, we use TP concentrations in wet-only precipitation samples collected at eleven land-based sites (2001–2009) in the Great Lakes region. For both wet and dry deposition, a seasonal cycle is evident with higher concentrations in warmer and wetter months when compared to colder months. Additionally, there is an increasing gradient from north to south in wet deposition, likely driven by both higher precipitation and increased emissions near southern sites. Despite different sampling time periods, these updated observations can provide further constraints on the TP loadings to each of the five Great Lakes. We estimate annual deposition of TP to Lakes Superior, Michigan, Huron, Erie and Ontario at 526, 702, 495, 212, and 185 MTA per year, which is lower than prior estimates for Lakes Superior, Erie and Ontario, comparable for Lake Huron, and about two times greater for Lake Michigan. When considering only the contribution of fine particulate PM to the dry deposition, wet deposition dominated over dry at all lakes except for Lake Huron. However, prior global estimates suggest greater contributions from larger particles (PM10 and PM100), yet observations to validate these estimates over the Great Lakes are not available. Our findings indicate that dry deposition of a range of particle sizes are needed to constrain the total atmospheric deposition of TP over the Great Lakes.

Forest–atmosphere exchange of reactive nitrogen in a remote region – Part II: Modeling annual budgets

Abstract. To monitor the effect of current nitrogen emissions and mitigation strategies, total (wet + dry) atmospheric nitrogen deposition to forests is commonly estimated using chemical transport models or canopy budget models in combination with throughfall measurements. Since flux measurements of reactive nitrogen (Nr) compounds are scarce, dry deposition process descriptions as well as the calculated flux estimates and annual budgets are subject to considerable uncertainties. In this study, we compared four different approaches to quantify annual dry deposition budgets of total reactive nitrogen (ΣNr) at a mixed forest site situated in the Bavarian Forest National Park, Germany. Dry deposition budgets were quantified based on (I) 2.5 years of eddy covariance flux measurements with the Total Reactive Atmospheric Nitrogen Converter (TRANC); (II) an in situ application of the bidirectional inferential flux model DEPAC (Deposition of Acidifying Compounds), here called DEPAC-1D; (III) a simulation with the chemical transport model LOTOS-EUROS (Long-Term Ozone Simulation – European Operational Smog) v2.0, using DEPAC as dry deposition module; and (IV) a canopy budget technique (CBT). Averaged annual ΣNr dry deposition estimates determined from TRANC measurements were 4.7 ± 0.2 and 4.3 ± 0.4 kg N ha−1 a−1, depending on the gap-filling approach. DEPAC-1D-modeled dry deposition, using concentrations and meteorological drivers measured at the site, was 5.8 ± 0.1 kg N ha−1 a−1. In comparison to TRANC fluxes, DEPAC-1D estimates were systematically higher during summer and in close agreement in winter. Modeled ΣNr deposition velocities (vd) of DEPAC-1D were found to increase with lower temperatures and higher relative humidity and in the presence of wet leaf surfaces, particularly from May to September. This observation was contrary to TRANC-observed fluxes. LOTOS-EUROS-modeled annual dry deposition was 6.5 ± 0.3 kg N ha−1 a−1 for the site-specific weighting of land-use classes within the site's grid cell. LOTOS-EUROS showed substantial discrepancies to measured ΣNr deposition during spring and autumn, which was related to an overestimation of ammonia (NH3) concentrations by a factor of 2 to 3 compared to measured values as a consequence of a mismatch between gridded input NH3 emissions and the site's actual (rather low) pollution climate. According to LOTOS-EUROS predictions, ammonia contributed most to modeled input ΣNr concentrations, whereas measurements showed NOx as the prevailing compound in ΣNr concentrations. Annual deposition estimates from measurements and modeling were in the range of minimum and maximum estimates determined from CBT being at 3.8 ± 0.5 and 6.7 ± 0.3 kg N ha−1 a−1, respectively. By adding locally measured wet-only deposition, we estimated an annual total nitrogen deposition input between 11.5 and 14.8 kg N ha−1 a−1, which is within the critical load ranges proposed for deciduous and coniferous forests.

Measurements and predictions of ambient air particulates dry depositions at Taichung Shuinan Economic and Trade Park (T.S.E.T.P) during summer and autumn seasons

This study collected ambient air particulate concentrations and dry depositions at Taichung Shuinan Economic and Trade Park (T.S.E.T.P.) sampling site. The global dry depositions model was applied with known particle sizes, pollutant concentrations in ambient air pollutants dry deposition estimates at T.S.E.T.P. site in Central Taiwan. Statistical analysis of the correlated relationships among ambient air particulate concentration, dry depositions, and dry deposition velocities with respect to the meteorological conditions at T.S.E.T.P. site was also conducted. The results indicated that the average dry deposition fluxes were 377.81 µg/m2*min, the average TSP concentrations were 41.53 µg/m3, and the average dry depositions velocity (Vd ) was 15.26 cm/s. In addition, 40 μm was selected as the best ambient air particulate size for the calculated dry deposition velocities to estimate ambient air dry deposition fluxes using the Global model at this T.S.E.T.P. sampling site. Moreover, ambient air particulates concentrations were higher in the fall season than that of the summer season. Sincepollutants parcels were not easily diffused during the fall season because of the low mixed atmospheric layer in this season. Therefore, atmospheric particulates concentrations were higher from the northern side than that of southern side in this study. Furthermore, wind speed V.S. particulate dry depositions and wind V.S. dry depositions velocity displayed a moderate correlated relationship, while particulate dry depositions V.S. particulate dry depositions velocity presented the highest correlated relationship at this T.S.E.T.P. sampling site. However, particulate dry depositions and dry depositions velocity presented significant differences. Finally, particulate dry depositions and dry depositions velocity were not only highly correlation related but also displayed significant differences at the T.S.E.T.P. sampling site.

Estimation of the historical dry deposition of air pollution indoors to the monumental paintings by Edvard Munch in the University Aula, in Oslo, Norway

The historical (1835–2020) deposition of major air pollutants (SO2, NOx, O3 and PM2.5) indoors, as represented by the monumental Edvard Munch paintings (c. 220 m2) installed in 1916 in the Oslo University Aula in Norway, were approximated from the outdoor air concentrations, indoor to outdoor concentration ratios and dry deposition velocities. The annual deposition of the pollutants to the paintings was found to have been 4–25 times lower than has been reported to buildings outdoors in the urban background in the centre of Oslo. It reflected the outdoor deposition but varied less, from 0.3 to 1.2 g m−2 a−1. The accumulated deposition since 1916, and then not considering the regularly performed cleaning of the paintings, was found to have been 43 ± 13 g m−2, and 110 ± 40 g m−2 in a similar situation since 1835. The ozone deposition, and the PM2.5 deposition before the 1960s, were a relatively larger part of the accumulated total indoor (to the paintings) than reported outdoor deposition. About 18 and 33 times more O3 than NOx and PM2.5 deposition was estimated to the paintings in 2020, as compared to the about similar reported outdoor dry deposition of O3 and NOx. The deposition of PM2.5 to the paintings was probably reduced with about 62% (50–80%) after installation of mechanical filtration in 1975 and was estimated to be 0.011 (± 0.006) g m−2 in 2020.Graphical

Recycling and persistence of iodine 127 and 129 in forested environments: A modelling approach

Differences in the source and behaviour of 129I compared to 127I isotopes have been described for a variety of surface environments, but little is known about the cycling rates of each isotope in terrestrial ecosystems. We developed a compartment model of the iodine cycle in a forest ecosystem, with a labile and non-labile pool to simplify the complex fate of iodine in the forest floor and soil. Simulations were performed using atmospheric 127I and 129I inputs for sites differing in climate, vegetation, and soil. In general, considering dry deposition in addition to wet deposition improved model simulations. Model results support the view that soil is the sink for atmospheric iodine deposited in forest ecosystems, while tree vegetation has little influence on long-term iodine budgets. Modelling also showed that iodine cycling reaches equilibrium after a period of about 5000 years, mainly due to a gradual incorporation of iodine into the bulk stabilised soil organic matter. At steady state, this pool of non-labile iodine in soil can retain about 20% of total deposition with a mean residence time of 900 years, while the labile iodine pool is renewed after 90 years. The proportions of modern anthropogenic 129I in each modelled pool reflect those of stable 127I at least several decades after input to the forest; this result explains why isotopic disequilibrium is common in field data analysis. Volatilisation plays a central role in regulating iodine storage in soil and, therefore, its residence time, while drainage is a minor export pathway, except at some calcareous sites. Dynamic modelling has been particularly helpful for gaining insight into the long-term response of iodine partitioning to continuous, single or even varying deposition. Our modelling study suggested that better estimates of dry deposition of atmospheric iodine, weathering of parent rock, and volatilisation of the deposited iodine from soil and vegetation will be required for reliable predictions of iodine cycling in specific forests, because these processes remain insufficiently explored.

Estimation of Atmospheric Dry and Wet Deposition of Particulate Elements at Four Monitoring Sites in the Canadian Athabasca Oil Sands Region

AbstractThis study develops a framework for estimating atmospheric dry deposition using the inferential approach, and wet deposition using the scavenging ratio approach for particulate elements monitored in the Athabasca oil sands region (AOSR) of Canada. The framework was applied to four monitoring sites (AMS01, AMS04, AMS17, and AMS18) in the AOSR where ambient concentrations of particulate elements were collected in 2016–2017 to estimate atmospheric dry and wet deposition fluxes of 35 elements, including eight USEPA priority elements. Annual total (dry + wet) deposition of the individual elements in PM10 varied by about five orders of magnitudes, ranging from 3 (μg/m2/year) for Yb to 172,000 (μg/m2/year) for Si. Total deposition of the elements that are typically associated with bitumen (e.g., Mo, Ni, and V) did not show any statistically significant spatial variations (p < 0.05). However, S, which is significantly enriched in bitumen and its byproducts, had up to 38% higher fluxes at AMS01 and AMS17 (closer to the oil sands facilities) than at AMS18 (background site). Wet deposition fluxes dominated over the dry deposition fluxes for almost all elements due to efficient snow scavenging and prolonged winter season. Dry deposition fluxes of the crustal elements were higher in the summer season due to their elevated concentrations in PM2.5–10 during the warmer months, whereas most anthropogenic elements did not show any significant seasonal variations. The total deposition of the individual priority toxic elements considered in this study ranged from 6 (μg/m2/year) (Cd; AMS18) to 2,290 (µg/m2/year) (Zn; AMS04), and ranked as follows: Zn > Cu > Ni > Cr > Sb > As > Pb > Cd.

Declining dry deposition of NO2 and SO2 with diverse spatiotemporal patterns in China from 2013 to 2018

The nitrogen and sulfur deposition results in damages on ecosystems, while the lack of direct observation on dry deposition limits our understanding of the total deposition. This study aimed to improve the methodology and estimates of NO2 and SO2 dry deposition in China and to explore the efficacy of China's recent emission control measures on dry deposition at the national and regional scales. We combined the random forest algorithm and the GEOS-Chem chemical transport model to predict the dry deposition fluxes of NO2 and SO2 and their inter-annual variabilities during 2013–2018 in mainland China. The annual NO2 dry deposition ranged between 2.1 and 3.1 kg N ha−1 yr−1, with an annual reduction rate of 0.21 kg N ha−1 yr−1 over this period. The areas with large deposition were located in the east, while the biggest reduction existed in the relatively clean Tibet Plateau region. The annual SO2 dry deposition ranged between 7.5 and 18.4 kg S ha−1 yr−1, with the annual reduction rate at 2.4 kg S ha−1 yr−1. Both the magnitude and relative reduction in the north were generally larger than the south. Regarding the four typical economically developed regions, the NO2 deposition declined slower than the national average, while SO2 generally declined faster than or equivalently to the national average, except for Pearl River Delta. The reduced emissions attributed to the national action on air pollution control were identified as an important reason for the declining deposition. However, the increased traffic and industrial capacity in the east weakened its benefit on NO2.

A comparison of two bidirectional air-surface exchange models for gaseous elemental mercury over vegetated surfaces

Uncertainties exist in the current estimates of atmospheric dry deposition and air-surface exchange of atmospheric mercury in chemical transport models and monitoring networks. To quantitatively assess these uncertainties, two bidirectional air-surface exchange models for gaseous elemental mercury (Hg0), originally developed by Wang et al. (2014, Atmos. Chem. Phys., doi:10.5194/acp-14-6273-2014) and Wright and Zhang (2015, J. Adv. Model. Earth Syst., doi:10.1002/2014MS000367), were compared quantitatively. The two models were applied to two vegetated land covers, including a deciduous broadleaf forest and a cropland, near a monitoring site in Georgia, USA for calculating air-surface exchange fluxes of Hg0. The model inputs include measured 2-hourly ambient Hg0 concentrations and archived surface meteorology data produced from a weather forecast model. The estimated annual net fluxes differed significantly between the two models, i.e., −0.7 μg m−2yr−1 by Wang et al.’s model vs. −8.6 μg m−2yr−1 by Wright & Zhang's model over the deciduous broadleaf forest and 8.4 μg m−2yr−1 vs. −10.7 μg m−2yr−1 over the cropland. When considering dry deposition and emission fluxes separately, similar deposition fluxes were produced by the two models, regardless of season and land cover, due to the similar canopy resistance formulas used in the two models. Much higher soil and lower stomatal emission fluxes were produced by Wang et al.’s model than Wright & Zhang's model (soil: 30 vs. 8.9 μg m−2yr−1 and stomata: 0.5 vs. 8.3 μg m−2yr−1, averaged over the two canopies) due to the very different emission potentials used in the two models. Cuticle emission fluxes contributed less than 0.1% to the total emission flux in Wang et al.’s model, and were not considered in Wright & Zhang's model. The differences in soil emission flux, total emission flux, and net flux were more pronounced in winter than in the other seasons. The large differences in the net fluxes between the two models were primarily caused by their very different schemes of soil emission potential.

Comparison of Methods for the Estimation of Total Inorganic Nitrogen Deposition to Forests in Germany

A reliable quantification of total inorganic nitrogen (TIN) deposition to forests is required for the evaluation of ecological effects of TIN inputs to forests and to monitor the success of clean-air policy. As direct measurements are scarce, different modeling approaches have been developed to estimate TIN deposition to forests. Three common methods are the (i) “canopy budget model,” (ii) “inferential method,” and (iii) “emission based estimates” using a chemical transport model. Previous studies have reported considerable and site-specific differences between these methods, complicating the interpretation of results. We use data from more than 100 German intensive forest monitoring sites over a period of 16 years for a cross-comparison of these approaches. Non-linear mixed-effect models were applied to evaluate how factors like meteorology, terrain and stand characteristics affect discrepancies between the model approaches. Taking into account the uncertainties in deposition estimates, there is a good agreement between the canopy budget and the inferential method when using semi-empirical correction factors for deposition velocity. Wet deposition estimates of the emission based approach were in good agreement with wet-only corrected bulk open field deposition measurements used by the other two approaches. High precipitation amounts partly explained remaining differences in wet deposition. Larger discrepancies were observed when dry deposition estimates are compared between the emissions based approach and the other two approaches, which appear to be related to a combination of meteorological conditions and tree species effects.

Global estimates of dry ammonia deposition inferred from space-measurements

Ammonia (NH3), as an alkaline gas, contributes substantially to atmospheric nitrogen deposition, which can cause biodiversity loss, water eutrophication and soil acidification. Advances in the application of satellite observations allow us to gain deeper insights into atmospheric NH3 concentrations at large spatial scales. A new satellite-based methodology is proposed for estimating dry NH3 deposition with consideration of bi-directional NH3 exchange. We estimate the global dry NH3 deposition for nine years (2008–2016) by using the Infrared Atmospheric Sounding Interferometer Instrument (IASI) NH3 retrievals. Satellite-based dry NH3 deposition is in general consistent with measured dry NH3 deposition over the monitoring sites (R2 = 0.65). Global dry NH3 deposition over 8 kg N ha−1 is mainly distributed in the Eastern China, Northern and Central Pakistan, and Northern India. An annual increase rate of 0.27 and 0.13 kg N ha−1 y−1 in dry NH3 deposition during 2008–2016 occurs in Eastern China and Sichuan Basin, which are the major Chinese agricultural regions. The NH3 compensation point is high during warm months, and can be above 1 μg m−3 such as in Eastern China, implying the importance of considering the NH3 compensation points for estimating dry NH3 deposition. We find, if the upward NH3 flux was ignored, it will cause 11%, 17%, 5% and 3% overestimation in dry NH3 deposition in Eastern China, Northern India, Eastern United States and Western Europe, respectively. This study presents the potential of using the satellite retrievals to estimate the large-scale dry NH3 deposition, and the methodology is able to provide temporally continuous and spatially complete fine-resolution datasets.

Carbon–nitrogen interactions in European forests and semi-natural vegetation – Part 1: Fluxes and budgets of carbon, nitrogen and greenhouse gases from ecosystem monitoring and modelling

Abstract. The impact of atmospheric reactive nitrogen (Nr) deposition on carbon (C) sequestration in soils and biomass of unfertilized, natural, semi-natural and forest ecosystems has been much debated. Many previous results of this dC∕dN response were based on changes in carbon stocks from periodical soil and ecosystem inventories, associated with estimates of Nr deposition obtained from large-scale chemical transport models. This study and a companion paper (Flechard et al., 2020) strive to reduce uncertainties of N effects on C sequestration by linking multi-annual gross and net ecosystem productivity estimates from 40 eddy covariance flux towers across Europe to local measurement-based estimates of dry and wet Nr deposition from a dedicated collocated monitoring network. To identify possible ecological drivers and processes affecting the interplay between C and Nr inputs and losses, these data were also combined with in situ flux measurements of NO, N2O and CH4 fluxes; soil NO3- leaching sampling; and results of soil incubation experiments for N and greenhouse gas (GHG) emissions, as well as surveys of available data from online databases and from the literature, together with forest ecosystem (BASFOR) modelling. Multi-year averages of net ecosystem productivity (NEP) in forests ranged from −70 to 826 g C m−2 yr−1 at total wet + dry inorganic Nr deposition rates (Ndep) of 0.3 to 4.3 g N m−2 yr−1 and from −4 to 361 g C m−2 yr−1 at Ndep rates of 0.1 to 3.1 g N m−2 yr−1 in short semi-natural vegetation (moorlands, wetlands and unfertilized extensively managed grasslands). The GHG budgets of the forests were strongly dominated by CO2 exchange, while CH4 and N2O exchange comprised a larger proportion of the GHG balance in short semi-natural vegetation. Uncertainties in elemental budgets were much larger for nitrogen than carbon, especially at sites with elevated Ndep where Nr leaching losses were also very large, and compounded by the lack of reliable data on organic nitrogen and N2 losses by denitrification. Nitrogen losses in the form of NO, N2O and especially NO3- were on average 27 % (range 6 %–54 %) of Ndep at sites with Ndep < 1 g N m−2 yr−1 versus 65 % (range 35 %–85 %) for Ndep > 3 g N m−2 yr−1. Such large levels of Nr loss likely indicate that different stages of N saturation occurred at a number of sites. The joint analysis of the C and N budgets provided further hints that N saturation could be detected in altered patterns of forest growth. Net ecosystem productivity increased with Nr deposition up to 2–2.5 g N m−2 yr−1, with large scatter associated with a wide range in carbon sequestration efficiency (CSE, defined as the NEP ∕ GPP ratio). At elevated Ndep levels (> 2.5 g N m−2 yr−1), where inorganic Nr losses were also increasingly large, NEP levelled off and then decreased. The apparent increase in NEP at low to intermediate Ndep levels was partly the result of geographical cross-correlations between Ndep and climate, indicating that the actual mean dC∕dN response at individual sites was significantly lower than would be suggested by a simple, straightforward regression of NEP vs. Ndep.

Dry Deposition of Ozone over Land: Processes, Measurement, and Modeling.

Dry deposition of ozone is an important sink of ozone in near surface air. When dry deposition occurs through plant stomata, ozone can injure the plant, altering water and carbon cycling and reducing crop yields. Quantifying both stomatal and nonstomatal uptake accurately is relevant for understanding ozone's impact on human health as an air pollutant and on climate as a potent short-lived greenhouse gas and primary control on the removal of several reactive greenhouse gases and air pollutants. Robust ozone dry deposition estimates require knowledge of the relative importance of individual deposition pathways, but spatiotemporal variability in nonstomatal deposition is poorly understood. Here we integrate understanding of ozone deposition processes by synthesizing research from fields such as atmospheric chemistry, ecology, and meteorology. We critically review methods for measurements and modeling, highlighting the empiricism that underpins modeling and thus the interpretation of observations. Our unprecedented synthesis of knowledge on deposition pathways, particularly soil and leaf cuticles, reveals process understanding not yet included in widely-used models. If coordinated with short-term field intensives, laboratory studies, and mechanistic modeling, measurements from a few long-term sites would bridge the molecular to ecosystem scales necessary to establish the relative importance of individual deposition pathways and the extent to which they vary in space and time. Our recommended approaches seek to close knowledge gaps that currently limit quantifying the impact of ozone dry deposition on air quality, ecosystems, and climate.

Ammonia measurements from space with the Cross-track Infrared Sounder: characteristics and applications

Abstract. Despite its clear importance, the monitoring of atmospheric ammonia, including its sources, sinks, and links to the greater nitrogen cycle, remains limited. Satellite data are helping to fill the gap in monitoring from sporadic conventional ground- and aircraft-based observations to better inform policymakers and assess the impact of any ammonia-related policies. Presented is a description and survey that demonstrate the capabilities of the Cross-track Infrared Sounder (CrIS) ammonia product for monitoring, air quality forecast model evaluation, dry deposition estimates, and emission estimates from an agricultural hotspot. For model evaluation, while there is a general agreement in the spatial allocation of known major agricultural ammonia hotspots across North America, the satellite observations show some high-latitude regions during peak forest fire activity often have ammonia concentrations approaching those in agricultural hotspots. The CrIS annual ammonia dry depositions in Canada (excluding the territories) and the US have average and annual variability values of ∼0.8±0.08 and ∼1.23±0.09 Tg N yr−1, respectively. These satellite-derived dry depositions of reactive nitrogen from NH3 with NO2 show an annual ratio of NH3 compared to their sum (NH3+NO2) of ∼82 % and ∼55 % in Canada and the US, respectively. Furthermore, we show the use of CrIS satellite observations to estimate annual and seasonal emissions near Lethbridge, Alberta, Canada, a region dominated by high-emission concentrated animal feeding operations (CAFOs); the satellite annual emission estimate of 37.1±6.3 kt yr−1 is at least double the value reported in current bottom-up emission inventories for this region.

The impact of air pollutant deposition on solar energy system efficiency: An approach to estimate PV soiling effects with the Community Multiscale Air Quality (CMAQ) model

Deposition and accumulation of aerosol particles on photovoltaics (PV) panels, which is commonly referred to as “soiling of PV panels,” impacts the performance of the PV energy system. It is desirable to estimate the soiling effect at different locations and times for modeling the PV system performance and devising cost-effective mitigation. This study presents an approach to estimate the soiling effect by utilizing particulate matter (PM) dry deposition estimates from air quality model simulations. The Community Multiscale Air Quality (CMAQ) modeling system used in this study was developed by the U.S. Environmental Protection Agency (U.S. EPA) for air quality assessments, rule-making, and research. Three deposition estimates based on different surface roughness length parameters assumed in CMAQ were used to illustrate the soling effect in different land-use types. The results were analyzed for three locations in the U.S. for year 2011. One urban and one suburban location in Colorado were selected because there have been field measurements of particle deposition on solar panels and analysis on the consequent soiling effect performed at these locations. The third location is a coastal city in Texas, the City of Brownsville. These three locations have distinct ambient environments. CMAQ underestimates particle deposition by 40% to 80% when compared to the field measurements at the two sites in Colorado due to the underestimations in both the ambient PM10 concentration and deposition velocity. The estimated panel transmittance sensitivity due to the deposited particles is higher than the sensitivity obtained from the measurements in Colorado. The final soiling effect, which is transmittance loss, is estimated as 3.17 ± 4.20% for the Texas site, 0.45 ± 0.33%, and 0.31 ± 0.25% for the Colorado sites. Although the numbers are lower compared to the measurements in Colorado, the results are comparable with the soiling effects observed in U.S.

Observation- and Model-Based Estimates of Particulate Dry Nitrogen Deposition to the Oceans.

Anthropogenic nitrogen (N) emissions to the atmosphere have increased significantly the deposition of nitrate (NO3-) and ammonium (NH4+) to the surface waters of the open ocean, with potential impacts on marine productivity and the global carbon cycle. Global-scale understanding of the impacts of N deposition to the oceans is reliant on our ability to produce and validate models of nitrogen emission, atmospheric chemistry, transport and deposition. In this work, ~2900 observations of aerosol NO3- and NH4+ concentrations, acquired from sampling aboard ships in the period 1995 - 2012, are used to assess the performance of modelled N concentration and deposition fields over the remote ocean. Three ocean regions (the eastern tropical North Atlantic, the northern Indian Ocean and northwest Pacific) were selected, in which the density and distribution of observational data were considered sufficient to provide effective comparison to model products. All of these study regions are affected by transport and deposition of mineral dust, which alters the deposition of N, due to uptake of nitrogen oxides (NOx) on mineral surfaces. Assessment of the impacts of atmospheric N deposition on the ocean requires atmospheric chemical transport models to report deposition fluxes, however these fluxes cannot be measured over the ocean. Modelling studies such as the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), which only report deposition flux are therefore very difficult to validate for dry deposition. Here the available observational data were averaged over a 5° × 5° grid and compared to ACCMIP dry deposition fluxes (ModDep) of oxidised N (NOy) and reduced N (NHx) and to the following parameters from the TM4-ECPL (TM4) model: ModDep for NOy, NHx and particulate NO3- and NH4+, and surface-level particulate NO3- and NH4+ concentrations. As a model ensemble, ACCMIP can be expected to be more robust than TM4, while TM4 gives access to speciated parameters (NO3- and NH4+) that are more relevant to the observed parameters and which are not available in ACCMIP. Dry deposition fluxes (CalDep) were calculated from the observed concentrations using estimates of dry deposition velocities. Model - observation ratios, weighted by grid-cell area and numbers of observations, (RA,n) were used to assess the performance of the models. Comparison in the three study regions suggests that TM4 over-estimates NO3- concentrations (RA,n = 1.4 - 2.9) and under-estimates NH4+ concentrations (RA,n = 0.5 - 0.7), with spatial distributions in the tropical Atlantic and northern Indian Ocean not being reproduced by the model. In the case of NH4+ in the Indian Ocean, this discrepancy was probably due to seasonal biases in the sampling. Similar patterns were observed in the various comparisons of CalDep to ModDep (RA,n = 0.6 - 2.6 for NO3-, 0.6 - 3.1 for NH4+). Values of RA,n for NHx CalDep - ModDep comparisons were approximately double the corresponding values for NH4+ CalDep - ModDep comparisons due to the significant fraction of gas-phase NH3 deposition incorporated in the TM4 and ACCMIP NHx model products. All of the comparisons suffered due to the scarcity of observational data and the large uncertainty in dry deposition velocities used to derive deposition fluxes from concentrations. These uncertainties have been a major limitation on estimates of the flux of material to the oceans for several decades. Recommendations are made for improvements in N deposition estimation through changes in observations, modelling and model - observation comparison procedures. Validation of modelled dry deposition requires effective comparisons to observable aerosol-phase species concentrations and this cannot be achieved if model products only report dry deposition flux over the ocean.

Joint analysis of deposition fluxes and atmospheric concentrations of inorganic nitrogen and sulphur compounds predicted by six chemistry transport models in the frame of the EURODELTAIII project

In the framework of the UNECE Task Force on Measurement and Modelling (TFMM) under the Convention on Long-range Transboundary Air Pollution (LRTAP), the EURODELTAIII project is evaluating how well air quality models are able to reproduce observed pollutant air concentrations and deposition fluxes in Europe. In this paper the sulphur and nitrogen deposition estimates of six state-of-the-art regional models (CAMx, CHIMERE, EMEP MSC-W, LOTOS-EUROS, MINNI and CMAQ) are evaluated and compared for four intensive EMEP measurement periods (25 Feb–26 Mar 2009; 17 Sep–15 Oct 2008; 8 Jan–4 Feb 2007 and 1–30 Jun 2006).For sulphur, this study shows the importance of including sea salt sulphate emissions for obtaining better model results; CMAQ, the only model considering these emissions in its formulation, was the only model able to reproduce the high measured values of wet deposition of sulphur at coastal sites. MINNI and LOTOS-EUROS underestimate sulphate wet deposition for all periods and have low wet deposition efficiency for sulphur.For reduced nitrogen, all the models underestimate both wet deposition and total air concentrations (ammonia plus ammonium) in the summer campaign, highlighting a potential lack of emissions (or incoming fluxes) in this period. In the rest of campaigns there is a general underestimation of wet deposition by all models (MINNI and CMAQ with the highest negative bias), with the exception of EMEP, which underestimates the least and even overestimates deposition in two campaigns. This model has higher scavenging deposition efficiency for the aerosol component, which seems to partly explain the different behaviour of the models.For oxidized nitrogen, CMAQ, CAMx and MINNI predict the lowest wet deposition and the highest total air concentrations (nitric acid plus nitrates). Comparison with observations indicates a general underestimation of wet oxidized nitrogen deposition by these models, as well as an overestimation of total air concentration for all the campaigns, except for the 2006 campaign. This points to a low efficiency in the wet deposition of oxidized nitrogen for these models, especially with regards to the scavenging of nitric acid, which is the main driver of oxidized N deposition for all the models. CHIMERE, LOTOS-EUROS and EMEP agree better with the observations for both wet deposition and air concentration of oxidized nitrogen, although CHIMERE seems to overestimate wet deposition in the summer period. This requires further investigation, as the gas-particle equilibrium seems to be biased towards the gas phase (nitric acid) for this model.In the case of MINNI, the frequent underestimation of wet deposition combined with an overestimation of atmospheric concentrations for the three pollutants indicates a low efficiency of the wet deposition processes. This can be due to several reasons, such as an underestimation of scavenging ratios, large vertical concentration gradients (resulting in small concentrations at cloud height) or a poor parameterization of clouds.Large differences between models were also found for the estimates of dry deposition. However, the lack of suitable measurements makes it impossible to assess model performance for this process. These uncertainties should be addressed in future research, since dry deposition contributes significantly to the total deposition for the three deposited species, with values in the same range as wet deposition for most of the models, and with even higher values for some of them, especially for reduced nitrogen.

Comparison of dry deposition estimates of AERMOD and CALPUFF from area sources in flat terrain

The dry deposition algorithms of AERMOD and CALPUFF were compared, studying emissions from hypothetical area and point sources in flat terrain. The deposited fractions calculated by AERMOD and CALPUFF are different for the C, D and F stability classes. In all the studied scenarios the differences between the deposited fractions calculated by AERMOD and CALPUFF are much smaller than those calculated previously in complex terrain. Yet, the detected differences in the deposited fractions may affect the ambient concentrations calculated by AERMOD and CALPUFF in the receptor points as a part of an environmental impact assessment and lead to different conclusions on the residents' exposure. The distinct account of AERMOD and CALPUFF to certain wind speeds and stability classes, and their different algorithms for calculating the dispersion coefficients, is the only explanation for the different estimates of deposited fractions between AERMOD and CALPUFF over absolutely flat terrain.

Assessment of Global Mercury Deposition through Litterfall

There is a large uncertainty in the estimate of global dry deposition of atmospheric mercury (Hg). Hg deposition through litterfall represents an important input to terrestrial forest ecosystems via cumulative uptake of atmospheric Hg (most Hg(0)) to foliage. In this study, we estimate the quantity of global Hg deposition through litterfall using statistical modeling (Monte Carlo simulation) of published data sets of litterfall biomass production, tree density, and Hg concentration in litter samples. On the basis of the model results, the global annual Hg deposition through litterfall is estimated to be 1180 ± 710 Mg yr(-1), more than two times greater than the estimate by GEOS-Chem. Spatial distribution of Hg deposition through litterfall suggests that deposition flux decreases spatially from tropical to temperate and boreal regions. Approximately 70% of global Hg(0) dry deposition occurs in the tropical and subtropical regions. A major source of uncertainty in this study is the heterogeneous geospatial distribution of available data. More observational data in regions (Southeast Asia, Africa, and South America) where few data sets exist will greatly improve the accuracy of the current estimate. Given that the quantity of global Hg deposition via litterfall is typically 2-6 times higher than Hg(0) evasion from forest floor, global forest ecosystems represent a strong Hg(0) sink.