Improving Estimates of Sulfur, Nitrogen, and Ozone Total Deposition through Multi-Model and Measurement-Model Fusion Approaches

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Joshua S. Fu is John D. Tickle Professor and James G. Gibson Professor in the Department of Civil and Environmental Engineering at the University of Tennessee and Joint Appointment Professor in Computational Earth Sciences Group in Computational Sciences and Engineering Division at Oak Ridge National Laboratory. He has served Vice-Chair and member of the WMO Model Measurement Fusion Initiative, contributed as a coauthor of the Final Report of the Hemispheric Transport of Air Pollution for the UN ECE Hemispheric Transport of Air Pollution, and reviewing committee member for air quality status in East Asia for the EANET located in Japan. He also was a coauthor of Technical Report, Climate Change and Infrastructure, Urban System, and Vulnerability, to the U.S. Department of Energy in the support of the National Climate Assessment in 2012. He has received numerous awards from national and international associations and a Fellow of the AAAS and of the A&WMA and Board-Certified Environmental Engineering Member from AAEES and other distinguished and endowed professorship awards. Joshua has published more than 180 refereed journal articles and 110 peer-reviewed conference proceedings. Joshua obtained his PhD from North Carolina State University, MS from UCLA, and BS from Taiwan’s National Cheng Kung University.

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Gregory R. Carmichael is the Karl Kammermeyer professor of chemical and biochemical engineering at the University of Iowa, and codirector of the Center for Global and Regional Environmental Research. His research is focused on air pollution and climate change, where he uses comprehensive computer models and big data to simulate the interactions of air pollutants with weather and climate, and to estimate resulting environmental impacts. His models are also used to evaluate effectiveness of various air pollution and climate change mitigation strategies. He has authored or coauthored over 380 scientific publications. He has received numerous awards, including the American Institute of Chemical Engineer’s Lawrence K. Cecil Award for outstanding chemical engineering contribution and achievement in the preservation or improvement of the environment. He is a Fellow of the American Institute of Chemical Engineers and of the American Geophysical Union. He serves on numerous international advisory boards including serving as chair of the UN World Meteorological Organization’s Environmental Pollution and Atmospheric Chemistry Scientific Steering Committee.

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Frank Dentener has worked for 30 years in the field of climate change, agriculture, and atmospheric pollution. Frank is a senior expert and group leader at the European Commission’s Joint Research Centre. He completed a Ph.D. in Physics with Nobel prize-laureate Paul Crutzen at Utrecht University. He is a member of the scientific advisory board of the JPI FACCE, and cochair of WMO’s Scientific Advisory Group on near-real-time applications, member of the WMO Model Measurement Fusion initiative, and has served on a variety of international commissions. He has (co-) authored more than 200 peer-reviewed publications and four IPCC reports, Hirsch factor 94, and is a Clarivate highly cited scientist since 2015. Frank held assistant professorships at Wageningen and Utrecht University, The Netherlands, PrivatDozent at the ETH in Switzerland, and is currently affiliated with the Politechnical University of Torino. He supervised and examined ca. 10 Ph.D. and Habilitation candidates. Frank is an expert in atmospheric chemistry–land interactions, including ozone impacts on agriculture, agricultural production systems, climate change, and mitigation and adaptation.

This article references 64 other publications.

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   Ecological applications : a publication of the Ecological Society of America (2010), 20 (1), 30-59 ISSN:1051-0761.

   Atmospheric nitrogen (N) deposition is a recognized threat to plant diversity in temperate and northern parts of Europe and North America. This paper assesses evidence from field experiments for N deposition effects and thresholds for terrestrial plant diversity protection across a latitudinal range of main categories of ecosystems, from arctic and boreal systems to tropical forests. Current thinking on the mechanisms of N deposition effects on plant diversity, the global distribution of G200 ecoregions, and current and future (2030) estimates of atmospheric N-deposition rates are then used to identify the risks to plant diversity in all major ecosystem types now and in the future. This synthesis paper clearly shows that N accumulation is the main driver of changes to species composition across the whole range of different ecosystem types by driving the competitive interactions that lead to composition change and/or making conditions unfavorable for some species. Other effects such as direct toxicity of nitrogen gases and aerosols, long-term negative effects of increased ammonium and ammonia availability, soil-mediated effects of acidification, and secondary stress and disturbance are more ecosystem- and site-specific and often play a supporting role. N deposition effects in mediterranean ecosystems have now been identified, leading to a first estimate of an effect threshold. Importantly, ecosystems thought of as not N limited, such as tropical and subtropical systems, may be more vulnerable in the regeneration phase, in situations where heterogeneity in N availability is reduced by atmospheric N deposition, on sandy soils, or in montane areas. Critical loads are effect thresholds for N deposition, and the critical load concept has helped European governments make progress toward reducing N loads on sensitive ecosystems. More needs to be done in Europe and North America, especially for the more sensitive ecosystem types, including several ecosystems of high conservation importance. The results of this assessment show that the vulnerable regions outside Europe and North America which have not received enough attention are ecoregions in eastern and southern Asia (China, India), an important part of the mediterranean ecoregion (California, southern Europe), and in the coming decades several subtropical and tropical parts of Latin America and Africa. Reductions in plant diversity by increased atmospheric N deposition may be more widespread than first thought, and more targeted studies are required in low background areas, especially in the G200 ecoregions.
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   Bowman, W. D.; Cleveland, C. C.; Halada, L.; Hresko, J.; Baron, J. S. Negative Impact of Nitrogen Deposition on Soil Buffering Capacity. Nat. Geosci. 2008, 1 (11), 767– 770,  DOI: 10.1038/ngeo339

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   Nature Geoscience (2008), 1 (11), 767-770CODEN: NGAEBU; ISSN:1752-0894. (Nature Publishing Group)

   Anthropogenic nitrogen deposition over the past half century has had a detrimental impact on temperate ecosystems in Europe and North America, resulting in soil acidification and a redn. in plant biodiversity. During the acidification process, soils release base cations, such as calcium and magnesium, neutralizing the increase in acidity. Once these base cations have been depleted, aluminum is released from the soils, often reaching toxic levels. Here, the authors present results from a nitrogen deposition expt. that suggests that a long legacy of acid deposition in the Western Tatra Mountains of Slovakia has pushed soils to a new threshold of acidification usually assocd. with acid mine drainage soils. Increases in nitrogen deposition in the region resulted in a depletion of both base cations and sol. aluminum and an increase in extractable iron concns. In conjunction with this, a nitrogen-deposition-induced redn. in the biomass of vascular plants was obsd., assocd. with a decrease in shoot calcium and magnesium concns. It is suggested that this site, and potentially others in central Europe, have reached a new and potentially more toxic level of soil acidification in which aluminum release is superseded by iron release into soil water.
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   Doney, S. C.; Mahowald, N.; Lima, I.; Feely, R. A.; Mackenzie, F. T.; Lamarque, J.; Rasch, P. J. Impact of Anthropogenic Atmospheric Nitrogen and Sulfur Deposition on Ocean Acidification and the Inorganic Carbon System. Proc. Natl. Acad. Sci. U. S. A. 2007, 104 (37). 14580 DOI: 10.1073/pnas.0702218104

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   Impact of anthropogenic atmospheric nitrogen and sulfur deposition on ocean acidification and the inorganic carbon system

   Doney, Scott C.; Mahowald, Natalie; Lima, Ivan; Feely, Richard A.; Mackenzi, Fred T.; Lamarque, Jean-Francois; Rasch, Phil J.

   Proceedings of the National Academy of Sciences of the United States of America (2007), 104 (37), 14580-14585CODEN: PNASA6; ISSN:0027-8424. (National Academy of Sciences)

   Fossil fuel combustion and agriculture result in atm. deposition of 0.8 Tmol/yr reactive sulfur and 2.7 Tmol/yr nitrogen to the coastal and open ocean near major source regions in North America, Europe, and South and East Asia. Atm. inputs of dissocn. products of strong acids (HNO3 and H2SO4) and bases (NH3) alter surface seawater alky., pH, and inorg. carbon storage. We quantify the biogeochem. impacts by using atm. and ocean models. The direct acid/base flux to the ocean is predominately acidic (reducing total alky.) in the temperate Northern Hemisphere and alk. in the tropics because of ammonia inputs. However, because most of the excess ammonia is nitrified to nitrate (NO3-) in the upper ocean, the effective net atm. input is acidic almost everywhere. The decrease in surface alky. drives a net air-sea efflux of CO2, reducing surface dissolved inorg. carbon (DIC); the alky. and DIC changes mostly offset each other, and the decline in surface pH is small. Addnl. impacts arise from nitrogen fertilization, leading to elevated primary prodn. and biol. DIC drawdown that reverses in some places the sign of the surface pH and air-sea CO2 flux perturbations. On a global scale, the alterations in surface water chem. from anthropogenic nitrogen and sulfur deposition are a few percent of the acidification and DIC increases due to the oceanic uptake of anthropogenic CO2. However, the impacts are more substantial in coastal waters, where the ecosystem responses to ocean acidification could have the most severe implications for mankind.
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   Grennfelt, P.; Engleryd, A.; Forsius, M.; Hov, Å.; Rodhe, H.; Cowling, E. Acid Rain and Air Pollution: 50 Years of Progress in Environmental Science and Policy. Ambio 2020, 49 (4), 849– 864,  DOI: 10.1007/s13280-019-01244-4

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   Ambio (2020), 49 (4), 849-864CODEN: AMBOCX; ISSN:0044-7447. (Springer)

   A review. Because of its serious large-scale effects on ecosystems and its transboundary nature, acid rain received for a few decades at the end of the last century wide scientific and public interest, leading to coordinated policy actions in Europe and North America. Through these actions, in particular those under the UNECE Convention on Long-range Transboundary Air Pollution, air emissions were substantially reduced, and ecosystem impacts decreased. Widespread scientific research, long-term monitoring, and integrated assessment modeling formed the basis for the policy agreements. In this paper, which is based on an international symposium organised to commemorate 50 years of successful integration of air pollution research and policy, we briefly describe the scientific findings that provided the foundation for the policy development. We also discuss important characteristics of the science-policy interactions, such as the crit. loads concept and the large-scale ecosystem field studies. Finally, acid rain and air pollution are set in the context of future societal developments and needs, e.g. the UN's Sustainable Development Goals. We also highlight the need to maintain and develop supporting scientific infrastructures.
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   Tian, D.; Niu, S. A Global Analysis of Soil Acidification Caused by Nitrogen Addition. Environ. Res. Lett. 2015, 10 (2). 024019 DOI: 10.1088/1748-9326/10/2/024019 .

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   Nitrogen (N) deposition-induced soil acidification has become a global problem. However, the response patterns of soil acidification toNaddn. and the underlyingmechanisms remain far from clear. Here, we conducted ameta-anal. of 106 studies to reveal global patterns of soil acidification in responses toNaddn.We found thatNaddn. significantly reduced soil pHby 0.26 on av. globally. However, the responses of soil pH varied with ecosystem types,Naddn. rate,Nfertilization forms, and exptl. durations. Soil pH decreasedmost in grassland, whereas boreal forest was not obsd. a decrease toNaddn. in soil acidification. Soil pH decreased linearly withNaddn. rates. Addn. of urea andNH4NO3 contributedmore to soil acidification thanNH4-form fertilizer. When exptl. duration was longer than 20 years, Naddn. effects on soil acidification diminished. Environmental factors such as initial soil pH, soil carbon and nitrogen content, pptn., and temp. all influenced the responses of soil pH. Base cations of Ca2+,Mg2+ and K+ were crit. important in buffering against N-induced soil acidification at the early stage. However,Naddn. has shifted global soils into the Al3+ buffering phase. Overall, this study indicates that acidification in global soils is very sensitive toN deposition, which is greatlymodified by biotic and abiotic factors. Global soils are now at a buffering transition from base cations (Ca2+,Mg2+ and K+) to non-base cations (Mn2+ and Al3+). This calls our attention to care about the limitation of base cations and the toxic impact of non-base cations for terrestrial ecosystems withNdeposition.
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   Chen, X.; Wang, Y.; Ye, C.; Zhou, W.; Cai, Z.; Yang, H.; Han, X. Atmospheric Nitrogen Deposition Associated with the Eutrophication of Taihu Lake. J. Chem. 2018, 2018, 2018,  DOI: 10.1155/2018/4017107

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    Environmental Pollution (Oxford, United Kingdom) (2019), 244 (), 980-994CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)

    Av. nitrogen (N) deposition across Europe has declined since the 1990s. This resulted in decreased N inputs to forest ecosystems esp. in Central and Western Europe where deposition levels are highest. While the impact of atm. N deposition on forests has been receiving much attention for decades, ecosystem responses to the decline in N inputs received less attention. Here, we review observational studies reporting on trends in a no. of indicators: soil acidification and eutrophication, understory vegetation, tree nutrition (foliar element concns.) as well as tree vitality and growth in response to decreasing N deposition across Europe. Ecosystem responses varied with limited decrease in soil soln. nitrate concns. and potentially also foliar N concns. There was no large-scale response in understory vegetation, tree growth, or vitality. Exptl. studies support the observation of a more distinct reaction of soil soln. and foliar element concns. to changes in N supply compared to the three other parameters. According to the most likely scenarios, further decrease of N deposition will be limited. We hypothesize that this expected decline will not cause major responses of the parameters analyzed in this study. Instead, future changes might be more strongly controlled by the development of N pools accumulated within forest soils, affected by climate change and forest management.
11. 11

    Zhang, Y.; Li, Q.; Zhang, F.; Xie, G. Estimates of Economic Loss of Materials Caused by Acid Deposition in China. Sustainability 2017, 9 (488), 1– 14,  DOI: 10.3390/su9040488

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    Mills, G.; Sharps, K.; Simpson, D.; Davies, W. J.; Broberg, M.; Uddling, J.; Jaramillo, F.; Dentener, F.; Berg, M.; Van Den Agrawal, M.; Agrawal, S. B.; Ainsworth, E. A.; Patrick, B.; Emberson, L.; Feng, Z.; Harmens, H.; Hayes, F.; Dingenen, R. Van Ozone Pollution Will Compromise Efforts to Increase Global Wheat Production. Glob. Chang. Biol. 2018, 20 (4), 3560– 3574,  DOI: 10.1111/gcb.14157

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    Tan, J.; Fu, J. S.; Dentener, F.; Emmons, L. Multi-Model Study of HTAP II on Sulfur and Nitrogen Deposition. Atmos. Chem. Phys. 2018, 18, 6847– 6866,  DOI: 10.5194/acp-18-6847-2018

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    Multi-model study of HTAP II on sulfur and nitrogen deposition

    Tan, Jiani; Fu, Joshua S.; Dentener, Frank; Sun, Jian; Emmons, Louisa; Tilmes, Simone; Sudo, Kengo; Flemming, Johannes; Jonson, Jan Eiof; Gravel, Sylvie; Bian, Huisheng; Davila, Yanko; Henze, Daven K.; Lund, Marianne T.; Kucsera, Tom; Takemura, Toshihiko; Keating, Terry

    Atmospheric Chemistry and Physics (2018), 18 (9), 6847-6866CODEN: ACPTCE; ISSN:1680-7324. (Copernicus Publications)

    This study uses multi-model ensemble results of 11 models from the second phase of Task Force Hemispheric Transport of Air Pollution (HTAP II) to calc. the global sulfur (S) and nitrogen (N) deposition in 2010. The models underestimate SO42-, NO3- and NH4+ wet depositions in some European and East Asian stations but overestimate NO3- wet deposition in the eastern United States. The global S deposition is 84 Tg(S) in 2010, with 49% in continental regions and 51% in the ocean (19% of which coastal). The global N deposition consists of 59 Tg(N) oxidized nitrogen (NOy) deposition and 64 Tg(N) reduced nitrogen (NHx) deposition in 2010. The estd. outflow of pollution from land to ocean is about 4 Tg(S) for S deposition and 18 Tg(N) for N deposition. The global S deposition decreases 2 Tg(S) (3%) from 2001 to 2010, with significant decreases in Europe (5 Tg(S) and 55%), North America (3 Tg(S) and 29%) and Russia (2 Tg(S) and 26%), and increases in South Asia (2 Tg(S) and 42%) and the Middle East (1 Tg(S) and 44%). The global N deposition increases by 7 Tg(N) (6%), mainly contributed by South Asia (5 Tg(N) and 39%), East Asia (4 Tg(N) and 21%) and Southeast Asia (2 Tg(N) and 21%). The NHx deposition increases with no control policy on NH3 emission in North America. On the other hand, NOy deposition has started to dominate in East Asia (esp. China) due to boosted NOx emission.
14. 14

    Lamarque, J.-F.; Dentener, F.; Mcconnell, J.; Ro, C.; Shaw, M.; Vet, R.; Bergmann, D. Multi-Model Mean Nitrogen and Sulfur Deposition from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): Evaluation of Historical and Projected Future Changes. Atmos. Chem. Phys. 2013, 13, 7997– 8018,  DOI: 10.5194/acp-13-7997-2013

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    Multi-model mean nitrogen and sulfur deposition from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): evaluation of historical and projected future changes

    Lamarque, J.-F.; Dentener, F.; McConnell, J.; Ro, C.-U.; Shaw, M.; Vet, R.; Bergmann, D.; Cameron-Smith, P.; Dalsoren, S.; Doherty, R.; Faluvegi, G.; Ghan, S. J.; Josse, B.; Lee, Y. H.; MacKenzie, I. A.; Plummer, D.; Shindell, D. T.; Skeie, R. B.; Stevenson, D. S.; Strode, S.; Zeng, G.; Curran, M.; Dahl-Jensen, D.; Das, S.; Fritzsche, D.; Nolan, M.

    Atmospheric Chemistry and Physics (2013), 13 (16), 7997-8018, 22 pp.CODEN: ACPTCE; ISSN:1680-7324. (Copernicus Publications)

    We present multi-model global datasets of nitrogen and sulfate deposition covering time periods from 1850 to 2100, calcd. within the Atm. Chem. and Climate Model Intercomparison Project (ACCMIP). The computed deposition fluxes are compared to surface wet deposition and ice core measurements. We use a new dataset of wet deposition for 2000-2002 based on crit. assessment of the quality of existing regional network data. We show that for present day (year 2000 ACCMIP time slice), the ACCMIP results perform similarly to previously published multi-model assessments. For this time slice, we find a multimodel mean deposition of approx. 50 Tg(N) yr-1 from nitrogen oxide emissions, 60 Tg(N) yr-1 from ammonia emissions, and 83 Tg(S) yr-1 from sulfur emissions. The anal. of changes between 1980 and 2000 indicates significant differences between model and measurements over the United States but less so over Europe. This difference points towards a potential misrepresentation of 1980 NH3 emissions over North America. Based on ice core records, the 1850 deposition fluxes agree well with Greenland ice cores, but the change between 1850 and 2000 seems to be overestimated in the Northern Hemisphere for both nitrogen and sulfur species. Using the Representative Concn. Pathways (RCPs) to define the projected climate and atm. chem. related emissions and concns., we find large regional nitrogen deposition increases in 2100 in Latin America, Africa and parts of Asia under some of the scenarios considered. Increases in South Asia are esp. large, and are seen in all scenarios, with 2100 values more than double their 2000 counterpart in some scenarios and reaching >1300 mg(N)m-2 yr-1 averaged over regional to continental-scale regions in RCP 2.6 and 8.5, ∼30-50 % larger than the values in any region currently (circa 2000). However, sulfur deposition rates in 2100 are in all regions lower than in 2000 in all the RCPs. The new ACCMIP multimodel deposition dataset provides state-of-the-science, consistent and evaluated time slice (spanning 1850-2100) global gridded deposition fields for use in a wide range of climate and ecol. studies.
15. 15

    Vet, R.; Artz, R. S.; Carou, S.; Shaw, M.; Ro, C.; Aas, W.; Baker, A.; Bowersox, V. C.; Dentener, F.; Galy-Lacaux, C.; Hou, A.; Pienaar, J. J.; Gillett, R.; Forti, M. C.; Gromov, S.; Hara, H.; Khodzher, T.; Mahowald, N. M.; Nickovic, S.; Rao, P. S. P.; Reid, N. W. A Global Assessment of Precipitation Chemistry and Deposition of Sulfur, Nitrogen, Sea Salt, Base Cations, Organic Acids, Acidity and PH, and Phosphorus. Atmos. Environ. 2014, 93, 3– 100,  DOI: 10.1016/j.atmosenv.2013.10.060

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    A global assessment of precipitation chemistry and deposition of sulfur, nitrogen, sea salt, base cations, organic acids, acidity and pH, and phosphorus

    Vet, Robert; Artz, Richard S.; Carou, Silvina; Shaw, Mike; Ro, Chul-Un; Aas, Wenche; Baker, Alex; Bowersox, Van C.; Dentener, Frank; Galy-Lacaux, Corinne; Hou, Amy; Pienaar, Jacobus J.; Gillett, Robert; Forti, M. Cristina; Gromov, Sergey; Hara, Hiroshi; Khodzher, Tamara; Mahowald, Natalie M.; Nickovic, Slobodan; Rao, P. S. P.; Reid, Neville W.

    Atmospheric Environment (2014), 93 (), 3-100CODEN: AENVEQ; ISSN:1352-2310. (Elsevier Ltd.)

    A review. A global assessment of pptn. chem. and deposition has been carried out under the direction of the World Meteorol. Organization (WMO) Global Atm. Watch (GAW) Scientific Advisory Group for Pptn. Chem. (SAG-PC). The assessment addressed three questions: (1) what do measurements and model ests. of pptn. chem. and wet, dry and total deposition of sulfur, nitrogen, sea salt, base cations, org. acids, acidity, and phosphorus show globally and regionally (2) has the wet deposition of major ions changed since 2000 (and, where information and data are available, since 1990) and (3) what are the major gaps and uncertainties in our knowledge. To that end, regionally-representative measurements for two 3-yr-averaging periods, 2000-2002 and 2005-2007, were compiled worldwide. Data from the 2000-2002 averaging period were combined with 2001 ensemble-mean modeling results from 21 global chem. transport models produced in Phase 1 of the Coordinated Model Studies Activities of the Task Force on Hemispheric Transport of Air Pollution (TF HTAP). The measurement data and modeling results were used to generate global and regional maps of major ion concns. in pptn. and deposition. A major product of the assessment is a database of quality assured ion concn. and wet deposition data gathered from regional and national monitoring networks. The database is available for download from the World Data Center for Pptn. Chem. (http://wdcpc.org/). The assessment concludes that global concns. and deposition of sulfur and nitrogen are reasonably well characterized with levels generally highest near emission sources and more than an order of magnitude lower in areas largely free of anthropogenic influences. In many parts of the world, wet deposition of reduced nitrogen exceeds that of oxidized nitrogen and is increasing. Sulfur and nitrogen concns. and deposition in North America and Europe have declined significantly in line with emission redn. policies. Major regions of the world, including South America, the more remote areas of North America, much of Asia, Africa, Oceania, polar regions, and all of the oceans, are inadequately sampled for all of the major ions in wet and dry deposition, and particularly so for phosphorus, org. forms of nitrogen, and weak acids including carbonates and org. acids. Measurement-based inferential ests. of dry deposition are limited to sulfur and some nitrogen in only a few regions of the world and methods are highly uncertain. The assessment concludes with recommendations to address major gaps and uncertainties in global ion concn. and deposition measurements.
16. 16

    Dentener, F.; Drevet, J.; Lamarque, J. F.; Bey, I.; Eickhout, B.; Fiore, A. M.; Hauglustaine, D.; Horowitz, L. W.; Krol, M.; Kulshrestha, U. C.; Lawrence, M. Nitrogen and Sulfur Deposition on Regional and Global Scales: A Multimodel Evaluation. Global Biogeochem. Cycle 2006, 20 (4). n/a DOI: 10.1029/2005GB002672 .

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    Kanakidou, M.; Duce, R. A.; Prospero, J. M.; Baker, A. R.; Benitez-Nelson, C.; Dentener, F. J.; Hunter, K. A.; Liss, P. S.; Mahowald, N.; Okin, G. S.; Sarin, M.; Tsigaridis, K. Atmospheric Fluxes of Organic N and P to the Global Ocean. Global Biogeochem. Cycles 2012, 26, 1– 12,  DOI: 10.1029/2011GB004277

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    Kanakidou, M.; Myriokefalitakis, S.; Daskalakis, N.; Fanourgakis, G. Past, Present, and Future Atmospheric Nitrogen Deposition. J. Atmos. Sci. 2016, 73 (5), 2039– 2047,  DOI: 10.1175/JAS-D-15-0278.1

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    Past, Present and Future Atmospheric Nitrogen Deposition

    Kanakidou M; Myriokefalitakis S; Daskalakis N; Fanourgakis G; Mihalopoulos N; Nenes A; Baker A R; Tsigaridis K; Tsigaridis K; Mihalopoulos N

    Journal of the atmospheric sciences (2016), 73 (5), 2039-2047 ISSN:0022-4928.

    Reactive nitrogen emissions into the atmosphere are increasing due to human activities, affecting nitrogen deposition to the surface and impacting the productivity of terrestrial and marine ecosystems. An atmospheric chemistry-transport model (TM4-ECPL) is here used to calculate the global distribution of total nitrogen deposition, accounting for the first time for both its inorganic and organic fractions in gaseous and particulate phases, and past and projected changes due to anthropogenic activities. The anthropogenic and biomass burning ACCMIP historical and RCP6.0 and RCP8.5 emissions scenarios are used. Accounting for organic nitrogen (ON) primary emissions, the present-day global nitrogen atmospheric source is about 60% anthropogenic, while total N deposition increases by about 20% relative to simulations without ON primary emissions. About 20-25% of total deposited N is ON. About 10% of the emitted nitrogen oxides are deposited as ON instead of inorganic nitrogen (IN) as is considered in most global models. Almost a 3-fold increase over land (2-fold over the ocean) has been calculated for soluble N deposition due to human activities from 1850 to present. The investigated projections indicate significant changes in the regional distribution of N deposition and chemical composition, with reduced compounds gaining importance relative to oxidized ones, but very small changes in the global total flux. Sensitivity simulations quantify uncertainties due to the investigated model parameterizations of IN partitioning onto aerosols and of N chemically fixed on organics to be within 10% for the total soluble N deposition and between 25-35% for the dissolved ON deposition. Larger uncertainties are associated with N emissions.
19. 19

    Itahashi, S.; Ge, B.; Sato, K.; Fu, J. S.; Wang, X.; Yamaji, K. MICS-Asia III: Overview of Model Intercomparison and Evaluation of Acid Deposition over Asia. Atmos. Chem. Phys. 2020, 20, 2667– 2693,  DOI: 10.5194/acp-20-2667-2020

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    19

    MICS-Asia III: overview of model intercomparison and evaluation of acid deposition over Asia

    Itahashi, Syuichi; Ge, Baozhu; Sato, Keiichi; Fu, Joshua S.; Wang, Xuemei; Yamaji, Kazuyo; Nagashima, Tatsuya; Li, Jie; Kajino, Mizuo; Liao, Hong; Zhang, Meigen; Wang, Zhe; Li, Meng; Kurokawa, Junichi; Carmichael, Gregory R.; Wang, Zifa

    Atmospheric Chemistry and Physics (2020), 20 (5), 2667-2693CODEN: ACPTCE; ISSN:1680-7324. (Copernicus Publications)

    A review. The Model Inter-Comparison Study for Asia (MICS-Asia) phase III was conducted to promote understanding of regional air quality and climate change in Asia, which have received growing attention due to the huge amt. of anthropogenic emissions worldwide. This study provides an overview of acid deposition. Specifically, dry and wet deposition of the following species was analyzed: S (sulfate aerosol, sulfur dioxide (SO2), and sulfuric acid (H2SO4)), N (nitrate aerosol, nitrogen monoxide (NO), nitrogen dioxide (NO2), and nitric acid (HNO3)), and A (ammonium aerosol and ammonia (NH3)). The wet deposition simulated by a total of nine models was analyzed and evaluated using ground observation data from the Acid Deposition Monitoring Network in East Asia (EANET). In the phase III study, the no. of observation sites was increased from 37 in the phase II study to 54, and southeast Asian countries were newly added. Addnl., whereas the anal. period was limited to representative months of each season in MICS-Asia phase II, the phase III study analyzed the full year of 2010. The scope of this overview mainly focuses on the annual accumulated deposition. In general, models can capture the obsd. wet deposition over Asia but underestimate the wet deposition of S and A, and show large differences in the wet deposition of N. Furthermore, the ratio of wet deposition to the total deposition (the sum of dry and wet deposition) was investigated in order to understand the role of important processes in the total deposition. The general dominance of wet deposition over Asia and attributions from dry deposition over land were consistently found in all models. Then, total deposition maps over 13 countries participating in EANET were produced, and the balance between deposition and anthropogenic emissions was calcd. Excesses of deposition, rather than of anthropogenic emissions, were found over Japan, northern Asia, and southeast Asia, indicating the possibility of long-range transport within and outside of Asia, as well as other emission sources. To improve the ability of models to capture the obsd. wet deposition, two approaches were attempted, namely, ensemble and pptn. adjustment. The ensemble approach was effective at modulating the differences in performance among models, and the pptn.-adjusted approach demonstrated that the model performance for pptn. played a key role in better simulating wet deposition. Finally, the lessons learned from the phase III study and future perspectives for phase IV are summarized.
20. 20

    Knutti, R.; Sedlá̌, J. Robustness and Uncertainties in the New CMIP5 Climate Model Projections. Nat. Clim. Change 2013, 3 (October 2012), 369– 373,  DOI: 10.1038/nclimate1716

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    There is no corresponding record for this reference.
21. 21

    Lamarque, J.-F.; Shindell, D. T.; Josse, B.; Young, P. J.; Cionni, I.; Eyring, V.; Bergmann, D.; Cameron-Smith, P.; Collins, W. J.; Doherty, R.; Dalsoren, S.; Faluvegi, G.; Folberth, G.; Ghan, S. J.; Horowitz, L. W.; Lee, Y. H.; MacKenzie, I. A.; Nagashima, T.; Niak, V.; Plummer, D.; Righi, M.; Rumbold, S.; Schulz, M.; Skeie, R. R.; Stevenson, D. S.; Strode, S.; Sudo, K.; Szopa, S.; Voulgarakis, A.; Zeng, G. The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): Overview and Description of Models, Simulations and Climate Diagnostics. Geosci. Model Dev. 2013, 6, 179– 206,  DOI: 10.5194/gmd-6-179-2013

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    21

    The atmospheric chemistry and climate model intercomparison project (ACCMIP): overview and description of models, simulations and climate diagnostics

    Lamarque, J.-F.; Shindell, D. T.; Josse, B.; Young, P. J.; Cionni, I.; Eyring, V.; Bergmann, D.; Cameron-Smith, P.; Collins, W. J.; Doherty, R.; Dalsoren, S.; Faluvegi, G.; Folberth, G.; Ghan, S. J.; Horowitz, L. W.; Lee, Y. H.; MacKenzie, I. A.; Nagashima, T.; Naik, V.; Plummer, D.; Righi, M.; Rumbold, S. T.; Schulz, M.; Skeie, R. B.; Stevenson, D. S.; Strode, S.; Sudo, K.; Szopa, S.; Voulgarakis, A.; Zeng, G.

    Geoscientific Model Development (2013), 6 (1), 179-206, 28 pp.CODEN: GMDEA9; ISSN:1991-9603. (Copernicus Publications)

    The Atm. Chem. and Climate Model Intercomparison Project (ACCMIP) consists of a series of time slice expts. targeting the long-term changes in atm. compn. between 1850 and 2100, with the goal of documenting compn. changes and the assocd. radiative forcing. In this overview paper, we introduce the ACCMIP activity, the various simulations performed (with a requested set of 14) and the assocd. model output. The 16 ACCMIP models have a wide range of horizontal and vertical resolns., vertical extent, chem. schemes and interaction with radiation and clouds. While anthropogenic and biomass burning emissions were specified for all time slices in the ACCMIP protocol, it is found that the natural emissions are responsible for a significant range across models, mostly in the case of ozone precursors. The anal. of selected present-day climate diagnostics (pptn., temp., specific humidity and zonal wind) reveals biases consistent with state-of-the-art climate models. The model-to-model comparison of changes in temp., specific humidity and zonal wind between 1850 and 2000 and between 2000 and 2100 indicates mostly consistent results. However, models that are clear outliers are different enough from the other models to significantly affect their simulation of atm. chem.
22. 22

    Baker, A. R.; Kanakidou, M.; Altieri, K. E.; Daskalakis, N.; Okin, G. S.; Myriokefalitakis, S.; Dentener, F.; Uematsu, M.; Sarin, M. M.; Duce, R. A.; Galloway, J. N.; Keene, W. C.; Singh, A.; Zamora, L.; Lamarque, J. F.; Hsu, S. C.; Rohekar, S. S.; Prospero, J. M. Observation- and Model-Based Estimates of Particulate Dry Nitrogen Deposition to the Oceans. Atmos. Chem. Phys. 2017, 17 (13), 8189– 8210,  DOI: 10.5194/acp-17-8189-2017

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    22

    Observation- and model-based estimates of particulate dry nitrogen deposition to the oceans

    Baker, Alex R.; Kanakidou, Maria; Altieri, Katye E.; Daskalakis, Nikos; Okin, Gregory S.; Myriokefalitakis, Stelios; Dentener, Frank; Uematsu, Mitsuo; Sarin, Manmohan M.; Duce, Robert A.; Galloway, James N.; Keene, William C.; Singh, Arvind; Zamora, Lauren; Lamarque, Jean-Francois; Hsu, Shih-Chieh; Rohekar, Shital S.; Prospero, Joseph M.

    Atmospheric Chemistry and Physics (2017), 17 (13), 8189-8210CODEN: ACPTCE; ISSN:1680-7324. (Copernicus Publications)

    Anthropogenic nitrogen (N) emissions to the atm. have increased significantly the deposition of nitrate (NO-3) and ammonium (NH+4) 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, atm. chem., transport and deposition. In this work, ∼ 2900 observations of aerosol NO-3 and NH+4 concns., acquired from sampling aboard ships in the period 1995-2012, are used to assess the performance of modelled N concn. 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 d. 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 atm. N deposition on the ocean requires atm. chem. transport models to report deposition fluxes; however, these fluxes cannot be measured over the ocean. Modeling studies such as the Atm. Chem. 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 Tracer Model 4 of the Environmental Chem. Processes Lab. (TM4): ModDep for NOy, NHx and particulate NO-3 and NH+4, and surface-level particulate NO-3 and NH+4 concns. As a model ensemble, ACCMIP can be expected to be more robust than TM4, while TM4 gives access to speciated parameters (NO-3 and NH+4) that are more relevant to the obsd. parameters and which are not available in ACCMIP. Dry deposition fluxes (CalDep) were calcd. from the obsd. concns. using ests. of dry deposition velocities. Model-observation ratios (RA,n), weighted by grid-cell area and no. of observations, were used to assess the performance of the models. Comparison in the three study regions suggests that TM4 overestimates NO-3 concns. (RA,n = 1.4-2.9) and underestimates NH+4 concns. (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 NH+4 in the Indian Ocean, this discrepancy was probably due to seasonal biases in the sampling. Similar patterns were obsd. in the various comparisons of CalDep to ModDep (RA,n = 0.6-2.6 for NO-3, 0.6-3.1 for NH+4). Values of RA,n for NHx CalDep-ModDep comparisons were approx. double the corresponding values for NH+4 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 concns. These uncertainties have been a major limitation on ests. of the flux of material to the oceans for several decades. Recommendations are made for improvements in N deposition estn. through changes in observations, modeling and model-observation comparison procedures. Validation of modelled dry deposition requires effective comparisons to observable aerosol-phase species' concns., and this cannot be achieved if model products only report dry deposition flux over the ocean.
23. 23

    Vivanco, M. G.; Theobald, M. R.; García-Gómez, H.; Garrido, J. L.; Prank, M.; Aas, W.; Adani, M.; Alyuz, U.; Andersson, C.; Bellasio, R.; Bessagnet, B.; Bianconi, R.; Bieser, J.; Brandt, J.; Briganti, G.; Cappelletti, A.; Curci, G.; Christensen, J. H.; Collette, A.; Couvidat, F.; Cuvelier, C.; D’Isidoro, M.; Flemming, J.; Fraser, A.; Geels, C.; Hansen, K. M.; Hogrefe, C.; Im, U.; Jorba, O.; Kitwiroon, N.; Manders, A.; Mircea, M.; Otero, N.; Pay, M.-T.; Pozzoli, L.; Solazzo, E.; Tsyro, S.; Unal, A.; Wind, P.; Galmarini, S.; Pozzer, A. Modeled Deposition of Nitrogen and Sulfur in Europe Estimated by 14 Air Quality Model Systems: Evaluation, Effects of Changes in Emissions and Implications for Habitat Protection. Atmos. Chem. Phys. 2018, 18 (14), 10199– 10218,  DOI: 10.5194/acp-18-10199-2018

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    23

    Modeled deposition of nitrogen and sulfur in Europe estimated by 14 air quality model systems: evaluation, effects of changes in emissions and implications for habitat protection

    Vivanco, Marta G.; Theobald, Mark R.; Garcia-Gomez, Hector; Garrido, Juan Luis; Prank, Marje; Aas, Wenche; Adani, Mario; Alyuz, Ummugulsum; Andersson, Camilla; Bellasio, Roberto; Bessagnet, Bertrand; Bianconi, Roberto; Bieser, Johannes; Brandt, Joergen; Briganti, Gino; Cappelletti, Andrea; Curci, Gabriele; Christensen, Jesper H.; Colette, Augustin; Couvidat, Florian; Cuvelier, Cornelis; D'Isidoro, Massimo; Flemming, Johannes; Fraser, Andrea; Geels, Camilla; Hansen, Kaj M.; Hogrefe, Christian; Im, Ulas; Jorba, Oriol; Kitwiroon, Nutthida; Manders, Astrid; Mircea, Mihaela; Otero, Noelia; Pay, Maria-Teresa; Pozzoli, Luca; Solazzo, Efisio; Tsyro, Svetlana; Unal, Alper; Wind, Peter; Galmarini, Stefano

    Atmospheric Chemistry and Physics (2018), 18 (14), 10199-10218CODEN: ACPTCE; ISSN:1680-7324. (Copernicus Publications)

    This paper jointly examines the results from both project communities by intercomparing and evaluating the deposition ests. of reduced and oxidized nitrogen (N) and sulfur (S) in Europe simulated by 14 air quality model systems for the year 2010. An accurate est. of deposition is key to an accurate simulation of atm. concns. This study reveals a large variability between the wet deposition ests. of the models, with some performing acceptably (according to previously defined criteria) and others underestimating wet deposition rates. For dry deposition, there are also considerable differences between the model ests. An ensemble of the models with the best performance for N wet deposition was made and used to explore the implications of N deposition in the conservation of protected European habitats. Moreover, simulations with reduced emissions in selected source areas indicated a fairly linear relationship between redns. in emissions and changes in the deposition rates of N and S. European emissions are by far the main contributor to deposition in Europe, whereas the redn. in deposition due to a decrease in emissions in North America is very small and confined to the western part of the domain. Redns. in European emissions led to substantial decreases in the protected habitat areas with crit. load exceedances (halving the exceeded area for certain habitats), whereas no change was found, on av., when reducing North American emissions in terms of av. values per habitat.
24. 24

    Hoesly, R. M.; Smith, S. J.; Feng, L.; Klimont, Z.; Janssens-Maenhout, G.; Seibert, J. J.; Vu, L.; Andres, R. J.; Bolt, R. M.; Bond, T. C.; Dawidowski, L.; Kholod, N.; Kurokawa, J.; Li, M.; Liu, L.; Lu, Z.; Moura, M. C. P.; Patrick, R.; Rourke, O.; Zhang, Q. Historical (1750–2014) Anthropogenic Emissions of Reactive Gases and Aerosols from the Community Emission Data System (CEDS). Geosci. Model Dev. 2018, 11, 369– 408,  DOI: 10.5194/gmd-11-369-2018

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    24

    Historical (1750-2014) anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS)

    Hoesly, Rachel M.; Smith, Steven J.; Feng, Leyang; Klimont, Zbigniew; Janssens-Maenhout, Greet; Pitkanen, Tyler; Seibert, Jonathan J.; Vu, Linh; Andres, Robert J.; Bolt, Ryan M.; Bond, Tami C.; Dawidowski, Laura; Kholod, Nazar; Kurokawa, June-ichi; Li, Meng; Liu, Liang; Lu, Zifeng; Moura, Maria Cecilia P.; O'Rourke, Patrick R.; Zhang, Qiang

    Geoscientific Model Development (2018), 11 (1Spec.Iss.), 369-408CODEN: GMDEA9; ISSN:1991-9603. (Copernicus Publications)

    We present a new data set of annual historical (1750-2014) anthropogenic chem. reactive gases (CO, CH4, NH3, NOx, SO2, NMVOCs), carbonaceous aerosols (black carbon - BC, and org. carbon - OC), and CO2 developed with the Community Emissions Data System (CEDS). We improve upon existing inventories with a more consistent and reproducible methodol. applied to all emission species, updated emission factors, and recent ests. through 2014. The data system relies on existing energy consumption data sets and regional and country-specific inventories to produce trends over recent decades. All emission species are consistently estd. using the same activity data over all time periods. Emissions are provided on an annual basis at the level of country and sector and gridded with monthly seasonality. These ests. are comparable to, but generally slightly higher than, existing global inventories. Emissions over the most recent years are more uncertain, particularly in low- and middle-income regions where country-specific emission inventories are less available. Future work will involve refining and updating these emission ests., estg. emissions' uncertainty, and publication of the system as open-source software.
25. 25

    Khan, T. R.; Perlinger, J. A. Evaluation of Five Dry Particle Deposition Parameterizations for Incorporation into Atmospheric Transport Models. Geosci. Model Dev. 2017, 10, 3861– 3888,  DOI: 10.5194/gmd-10-3861-2017

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    25

    Evaluation of five dry particle deposition parameterizations for incorporation into atmospheric transport models

    Khan, Tanvir R.; Perlinger, Judith A.

    Geoscientific Model Development (2017), 10 (10), 3861-3888CODEN: GMDEA9; ISSN:1991-9603. (Copernicus Publications)

    Despite considerable effort to develop mechanistic dry particle deposition parameterizations for atm. transport models, current knowledge has been inadequate to propose quant. measures of the relative performance of available parameterizations. In this study, we evaluated the performance of five dry particle deposition parameterizations developed by Zhang et al. (2001) ("Z01"), Petroff and Zhang (2010) ("PZ10"), Kouznetsov and Sofiev (2012) ("KS12"), Zhang and He (2014) ("ZH14"), and Zhang and Shao (2014) ("ZS14"), resp. The evaluation was performed in three dimensions: model ability to reproduce obsd. deposition velocities, Vd (accuracy); the influence of imprecision in input parameter values on the modeled Vd (uncertainty); and identification of the most influential parameter(s) (sensitivity). The accuracy of the modeled Vd was evaluated using observations obtained from five land use categories (LUCs): grass, coniferous and deciduous forests, natural water, and ice/snow. To ascertain the uncertainty in modeled Vd, and quantify the influence of imprecision in key model input parameters, a Monte Carlo uncertainty anal. was performed. The Sobol' sensitivity anal. was conducted with the objective to det. the parameter ranking from the most to the least influential. Comparing the normalized mean bias factors (indicators of accuracy), we find that the ZH14 parameterization is the most accurate for all LUCs except for coniferous forest, for which it is second most accurate. From Monte Carlo simulations, the estd. mean normalized uncertainties in the modeled Vd obtained for seven particle sizes (ranging from 0.005 to 2.5 μm) for the five LUCs are 17, 12, 13, 16, and 27% for the Z01, PZ10, KS12, ZH14, and ZS14 parameterizations, resp. From the Sobol' sensitivity results, we suggest that the parameter rankings vary by particle size and LUC for a given parameteriza tion. Overall, for dp = 0.001 to 1.0 μm, friction velocity was one of the three most influential parameters in all parameterizations. For giant particles (dp = 10 μm), relative humidity was the most influential parameter. Because it is the least complex of the five parameterizations, and it has the greatest accuracy and least uncertainty, we propose that the ZH14 parameterization is currently superior for incorporation into atm. transport models.
26. 26

    Flechard, C. R.; Nemitz, E.; Smith, R. I.; Fowler, D.; Vermeulen, A. T.; Bleeker, A.; Erisman, J. W.; Simpson, D. Dry Deposition of Reactive Nitrogen to European Ecosystems: A Comparison of Inferential Models across the NitroEurope Network. Atmos. Chem. Phys. 2011, 11, 2703– 2728,  DOI: 10.5194/acp-11-2703-2011

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    26

    Dry deposition of reactive nitrogen to European ecosystems: a comparison of inferential models across the NitroEurope network

    Flechard, C. R.; Nemitz, E.; Smith, R. I.; Fowler, D.; Vermeulen, A. T.; Bleeker, A.; Erisman, J. W.; Simpson, D.; Zhang, L.; Tang, Y. S.; Sutton, M. A.

    Atmospheric Chemistry and Physics (2011), 11 (6), 2703-2728CODEN: ACPTCE; ISSN:1680-7316. (Copernicus Publications)

    Inferential models have long been used to det. pollutant dry deposition to ecosystems from measurements of air concns. and as part of national and regional atm. chem. and transport models, and yet models still suffer very large uncertainties. An inferential network of 55 sites throughout Europe for atm. reactive nitrogen (Nr) was established in 2007, providing ambient concns. of gaseous NH3, NO2, HNO3 and HONO and aerosol NH+4 and NO-3 as part of the NitroEurope Integrated Project. Network results providing modelled inorg. Nr dry deposition to the 55 monitoring sites are presented, using four existing dry deposition routines, revealing inter-model differences and providing ensemble av. deposition ests. Dry deposition is generally largest over forests in regions with large ambient NH3 concns., exceeding 30-40 kg N ha-1 yr-1 over parts of the Netherlands and Belgium, while some remote forests in Scandinavia receive less than 2 kg N ha-1 yr-1. Turbulent Nr deposition to short vegetation ecosystems is generally smaller than to forests due to reduced turbulent exchange, but also because NH3 inputs to fertilised, agricultural systems are limited by the presence of a substantial NH3 source in the vegetation, leading to periods of emission as well as deposition. Differences between models reach a factor 2-3 and are often greater than differences between monitoring sites. For sol. Nr gases such as NH3 and HNO3, the non-stomatal pathways are responsible for most of the annual uptake over many surfaces, esp. the non-agricultural land uses, but parameterisations of the sink strength vary considerably among models. For aerosol NH+4 and NO-3, discrepancies between theor. models and field flux measurements lead to much uncertainty in dry deposition rates for fine particles (0.1-0.5 μm). The validation of inferential models at the ecosystem scale is best achieved by comparison with direct long-term micrometerol. Nr flux measurements, but too few such datasets are available, esp. for HNO3 and aerosol NH+4 and NO-3.
27. 27

    Jickells, T.; Baker, A. R.; Cape, J. N.; Cornell, S. E.; Nemitz, E. The Cycling of Organic Nitrogen through the Atmosphere. Philos. Trans. R. Soc. Lond. B: Biol. Sci. 2013. 3681621 DOI: 10.1098/rstb.2013.0115

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    Lessmann, S.; Baesens, B.; Seow, H.; Thomas, L. C. Benchmarking State-of-the-Art Classification Algorithms for Credit Scoring: An Update of Research. Eur. J. Oper. Res. 2015, 247 (1), 124– 136,  DOI: 10.1016/j.ejor.2015.05.030

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29. 29

    Li, R.; Cui, L.; Zhao, Y.; Zhang, Z.; Sun, T.; Li, J.; Zhou, W.; Meng, Y.; Huang, K. Wet Deposition of Inorganic Ions in 320 Cities across China: Spatio-Temporal Variation, Source Apportionment, and Dominant Factors. Atmos. Chem. Phys. 2019, 19, 11043– 11070,  DOI: 10.5194/acp-19-11043-2019

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    29

    Wet deposition of inorganic ions in 320 cities across China: spatio-temporal variation, source apportionment, and dominant factors

    Li, Rui; Cui, Lulu; Zhao, Yilong; Zhang, Ziyu; Sun, Tianming; Li, Junlin; Zhou, Wenhui; Meng, Ya; Huang, Kan; Fu, Hongbo

    Atmospheric Chemistry and Physics (2019), 19 (17), 11043-11070CODEN: ACPTCE; ISSN:1680-7324. (Copernicus Publications)

    The acid deposition has been considered to be a severe environmental issue in China. The pH, elec. cond. (EC), and concns. of water sol. ions (NO-3, Cl-, Ca2+, K+, F-, NH+4, Mg2+, SO2-4, and Na+) in the pptn. samples collected from 320 cities during 2011-2016 across China were measured. The mean concns. of F-, NO-3, and SO2-4 were in the order of winter (6.10, 19.44, and 45.74μeq L-1) > spring (3.45, 13.83, and 42.61μeq L-1) > autumn (2.67, 9.73, and 28.85μeq L-1) > summer (2.04, 7.66, and 19.26μeq L-1). Secondary ions (SO2-4, NO-3, and NH+4 and F-)peaked in the Yangtze River Delta (YRD) and Sichuan basin (SB). Crustal ions (i.e. Ca2+, Mg2+), Na+, and Cl- showed the highest concns. in the semi-arid regions and the coastal cities. The statistical methods confirmed that the mean anthropogenic contribution ratios to SO2-4, F-, NO-3, and NH+4 at a national scale were 46.12%, 71.02%, 79.10%, and 82.40%, resp. However, Mg2+ (70.51%), K+ (77.44%), and Ca2+ (82.17%) mostly originated from the crustal source. Both Na+ (70.54%) and Cl- (60.42%) were closely linked to sea salt aerosols. On the basis of the stepwise regression (SR) anal., it was proposed that most of the secondary ions and F- were closely related to gross industrial prodn. (GIP), total energy consumption (TEC), vehicle ownership, and N fertilizer use, but the crustal ions (Ca2+ and K+) were mainly controlled by the dust events.
30. 30

    Schwede, D. B.; Lear, G. G. A Novel Hybrid Approach for Estimating Total Deposition in the United States. Atmos. Environ. 2014, 92, 207– 220,  DOI: 10.1016/j.atmosenv.2014.04.008

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    A novel hybrid approach for estimating total deposition in the United States

    Schwede, Donna B.; Lear, Gary G.

    Atmospheric Environment (2014), 92 (), 207-220CODEN: AENVEQ; ISSN:1352-2310. (Elsevier Ltd.)

    Atm. deposition of nitrogen and sulfur causes many deleterious effects on ecosystems including acidification and excess eutrophication. Assessments to support development of strategies to mitigate these effects require spatially and temporally continuous values of nitrogen and sulfur deposition. In the U. S., national monitoring networks exist that provide values of wet and dry deposition at discrete locations. While wet deposition can be interpolated between the monitoring locations, dry deposition cannot. Addnl., monitoring networks do not measure the complete suite of chems. that contribute to total sulfur and nitrogen deposition. Regional air quality models provide spatially continuous values of deposition of monitored species as well as important unmeasured species. However, air quality modeling values are not generally available for an extended continuous time period. Air quality modeling results may also be biased for some chem. species. We developed a novel approach for estg. dry deposition using data from monitoring networks such as the Clean Air Status and Trends Network (CASTNET), the National Atm. Deposition Program (NADP) Ammonia Monitoring Network (AMoN), and the Southeastern Aerosol Research and Characterization (SEARCH) network and modeled data from the Community Multiscale Air Quality (CMAQ) model. These dry deposition values ests. are then combined with wet deposition values from the NADP National Trends Network (NTN) to develop values of total deposition of sulfur and nitrogen. Data developed using this method are made available via the CASTNET website.
31. 31

    Schwede, D.; Cole, A.; Vet, R.; Lear, G.; Canada, O. U. S. On-Going U.S.-Canada Collaboration on Nitrogen and Sulfur Deposition on Nitrogen and Sulfur Deposition. Magazine for Environmental Managers , 2019.

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    Andersson, C.; Wylde, H. A.; Engardt, M. Long-Term Sulfur and Nitrogen Deposition in Sweden 1983–2013, 2018, No. 163.

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33. 33

    Schwede, D. B.; Simpson, D.; Tan, J.; Fu, J. S.; Dentener, F.; Du, E.; deVries, W. Spatial Variation of Modelled Total, Dry and Wet Nitrogen Deposition to Forests at Global Scale. Environ. Pollut. 2018, 243, 1287– 1301,  DOI: 10.1016/j.envpol.2018.09.084

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    Spatial variation of modelled total, dry and wet nitrogen deposition to forests at global scale

    Schwede, Donna B.; Simpson, David; Tan, Jiani; Fu, Joshua S.; Dentener, Frank; Du, Enzai; deVries, Wim

    Environmental Pollution (Oxford, United Kingdom) (2018), 243 (Part_B), 1287-1301CODEN: ENPOEK; ISSN:0269-7491. (Elsevier Ltd.)

    Forests are an important biome that covers about one third of the global land surface and provides important ecosystem services. Since atm. deposition of nitrogen (N) can have both beneficial and deleterious effects, it is important to quantify the amt. of N deposition to forest ecosystems. Measurements of N deposition to the numerous forest biomes across the globe are scarce, so chem. transport models are often used to provide ests. of atm. N inputs to these ecosystems. We provide an overview of approaches used to calc. N deposition in commonly used chem. transport models. The Task Force on Hemispheric Transport of Air Pollution (HTAP2) study intercompared N deposition values from a no. of global chem. transport models. Using a multi-model mean calcd. from the HTAP2 deposition values, we map N deposition to global forests to examine spatial variations in total, dry and wet deposition. Highest total N deposition occurs in eastern and southern China, Japan, Eastern U. S. and Europe while the highest dry deposition occurs in tropical forests. The European Monitoring and Evaluation Program (EMEP) model predicts grid-av. deposition, but also produces deposition by land use type allowing us to compare deposition specifically to forests with the grid-av. value. We found that, for this study, differences between the grid-av. and forest specific could be as much as a factor of two and up to more than a factor of five in extreme cases. This suggests that consideration should be given to using forest-specific deposition for input to ecosystem assessments such as crit. loads detns.
34. 34

    Robichaud, A.; Cole, A.; Moran, M.; Lupu, A.; Shaw, M.; Roy, G.; Beauchemin, M.; Fortin, V.; Vet, R. Total Deposition Maps Evaluated from Measurement-Model Fusion in North America (ADAGIO Project). Springer Proc. Complex. 2020, (June), 255– 259,  DOI: 10.1007/978-3-030-22055-6_40

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    National Atmospheric Deposition Program.TDep - Total Deposition Science Committee http://nadp.slh.wisc.edu/committees/tdep/ (accessed 2021/1/13).

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    World Meteorological Organization. Manual for the GAW Precipitation Chemistry Programme, 2018.

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    World Meteorological Organization. GAW Report No. 209 Guidelines for Continuous Measurements of Ozone in the Troposphere, 2013.

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    There is no corresponding record for this reference.
38. 38

    Aas, W.; Tsyro, S.; Bieber, E.; Bergstr, R. Lessons Learnt from the First EMEP Intensive Measurement Periods. Atmos. Chem. Phys. 2012, 12, 8073– 8094,  DOI: 10.5194/acp-12-8073-2012

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    38

    Lessons learnt from the first EMEP intensive measurement periods

    Aas, W.; Tsyro, S.; Bieber, E.; Bergstrom, R.; Ceburnis, D.; Ellermann, T.; Fagerli, H.; Frolich, M.; Gehrig, R.; Makkonen, U.; Nemitz, E.; Otjes, R.; Perez, N.; Perrino, C.; Prevot, A. S. H.; Putaud, J.-P.; Simpson, D.; Spindler, G.; Vana, M.; Yttri, K. E.

    Atmospheric Chemistry and Physics (2012), 12 (17), 8073-8094CODEN: ACPTCE; ISSN:1680-7316. (Copernicus Publications)

    The first EMEP intensive measurement periods were held in June 2006 and Jan. 2007. The measurements aimed to characterize the aerosol chem. compns., including the gas/aerosol partitioning of inorg. compds. The measurement program during these periods included daily or hourly measurements of the secondary inorg. components, with addnl. measurements of elemental- and org. carbon (EC and OC) and mineral dust in PM1, PM2.5 and PM10. These measurements have provided extended knowledge regarding the compn. of particulate matter and the temporal and spatial variability of PM, as well as an extended database for the assessment of chem. transport models. This paper summarizes the first experiences of making use of measurements from the first EMEP intensive measurement periods along with EMEP model results from the updated model version to characterize aerosol compn. We investigated how the PM chem. compn. varies between the summer and the winter month and geog. The observation and model data are in general agreement regarding the main features of PM10 and PM2.5 compn. and the relative contribution of different components, though the EMEP model tends to give slightly lower ests. of PM10 and PM2.5 compared to measurements. The intensive measurement data has identified areas where improvements are needed. Hourly concurrent measurements of gaseous and particulate components for the first time facilitated testing of modeled diurnal variability of the gas/aerosol partitioning of nitrogen species. In general, the modeled diurnal cycles of nitrate and ammonium aerosols are in fair agreement with the measurements, but the diurnal variability of ammonia is not well captured. The largest differences between model and observations of aerosol mass are seen in Italy during winter, which to a large extent may be explained by an underestimation of residential wood burning sources. It should be noted that both primary and secondary OC has been included in the calcns. for the first time, showing promising results. Mineral dust is important, esp. in southern Europe, and the model seems to capture the dust episodes well. The lack of measurements of mineral dust hampers the possibility for model evaluation for this highly uncertain PM component. There are also lessons learnt regarding improved measurements for future intensive periods. There is a need for increased comparability between the measurements at different sites. For the nitrogen compds. it is clear that more measurements using artifact free methods based on continuous measurement methods and/or denuders are needed. For EC/OC, a ref. methodol. (both in field and lab.) was lacking during these periods giving problems with comparability, though measurement protocols have recently been established and these should be followed by the Parties to the EMEP Protocol. For measurements with no defined protocols, it might be a good soln. to use centralized labs. to ensure comparability across the network. To cope with the introduction of these new measurements, new reporting guidelines have been developed to ensure that all proper information about the methodologies and data quality is given.
39. 39

    Yu, X.; Lee, T.; Ayres, B.; Kreidenweis, S. M.; Malm, W.; Collett, J. L. Loss of Fine Particle Ammonium from Denuded Nylon Filters. Atmos. Environ. 2006, 40, 4797– 4807,  DOI: 10.1016/j.atmosenv.2006.03.061

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    39

    Loss of fine particle ammonium from denuded nylon filters

    Yu, Xiao-Ying; Lee, Taehyoung; Ayres, Benjamin; Kreidenweis, Sonia M.; Malm, William; Collett, Jeffrey L.

    Atmospheric Environment (2006), 40 (25), 4797-4807CODEN: AENVEQ; ISSN:1352-2310. (Elsevier Ltd.)

    Ammonium is an important constituent of fine particulate mass in the atm., but can be difficult to quantify due to possible sampling artifacts. Losses of semivolatile species such as NH4NO3 can be particularly problematic. To evaluate ammonium losses from aerosol particles collected on filters, field expts. were conducted using denuded nylon and Teflon filters at Bondville, IL (Feb. 2003), San Gorgonio, CA (Apr. 2003 and July 2004), Grand Canyon NP, AZ (May, 2003), Brigantine, NJ (Nov. 2003), and Great Smoky Mountains National Park (NP), TN (July-August 2004). Samples were collected over 24 h periods. Losses from denuded nylon filters ranged from 10% (monthly av.) in Bondville, IL to 28% in San Gorgonio, CA in summer. Losses on individual sample days ranged from 1% to 65%. Losses tended to increase with increasing diurnal temp. and relative humidity changes and with the fraction of ambient total N(-III) (particulate NH4 + + gaseous NH3) present as gaseous NH3. The amt. of ammonium lost at most sites could be explained by the amt. of NH4NO3 present in the sampled aerosol. Ammonium losses at Great Smoky Mountains NP, however, significantly exceeded the amt. of NH4NO3 collected. Ammoniated org. salts are suggested as addnl. important contributors to obsd. ammonium loss at this location.
40. 40

    Holland, E. A.; Braswell, B. H.; Sulzman, J.; Lamarque, J.-F. Nitrogen Deposition onto the United States and Western Europe: Synthesis of Observations and Models. Ecol. Appl. 2014, 15 (1), 38– 57,  DOI: 10.1890/03-5162

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41. 41

    Emerson, E. W.; Katich, J. M.; Farmer, D. K. Direct Measurements of Dry and Wet Deposition of Black Carbon Over a Grassland. J. Geophys. Res.: Atmos. 2018, 123, 277– 290,  DOI: 10.1029/2018JD028954

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42. 42

    Baker, A. R.; Myriokefalitakis, S.; Altieri, K. E.; Daskalakis, N.; Okin, G. S.; Myriokefalitakis, S.; Dentener, F.; Uematsu, M.; Sarin, M. M.; Duce, R. A.; Galloway, J. N.; Keene, W. C.; Singh, A.; Zamora, L.; Lamarque, J.-F.; Hsu, S.-C.; Rohekar, S. S.; Prospero, J. M. Observation- and Model-Based Estimates of Particulate Dry Nitrogen Deposition to the Oceans. Atmos. Chem. Phys. 2017, 17 (13), 8189– 8210,  DOI: 10.5194/acp-17-8189-2017

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    42

    Observation- and model-based estimates of particulate dry nitrogen deposition to the oceans

    Baker, Alex R.; Kanakidou, Maria; Altieri, Katye E.; Daskalakis, Nikos; Okin, Gregory S.; Myriokefalitakis, Stelios; Dentener, Frank; Uematsu, Mitsuo; Sarin, Manmohan M.; Duce, Robert A.; Galloway, James N.; Keene, William C.; Singh, Arvind; Zamora, Lauren; Lamarque, Jean-Francois; Hsu, Shih-Chieh; Rohekar, Shital S.; Prospero, Joseph M.

    Atmospheric Chemistry and Physics (2017), 17 (13), 8189-8210CODEN: ACPTCE; ISSN:1680-7324. (Copernicus Publications)

    Anthropogenic nitrogen (N) emissions to the atm. have increased significantly the deposition of nitrate (NO-3) and ammonium (NH+4) 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, atm. chem., transport and deposition. In this work, ∼ 2900 observations of aerosol NO-3 and NH+4 concns., acquired from sampling aboard ships in the period 1995-2012, are used to assess the performance of modelled N concn. 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 d. 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 atm. N deposition on the ocean requires atm. chem. transport models to report deposition fluxes; however, these fluxes cannot be measured over the ocean. Modeling studies such as the Atm. Chem. 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 Tracer Model 4 of the Environmental Chem. Processes Lab. (TM4): ModDep for NOy, NHx and particulate NO-3 and NH+4, and surface-level particulate NO-3 and NH+4 concns. As a model ensemble, ACCMIP can be expected to be more robust than TM4, while TM4 gives access to speciated parameters (NO-3 and NH+4) that are more relevant to the obsd. parameters and which are not available in ACCMIP. Dry deposition fluxes (CalDep) were calcd. from the obsd. concns. using ests. of dry deposition velocities. Model-observation ratios (RA,n), weighted by grid-cell area and no. of observations, were used to assess the performance of the models. Comparison in the three study regions suggests that TM4 overestimates NO-3 concns. (RA,n = 1.4-2.9) and underestimates NH+4 concns. (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 NH+4 in the Indian Ocean, this discrepancy was probably due to seasonal biases in the sampling. Similar patterns were obsd. in the various comparisons of CalDep to ModDep (RA,n = 0.6-2.6 for NO-3, 0.6-3.1 for NH+4). Values of RA,n for NHx CalDep-ModDep comparisons were approx. double the corresponding values for NH+4 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 concns. These uncertainties have been a major limitation on ests. of the flux of material to the oceans for several decades. Recommendations are made for improvements in N deposition estn. through changes in observations, modeling and model-observation comparison procedures. Validation of modelled dry deposition requires effective comparisons to observable aerosol-phase species' concns., and this cannot be achieved if model products only report dry deposition flux over the ocean.
43. 43

    Roy, D. P.; Wulder, M. A.; Loveland, T. R.; Woodcock, C. E.; Allen, R. G.; Anderson, M. C.; Helder, D.; Irons, J. R.; Johnson, D. M.; Kennedy, R.; Scambos, T. A.; Schaaf, C. B.; Schott, J. R.; Sheng, Y.; Vermote, E. F.; Belward, A. S.; Bindschadler, R.; Cohen, W. B.; Gao, F.; Hipple, J. D.; Hostert, P.; Huntington, J.; Justice, C. O.; Kilic, A.; Kovalskyy, V.; Lee, Z. P.; Lymburner, L.; Masek, J. G.; Mccorkel, J.; Shuai, Y.; Trezza, R.; Vogelmann, J.; Wynne, R. H.; Zhu, Z. Remote Sensing of Environment Landsat-8: Science and Product Vision for Terrestrial Global Change Research. Remote Sens. Environ. 2014, 145, 154– 172,  DOI: 10.1016/j.rse.2014.02.001

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44. 44

    Schneider, U.; Ziese, M.; Meyer-Christoffer, A.; Finger, P.; Rustemeier, E. The New Portfolio of Global Precipitation Data Products of the Global Precipitation Climatology Centre Suitable to Assess and Quantify the Global Water Cycle and Resources. Proc. IAHS 2016, 374, 29– 34,  DOI: 10.5194/piahs-374-29-2016

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45. 45

    Lorente, A.; Boersma, K. F.; Eskes, H. J.; Veefkind, J. P.; vanGeffen, J. H. G. M.; deZeeuw, M. B.; van derGon, H. A. C. D.; Beirle, S.; Krol, M. C. Quantification of Nitrogen Oxides Emissions from Build-up of Pollution over Paris with TROPOMI. Sci. Rep. 2019, 9 (20033), 1– 10,  DOI: 10.1038/s41598-019-56428-5

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    45

    Analysis of thermochemical energy storage in an elemental configuration

    Malley-Ernewein, Alexandre; Lorente, Sylvie

    Scientific Reports (2019), 9 (1), 1-9CODEN: SRCEC3; ISSN:2045-2322. (Nature Research)

    Here we show theor. that the design of a thermochem. energy storage system for fast response and high thermal power can be predicted in accord with the constructal law of design. In this fundamental configuration, the walls of the elemental cylinder are impregnated with salt, while humid air is blown through the tube. Cases with const. salt vol. or const. fluid vol. or both are considered. It is shown that the best design in each case meets the equipartition of imperfections principle. The predictions are confirmed by full numerical expts., allowing to consider various shape ratios and study their impact on the overall performance.
46. 46

    Shephard, M. W.; Dammers, E.; Cady-Pereira, K. E.; Kharol, S. K.; Thompson, J.; Gainariu-Matz, Y.; Zhang, J.; Mclinden, C. A.; Kovachik, A.; Moran, M. Ammonia Measurements from Space with the Cross-Track Infrared Sounder: Characteristics and Applications. Atmos. Chem. Phys. 2020, 20, 2277– 2302,  DOI: 10.5194/acp-20-2277-2020

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    46

    Ammonia measurements from space with the cross-track infrared sounder: characteristics and applications

    Shephard, Mark W.; Dammers, Enrico; Cady-Pereira, Karen E.; Kharol, Shailesh K.; Thompson, Jesse; Gainariu-Matz, Yonatan; Zhang, Junhua; McLinden, Chris A.; Kovachik, Andrew; Moran, Michael; Bittman, Shabtai; Sioris, Christopher E.; Griffin, Debora; Alvarado, Matthew J.; Lonsdale, Chantelle; Savic-Jovcic, Verica; Zheng, Qiong

    Atmospheric Chemistry and Physics (2020), 20 (4), 2277-2302CODEN: ACPTCE; ISSN:1680-7324. (Copernicus Publications)

    Despite its clear importance, the monitoring of atm. 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 IR Sounder (CrIS) ammonia product for monitoring, air quality forecast model evaluation, dry deposition ests., and emission ests. 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 concns. approaching those in agricultural hotspots. The CrIS annual ammonia dry depositions in Canada (excluding the territories) and the US have av. and annual variability values of ∼0.8±0.08 and ∼1.23±0.09Tg N yr-1, resp. 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, resp. Furthermore, we show the use of CrIS satellite observations to est. annual and seasonal emissions near Lethbridge, Alberta, Canada, a region dominated by high-emission concd. animal feeding operations (CAFOs); the satellite annual emission est. of 37.1±6.3 kt yr-1 is at least double the value reported in current bottom-up emission inventories for this region.
47. 47

    Lamsal, L. N.; Martin, R. V.; vanDonkelaar, A.; Steinbacher, M.; Celarier, E. A.; Bucsela, E.; Dunlea, E. J.; Pinto, J. P. Ground-Level Nitrogen Dioxide Concentrations Inferred from the Satellite-Borne Ozone Monitoring Instrument. J. Geophys. Res. 2008, 113 (16), 1– 15,  DOI: 10.1029/2007JD009235

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48. 48

    Nowlan, C. R.; Martin, R. V.; Philip, S.; Lamsal, L. N.; Krotkov, N. A.; Marais, E. A.; Wang, S.; Zhang, Q. Global Dry Deposition of Nitrogen Dioxide and Sulfur Dioxide Inferred from Space-Based Measurements. Global Biogeochem. Cycles 2014, 28 (10), 1025– 1043,  DOI: 10.1002/2014GB004805

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    48

    Global dry deposition of nitrogen dioxide and sulfur dioxide inferred from space-based measurements

    Nowlan, C. R.; Martin, R. V.; Philip, S.; Lamsal, L. N.; Krotkov, N. A.; Marais, E. A.; Wang, S.; Zhang, Q.

    Global Biogeochemical Cycles (2014), 28 (10), 1025-1043CODEN: GBCYEP; ISSN:1944-9224. (Wiley-Blackwell)

    A method is developed to est. global NO2 and SO2 dry deposition fluxes at high spatial resoln. (0.1°×0.1°) using satellite measurements from the Ozone Monitoring Instrument (OMI) on the Aura satellite, in combination with simulations from the Goddard Earth Observing System chem. transport model (GEOS-Chem). These global maps for 2005-2007 provide a data set for use in examg. global and regional budgets of deposition. In order to properly assess SO2 on a global scale, a method is developed to account for the geospatial character of background offsets in retrieved satellite columns. Globally, annual dry deposition to land estd. from OMI as NO2 contributes 1.5 ± 0.5 Tg of nitrogen and as SO2 contributes 13.7 ± 4.0 Tg of sulfur. Differences between OMI-inferred NO2 dry deposition fluxes and those of other models and observations vary from excellent agreement to an order of magnitude difference, with OMI typically on the low end of ests. SO2 dry deposition fluxes compare well with in situ Clear Air Status and Trends Network-inferred flux over North America (slope = 0.98, r = 0.71). The most significant NO2 dry deposition flux to land per area occurs in the Pearl River Delta, China, at 13.9 kg N ha-1 yr-1, while SO2 dry deposition has a global max. rate of 72.0 kg S ha-1 yr-1 to the east of Jinan in China's Shandong province. Dry deposition fluxes are explored in several urban areas, where NO2 contributes on av. 9-36% and as much as 85% of total NOy dry deposition.
49. 49

    Kharol, S. K.; Shephard, M. W.; McLinden, C. A.; Zhang, L.; Sioris, C. E.; O’Brien, J. M.; Vet, R.; Cady-Pereira, K. E.; Hare, E.; Siemons, J.; Krotkov, N. A. Dry Deposition of Reactive Nitrogen From Satellite Observations of Ammonia and Nitrogen Dioxide Over North America. Geophys. Res. Lett. 2018, 45 (2), 1157– 1166,  DOI: 10.1002/2017GL075832

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    49

    Dry Deposition of Reactive Nitrogen From Satellite Observations of Ammonia and Nitrogen Dioxide Over North America

    Kharol, S. K.; Shephard, M. W.; McLinden, C. A.; Zhang, L.; Sioris, C. E.; O'Brien, J. M.; Vet, R.; Cady-Pereira, K. E.; Hare, E.; Siemons, J.; Krotkov, N. A.

    Geophysical Research Letters (2018), 45 (2), 1157-1166CODEN: GPRLAJ; ISSN:1944-8007. (Wiley-Blackwell)

    Reactive nitrogen (Nr) is an essential nutrient to plants and a limiting element for growth in many ecosystems, but it can have harmful effects on ecosystems when in excess. Satellite-derived surface observations are used together with a dry deposition model to est. the dry deposition flux of the most abundant short-lived nitrogen species, NH3 and NO2, over North America during the 2013 warm season. These fluxes demonstrate that the NH3 contribution dominates over NO2 for most regions (comprising ~ 85% of their sum in Canada and ~ 65% in the U.S.), with some regional exceptions (e.g. Alberta and northeastern U.S.). Nationwide, ~ 51 t of N from these species were dry deposited in the U.S., approx. double the ~ 28 t in Canada over this period. Forest fires are shown to be the major contributor of dry deposition of Nr from NH3 in northern latitudes, leading to deposition fluxes 2-3 times greater than from expected amts. without fires.
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    Geddes, J. A.; Martin, R. V.; Boys, B. L.; vanDonkelaar, A. Long-Term Trends Worldwide in Ambient NO2 Concentrations Inferred from Satellite Observations. Environ. Health Perspect. 2016, 124 (3), 281– 289,  DOI: 10.1289/ehp.1409567

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    50

    Long-term trends worldwide in ambient NO2 concentrations inferred from satellite observations

    Geddes, Jeffrey A.; Martin, Randall V.; Boys, Brian L.; van Donkelaar, Aaron

    Environmental Health Perspectives (2016), 124 (3), 281-289CODEN: EVHPAZ; ISSN:1552-9924. (U. S. Department of Health and Human Services, National Institutes of Health)

    Background: Air pollution is assocd. with morbidity and premature mortality. Satellite remote sensing provides globally consistent decadal-scale observations of ambient nitrogen dioxide (NO2) pollution. Objective: We detd. global population-weighted annual mean NO2 concns. from 1996 through 2012. Methods: We used observations of NO2 tropospheric column densities from three satellite instruments in combination with chem. transport modeling to produce a global 17-yr record of ground-level NO2 at 0.1 ° × 0.1 ° resoln. We calcd. linear trends in population-weighted annual mean NO2 (PWMNO2) concns. in different regions around the world. Results: We found that PWMNO2 in high-income North America (Canada and the United States) decreased more steeply than in any other region, having declined at a rate of -4.7%/yr [95% confidence interval (CI): -5.3, -4.1]. PWMNO2 decreased in western Europe at a rate of -2.5%/yr (95% CI: -3.0, -2.1). The highest PWMNO2 occurred in high-income Asia Pacific (predominantly Japan and South Korea) in 1996, with a subsequent decrease of -2.1%/yr (95% CI: -2.7, -1.5). In contrast, PWMNO2 almost tripled in East Asia (China, North Korea, and Taiwan) at a rate of 6.7%/yr (95% CI: 6.0, 7.3). The satellite-derived ests. of trends in ground-level NO2 were consistent with regional trends inferred from data obtained from ground-station monitoring networks in North America (within 0.7%/yr) and Europe (within 0.3%/yr). Our rankings of regional av. NO2 and long-term trends differed from the satellite-derived ests. of fine particulate matter reported elsewhere, demonstrating the utility of both indicators to describe changing pollutant mixts. Conclusions: Long-term trends in satellite-derived ambient NO2 provide new information about changing global exposure to ambient air pollution.
51. 51

    Liu, L.; Zhang, X.; Wong, A. Y. H.; Xu, W.; Liu, X.; Li, Y.; Mi, H.; Lu, X.; Zhao, L.; Wang, Z.; Wu, X. Estimating Global Surface Ammonia Concentrations Inferred from Satellite Retrievals. Atmos. Chem. Phys. 2019, 19, 12051– 12–66,  DOI: 10.5194/acp-19-12051-2019

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    51

    Estimating global surface ammonia concentrations inferred from satellite retrievals

    Liu, Lei; Zhang, Xiuying; Wong, Anthony Y. H.; Xu, Wen; Liu, Xuejun; Li, Yi; Mi, Huan; Lu, Xuehe; Zhao, Limin; Wang, Zhen; Wu, Xiaodi; Wei, Jing

    Atmospheric Chemistry and Physics (2019), 19 (18), 12051-12066CODEN: ACPTCE; ISSN:1680-7324. (Copernicus Publications)

    Ammonia (NH3), as an alk. gas in the atm., can cause direct or indirect effects on the air quality, soil acidification, climate change and human health. Estg. surface NH3 concns. is critically important for modeling the dry deposition of NH3 and for modeling the formation of ammonium nitrate, which have important impacts on the natural environment. However, sparse monitoring sites make it challenging and difficult to understand the global distribution of surface NH3 concns. in both time and space. We estd. the global surface NH3 concns. for the years of 2008-2016 using satellite NH3 retrievals combining vertical profiles from GEOS-Chem. The accuracy assessment indicates that the satellite-based approach has achieved a high predictive power for annual surface NH3 concns. compared with the measurements of all sites in China, the US and Europe (R2 = 0:76 and RMSED1.50 μgNm-3). The satellite-derived surface NH3 concns. had higher consistency with the ground-based measurements in China (R2 = 0:71 and RMSED2.6 μgNm-3) than the US (R2 = 0:45 and RMSED0.76 μgNm-3) and Europe (R2 = 0:45 and RMSED0.86 μgNm-3) at a yearly scale. Annual surface NH3 concns. higher than 6 μgNm-3 are mainly concd. in the North China Plain of China and northern India, followed by 2-6 μgNm-3 mainly in southern and northeastern China, India, western Europe, and the eastern United States (US). High surface NH3 concns. were found in the croplands in China, the US and Europe, and surface NH3 concns. in the croplands in China were approx. double those in the croplands in the US and Europe. The linear trend anal. shows that an increase rate of surface NH3 concns. (> 0.2 μgNm-3 yr-1) appeared in eastern China during 2008-2016, and a middle increase rate (0.1-0.2 μgNm-3 yr-1) occurred in northern Xinjiang over China. NH3 increase was also found in agricultural regions in the central and eastern US with an annual increase rate of lower than 0.10 μgNm-3 yr-1. The satellite-derived surface NH3 concns. help us to det. the NH3 pollution status in the areas without monitoring sites and to est. the dry deposition of NH3 in the future.
52. 52

    Liu, L.; Zhang, X.; Xu, W.; Liu, X.; Wei, J.; Wang, Z.; Yang, Y. Global Estimates of Dry Ammonia Deposition Inferred from Space-Measurements. Sci. Total Environ. 2020, 730, 139189,  DOI: 10.1016/j.scitotenv.2020.139189

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    52

    Global estimates of dry ammonia deposition inferred from space-measurements

    Liu, Lei; Zhang, Xiuying; Xu, Wen; Liu, Xuejun; Wei, Jing; Wang, Zhen; Yang, Yuyu

    Science of the Total Environment (2020), 730 (), 139189CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)

    NH3, an alk. gas, substantially contributes to atm. N deposition, which can cause biodiversity loss, eutrophication, and soil acidification. Advances in using satellite observations allow us to gain deeper insights into atm. NH3 concns. at large spatial scales. A new satellite-based method was proposed to est. dry NH3 deposition considering bi-directional NH3 exchange. The authors estd. global dry NH3 deposition for nine years (2008-2016) using the IR atm. sounding interferometer instrument to retrieve NH3 data. Satellite-based dry NH3 deposition was generally consistent with measured dry NH3 deposition over monitoring sites (R2 = 0.65). Global dry NH3 deposition >8 kg N/ha was mainly distributed in eastern China, northern and central Pakistan, and northern India. An annual increased rate of 0.27 and 0.13 kg N/ha-yr in dry NH3 deposition in 2008-2016 occurred in eastern China and the Sichuan Basin, major Chinese agricultural regions. The NH3 compensation point was high in warm months, >1μg/m3 as in eastern China, implying the importance of considering NH3 compensation points to est. dry NH3 deposition. If the increasing NH3 flux was ignored, it resulted in 11, 17, 5, and 3% over-estn. of dry NH3 deposition in eastern China, northern India, eastern USA, and western Europe, resp. This work discusses the potential of using satellite retrievals to est. large-scale dry NH3 deposition. The method can provide temporally continuous, spatially complete fine-resoln. datasets.
53. 53

    van derGraaf, S. C.; Dammers, E.; Schaap, M.; Willem Erisman, J. Technical Note: How Are NH3 Dry Deposition Estimates Affected by Combining the LOTOS-EUROS Model with IASI-NH3 Satellite Observations?. Atmos. Chem. Phys. 2018, 18 (17), 13173– 13196,  DOI: 10.5194/acp-18-13173-2018

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54. 54

    Cheng, M.; Jiang, H.; Guo, Z.; Zhang, X.; Lu, X. Estimating NO2 Dry Deposition Using Satellite Data in Eastern China. Int. J. Remote Sens. 2013, 34 (7), 2548– 2565,  DOI: 10.1080/01431161.2012.747019

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55. 55

    Liu, L.; Yang, Y.; Xi, R.; Zhang, X.; Xu, W.; Liu, X.; Li, Y.; Liu, P.; Wang, Z.. Global Wet Reduced Nitrogen Deposition Derived from Combining Satellite Measurements with Output from a Chemistry Transport Model. J. Geophys. Res.: Atmos. 2021, December.  DOI: 10.1029/2020JD033977 .

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56. 56

    Liu, L.; Zhang, X.; Xu, W.; Liu, X.; Lu, X.; Chen, D.; Zhang, X.; Wang, S.; Zhang, W. Estimation of Monthly Bulk Nitrate Deposition in China Based on Satellite NO2Measurement by the Ozone Monitoring Instrument. Remote Sens. Environ. 2017, 199, 93– 106,  DOI: 10.1016/j.rse.2017.07.005

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    Jia, Y.; Yu, G.; Gao, Y.; He, N.; Wang, Q.; Jiao, C.; Zuo, Y. Global Inorganic Nitrogen Dry Deposition Inferred from Ground- and Space-Based Measurements. Sci. Rep. 2016, 6, 1– 11,  DOI: 10.1038/srep19810

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    There is no corresponding record for this reference.
58. 58

    Miyazaki, K.; Eskes, H. J.; Sudo, K. A Tropospheric Chemistry Reanalysis for the Years 2005–2012 Based on an Assimilation of OMI, MLS, TES and MOPITT Satellite Data. Atmos. Chem. Phys. 2015, 15, 8315– 8348,  DOI: 10.5194/acp-15-8315-2015

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    58

    A tropospheric chemistry reanalysis for the years 2005-2012 based on an assimilation of OMI, MLS, TES, and MOPITT satellite data

    Miyazaki, K.; Eskes, H. J.; Sudo, K.

    Atmospheric Chemistry and Physics (2015), 15 (14), 8315-8348CODEN: ACPTCE; ISSN:1680-7324. (Copernicus Publications)

    We present the results from an 8-yr tropospheric chem. reanal. for the period 2005-2012 obtained by assimilating multiple data sets from the OMI, MLS, TES, and MOPITT satellite instruments. The reanal. calcn. was conducted using a global chem. transport model and an ensemble Kalman filter technique that simultaneously optimizes the chem. concns. of various species and emissions of several precursors. The optimization of both the concn. and the emission fields is an efficient method to correct the entire tropospheric profile and its year-to-year variations, and to adjust various tracers chem. linked to the species assimilated. Comparisons against independent aircraft, satellite, and ozonesonde observations demonstrate the quality of the analyzed O3, NO2, and CO concns. on regional and global scales and for both seasonal and year-to-year variations from the lower troposphere to the lower stratosphere. The data assimilation statistics imply persistent redn. of model error and improved representation of emission variability, but they also show that discontinuities in the availability of the measurements lead to a degrdn. of the reanal. The decrease in the no. of assimilated measurements increased the ozonesonde-minus-anal. difference after 2010 and caused spurious variations in the estd. emissions. The Northern/Southern Hemisphere OH ratio was modified considerably due to the multiple-species assimilation and became closer to an observational est., which played an important role in propagating observational information among various chem. fields and affected the emission ests. The consistent concn. and emission products provide unique information on year-to-year variations in the atm. environment.
59. 59

    Jacobs, G. A.; Ngodock, H. E. The Maintenance of Conservative Physical Laws within Data Assimilation Systems. Mon. Weather Rev. 2003, 131, 2595– 2607,  DOI: 10.1175/1520-0493(2003)131<2595:TMOCPL>2.0.CO;2

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60. 60

    Liu, L.; Zhang, X.; Xu, W.; Liu, X.; Lu, X.; Wei, J.; Li, Y.; Yang, Y.; Wang, Z.; Wong, A. Reviewing Global Estimates of Surface Reactive Nitrogen Concentration and Deposition Using Satellite Observation. Atmos. Chem. Phys. 2020, 2, 1– 44,  DOI: 10.5194/acp-20-8641-2020

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61. 61

    Inness, A.; Blechschmidt, A. M.; Bouarar, I.; Chabrillat, S.; Crepulja, M.; Engelen, R. J.; Eskes, H.; Flemming, J.; Gaudel, A.; Hendrick, F.; Huijnen, V.; Jones, L.; Kapsomenakis, J.; Katragkou, E.; Keppens, A.; Langerock, B.; DeMazière, M.; Melas, D.; Parrington, M.; Peuch, V. H.; Razinger, M.; Richter, A.; Schultz, M. G.; Suttie, M.; Thouret, V.; Vrekoussis, M.; Wagner, A.; Zerefos, C. Data Assimilation of Satellite-Retrieved Ozone, Carbon Monoxide and Nitrogen Dioxide with ECMWF’s Composition-IFS. Atmos. Chem. Phys. 2015, 15 (9), 5275– 5303,  DOI: 10.5194/acp-15-5275-2015

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    61

    Data assimilation of satellite-retrieved ozone, carbon monoxide and nitrogen dioxide with ECMWF's Composition-IFS

    Inness, A.; Blechschmidt, A.-M.; Bouarar, I.; Chabrillat, S.; Crepulja, M.; Engelen, R. J.; Eskes, H.; Flemming, J.; Gaudel, A.; Hendrick, F.; Huijnen, V.; Jones, L.; Kapsomenakis, J.; Katragkou, E.; Keppens, A.; Langerock, B.; de Maziere, M.; Melas, D.; Parrington, M.; Peuch, V. H.; Razinger, M.; Richter, A.; Schultz, M. G.; Suttie, M.; Thouret, V.; Vrekoussis, M.; Wagner, A.; Zerefos, C.

    Atmospheric Chemistry and Physics (2015), 15 (9), 5275-5303CODEN: ACPTCE; ISSN:1680-7324. (Copernicus Publications)

    Daily global analyses and 5-day forecasts are generated in the context of the European Monitoring Atm. Compn. and Climate (MACC) project using an extended version of the Integrated Forecasting System (IFS) of the European Center for Medium-Range Weather Forecasts (ECMWF). The IFS now includes modules for chem., deposition and emission of reactive gases, aerosols, and greenhouse gases, and the 4-dimensional variational data assimilation scheme makes use of multiple satellite observations of atm. compn. in addn. to meteorol. observations. This paper describes the data assimilation setup of the new Compn.-IFS (C-IFS) with respect to reactive gases and validates anal. fields of ozone (O3), carbon monoxide (CO), and nitrogen dioxide (NO2) for the year 2008 against independent observations and a control run without data assimilation. The largest improvement in CO by assimilation of Measurements of Pollution in the Troposphere (MOPITT) CO columns is seen in the lower troposphere of the Northern Hemisphere (NH) extratropics during winter, and during the South African biomass-burning season. The assimilation of several O3 total column and stratospheric profile retrievals greatly improves the total column, stratospheric and upper tropospheric O3 anal. fields relative to the control run. The impact on lower tropospheric ozone, which comes from the residual of the total column and stratospheric profile O3 data, is smaller, but nevertheless there is some improvement particularly in the NH during winter and spring. The impact of the assimilation of tropospheric NO2 columns from the Ozone Monitoring Instrument (OMI) is small because of the short lifetime of NO2, suggesting that NO2 observations would be better used to adjust emissions instead of initial conditions. The results further indicate that the quality of the tropospheric analyses and of the stratospheric ozone anal. obtained with the C-IFS system has improved compared to the previous "coupled" model system of MACC.
62. 62

    Geddes, J. A.; Martin, R. V. Global Deposition of Total Reactive Nitrogen Oxides From. Atmos. Chem. Phys. 2017, 17, 10071– 10091,  DOI: 10.5194/acp-17-10071-2017

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    62

    Global deposition of total reactive nitrogen oxides from 1996 to 2014 constrained with satellite observations of NOcolumns

    Geddes, Jeffrey A.; Martin, Randall V.

    Atmospheric Chemistry and Physics (2017), 17 (16), 10071-10091CODEN: ACPTCE; ISSN:1680-7324. (Copernicus Publications)

    Reactive nitrogen oxides (NOy) are a major constituent of the nitrogen deposited from the atm., but observational constraints on their deposition are limited by poor or nonexistent measurement coverage in many parts of the world. Here we apply NO observations from multiple satellite instruments (GOME, SCIAMACHY, and GOME- 2) to constrain the global deposition of NOy over the last 2 decades. We accomplish this by producing top-down ests. of NOy emissions from inverse modeling of satellite NO columns over 1996-2014, and including these emissions in the GEOS-Chem chem. transport model to simulate chem., transport, and deposition of NOy . Our ests. of long-term mean wet nitrate NO y deposition are highly consistent with available measurements in North America, Europe, and East Asia combined. Likewise, our calcd. trends in wet NOy deposition are largely consistent with the measurements, with 129 of the 136 gridded model- data pairs sharing overlapping confidence intervals. About of the global NOy deposition occurs over oceans, with deposition to the North Atlantic Ocean declining and deposition to the northwestern Pacific Ocean increasing. A sensitivity study indicates that simulated NOy deposition is robust to uncertainties in NH3 emissions with a few exceptions. Our novel long-term study provides timely context on the rapid redistribution of atm. nitrogen transport and subsequent deposition to ecosystems around the world.
63. 63

    Silva, S. J.; Heald, C. L.; Ravela, S.; Mammarella, I.; Munger, J. W. A Deep Learning Parameterization for Ozone Dry Deposition Velocities. Geophys. Res. Lett. 2019, 46 (2), 983– 989,  DOI: 10.1029/2018GL081049

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64. 64

    Paulot, F.; Malyshev, S.; Nguyen, T.; Crounse, J. D.; Shevliakova, E.; Horowitz, L. W. Representing Sub-Grid Scale Variations in Nitrogen Deposition Associated with Land Use in a Global Earth System Model: Implications for Present and Future Nitrogen Deposition Fluxes over North America. Atmos. Chem. Phys. 2018, 18, 17963– 17978,  DOI: 10.5194/acp-18-17963-2018

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    64

    Representing sub-grid scale variations in nitrogen deposition associated with land use in a global Earth system model: implications for present and future nitrogen deposition fluxes over North America

    Paulot, Fabien; Malyshev, Sergey; Nguyen, Tran; Crounse, John D.; Shevliakova, Elena; Horowitz, Larry W.

    Atmospheric Chemistry and Physics (2018), 18 (24), 17963-17978CODEN: ACPTCE; ISSN:1680-7324. (Copernicus Publications)

    Reactive nitrogen (N) emissions have increased over the last 150 years as a result of greater fossil fuel combustion and food prodn. The resulting increase in N deposition can alter the function of ecosystems, but characterizing its ecol. impacts remains challenging, in part because of uncertainties in model-based ests. of N dry deposition. Here, we use the Geophys. Fluid Dynamics Lab. (GFDL) atm. chem.-climate model (AM3) coupled with the GFDL land model (LM3) to est. dry deposition velocities. We leverage the tiled structure of LM3 to represent the impact of phys., hydrol., and ecol. heterogeneities on the surface removal of chem. tracers. We show that this framework can be used to est. N deposition at more ecol. relevant scales (e.g., natural vegetation, water bodies) than from the coarseresoln. global model AM3. Focusing on North America, we show that the faster removal of N over forested ecosystems relative to cropland and pasture implies that coarseresoln. ests. of N deposition from global models systematically underestimate N deposition to natural vegetation by 10% to 30% in the central and eastern US. Neglecting the sub-grid scale heterogeneity of dry deposition velocities also results in an underestimate (overestimate) of the amt. of reduced (oxidized) nitrogen deposited to water bodies. Overall, changes in land cover assocd. with human activities are found to slow down the removal of N from the atm., causing a redn. in the dry oxidized, dry reduced, and total (wet+dry) N deposition over the contiguous US of 8 %, 26 %, and 6 %, resp. We also find that the redn. in the overall rate of removal of N assocd. with land-use change tends to increase N deposition on the remaining natural vegetation and facilitate N export to Canada. We show that sub-grid scale differences in the surface removal of oxidized and reduced nitrogen imply that projected near-term (2010-2050) changes in oxidized (-47 %) and reduced (+40 %) US N emissions will cause opposite changes in N deposition to water bodies (increase) and natural vegetation (decrease) in the eastern US, with potential implications for acidification and ecosystems.