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3. Patterns and trends of atmospheric mercury in the GMOS network: Insights based on a decade of measurements

Author

Bencardino, Mariantonia, D’Amore, Francesco, Angot, Hélène, Angiuli, Lorenzo, Bertrand, Yann, Cairns, Warren, Diéguez, María C., Dommergue, Aurélien, Ebinghaus, Ralf, Esposito, Giulio, Komínková, Kateřina, Labuschagne, Casper, Mannarino, Valentino, Martin, Lynwill, Martino, Maria, Neves, Luis Mendes, Mashyanov, Nikolay, Magand, Olivier, Nelson, Peter, Norstrom, Claus, Read, Katie, Sholupov, Sergey, Skov, Henrik, Tassone, Antonella, Vítková, Gabriela, Cinnirella, Sergio, Sprovieri, Francesca, and Pirrone, Nicola

Published
2024
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4. Revising VOC emissions speciation improves the simulation of global background ethane and propane.

Author

Rowlinson, Matthew J., Evans, Mat J., Carpenter, Lucy J., Read, Katie A., Punjabi, Shalini, Adedeji, Adedayo, Fakes, Luke, Lewis, Ally, Richmond, Ben, Passant, Neil, Murrells, Tim, Henderson, Barron, Bates, Kelvin H., and Helmig, Detlev

Abstract

Non-methane volatile organic compounds (NMVOCs) generate ozone (O 3) when they are oxidised in the presence of oxides of nitrogen, modulate the oxidative capacity of the atmosphere and can lead to the formation of aerosol. Here, we assess the capability of a chemical transport model (GEOS-Chem) to simulate NMVOC concentrations by comparing ethane, propane and higher-alkane observations in remote regions from the NOAA flask Network and the World Meteorological Organization's Global Atmosphere Watch (GAW) network. Using the Community Emissions Data System (CEDS) inventory, we find a significant underestimate in the simulated concentration of both ethane (35 %) and propane (64 %), consistent with previous studies. We run a new simulation in which the total mass of anthropogenic NMVOC emitted in a grid box is the same as that used in CEDS but with the NMVOC speciation derived from regional inventories. For US emissions, we use the National Emissions Inventory (NEI); for Europe, we use the UK National Atmospheric Emissions Inventory (NAEI); and for China, we use the Multi-resolution Emission Inventory model for Climate and air pollution research (MEIC). These changes lead to a large increase in the modelled concentrations of ethane, improving the mean model bias from - 35 % to - 4 %. Simulated propane also improves (from - 64 % to - 48 % mean model bias), but there remains a substantial model underestimate. There were relatively minor changes to other NMVOCs. The low bias in simulated global ethane concentration is essentially removed, resolving one long-term issue in global simulations. Propane concentrations are improved but remain significantly underestimated, suggesting the potential for a missing global propane source. The change in the NMVOC emission speciation results in only minor changes in tropospheric O 3 and OH concentrations. [ABSTRACT FROM AUTHOR]

Published
2024
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5. Data supporting the North Atlantic Climate System: Integrated Studies (ACSIS) programme, including atmospheric composition, oceanographic and sea ice observations (2016–2022) and output from ocean, atmosphere, land and sea-ice models (1950–2050)

Author

Archibald, Alexander T., primary, Sinha, Bablu, additional, Russo, Maria, additional, Matthews, Emily, additional, Squires, Freya, additional, Abraham, N. Luke, additional, Bauguitte, Stephane, additional, Bannan, Thomas, additional, Bell, Thomas, additional, Berry, David, additional, Carpenter, Lucy, additional, Coe, Hugh, additional, Coward, Andrew, additional, Edwards, Peter, additional, Feltham, Daniel, additional, Heard, Dwayne, additional, Hopkins, Jim, additional, Keeble, James, additional, Kent, Elizabeth C., additional, King, Brian, additional, Lawrence, Isobel R., additional, Lee, James, additional, Macintosh, Claire R., additional, Megann, Alex, additional, Moat, Ben I., additional, Read, Katie, additional, Reed, Chris, additional, Roberts, Malcolm, additional, Schiemann, Reinhard, additional, Schroeder, David, additional, Smyth, Tim, additional, Temple, Loren, additional, Thamban, Navaneeth, additional, Whalley, Lisa, additional, Williams, Simon, additional, Wu, Huihui, additional, and Yang, Ming-Xi, additional

Published
2024
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6. Patterns and Trends of Atmospheric Mercury in the Gmos Network: Insights Based on a Decade of Measurements

Author

Bencardino, Mariantonia, primary, D'Amore, Francesco, additional, Angot, H., additional, Angiuli, Lorenzo, additional, Bertrand, Yann, additional, Cairns, W.R.L., additional, Diéguez, María, additional, Dommergue, Aurelien, additional, Ebinghaus, Ralf, additional, Esposito, Giulio, additional, Komínková, Kateřina, additional, Labuschagne, Casper, additional, Mannarino, Valentino, additional, Martin, Lynwill G., additional, Martino, Maria, additional, Neves, Luis, additional, Mashyanov, Nikolay, additional, Megand, Olivier, additional, Nelson, Peter, additional, Nordstrøm, Claus, additional, Read, Katie, additional, Sholupov, Sergey, additional, Skov, Henrik, additional, Tassone, Antonella, additional, Vítková, Gabriela, additional, Cinnirella, Sergio, additional, Sprovieri, Francesca, additional, and Pirrone, Nicola, additional

Published
2024
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7. Revising VOC emissions speciation improves global simulations of ethane and propane

Author

Rowlinson, Matthew James, primary, Carpenter, Lucy, additional, Read, Katie, additional, Punjabi, Shalini, additional, Adedeji, Adedayo, additional, Fakes, Luke, additional, Lewis, Ally, additional, Richmond, Ben, additional, Passant, Neil, additional, Murrells, Tim, additional, Henderson, Barron, additional, Bates, Kelvin, additional, Helmig, Deltev, additional, and Evans, Mat, additional

Published
2023
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10. Perspectives and Integration in SOLAS Science

Author

Garçon, Véronique C., Bell, Thomas G., Wallace, Douglas, Arnold, Steve R., Baker, Alex, Bakker, Dorothee C. E., Bange, Hermann W., Bates, Nicholas R., Bopp, Laurent, Boutin, Jacqueline, Boyd, Philip W., Bracher, Astrid, Burrows, John P., Carpenter, Lucy J., de Leeuw, Gerrit, Fennel, Katja, Font, Jordi, Friedrich, Tobias, Garbe, Christoph S., Gruber, Nicolas, Jaeglé, Lyatt, Lana, Arancha, Lee, James D., Liss, Peter S., Miller, Lisa A., Olgun, Nazli, Olsen, Are, Pfeil, Benjamin, Quack, Birgit, Read, Katie A., Reul, Nicolas, Rödenbeck, Christian, Rohekar, Shital S., Saiz-Lopez, Alfonso, Saltzman, Eric S., Schneising, Oliver, Schuster, Ute, Seferian, Roland, Steinhoff, Tobias, Traon, Pierre-Yves Le, Ziska, Franziska, Liss, Peter S., editor, and Johnson, Martin T., editor

Published
2014
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11. Revising VOC emissions speciation improves global simulations of ethane and propane.

Author

Rowlinson, Matthew James, Carpenter, Lucy, Read, Katie, Punjabi, Shalini, Adedeji, Adedayo, Fakes, Luke, Lewis, Ally, Richmond, Ben, Passant, Neil, Murrells, Tim, Henderson, Barron, Bates, Kelvin, Helmig, Deltev, and Evans, Mat

Subjects
ETHANES, PROPANE, VOLATILE organic compounds, EMISSION inventories, GENETIC speciation, CHEMICAL models
Abstract

Non-Methane Volatile Organic Compounds (NMVOCs) generate ozone (O3) when they are oxidized in the presence of oxides of nitrogen, modulate the oxidative capacity of the atmosphere and can lead to the formation of aerosol. Here, we assess the capability of a chemical transport model (GEOS-Chem) to simulate NMVOC concentrations by comparing ethane, propane and higher alkane observations in remote regions from the NOAA Flask Network and the World Meteorological Organization's Global Atmosphere Watch (GAW) network. Using the Community Emissions Data System (CEDS) inventory we find a significant underestimate in the simulated concentration of both ethane (35 %) and propane (64 %), consistent with previous studies. We run a new simulation where the total mass of anthropogenic NMVOC emitted in a grid box is the same as that used in CEDS, but with the NMVOC speciation derived from regional inventories. For US emissions we use the National Emissions Inventory (NEI), for Europe we use the UK National Atmospheric Emissions Inventory (NAEI), and for China, the Multi-resolution Emission Inventory for China (MEIC). These changes lead to a large increase in the modelled concentrations of ethane, improving the mean model bias from -35 % to -3.8 %. Simulated propane also improves (from -64 % to -48.0 % mean model bias), but there remains a substantial model underestimate. There were relatively minor changes to other NMVOCs. The low bias in simulated global ethane concentration is essentially removed, resolving one long-term issue in global simulations. Propane concentrations are improved but remain significantly underestimated, suggesting the potential for a missing global propane source. The change in the NMVOC emission speciation results in only minor changes in tropospheric O3 and OH concentrations. [ABSTRACT FROM AUTHOR]

Published
2023
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12. Revising VOC emissions speciation improves global simulations of ethane and propane.

Author

Rowlinson, Matthew J., Carpenter, Lucy J., Read, Katie A., Punjabi, Shalini, Adedeji, Adedayo, Fakes, Luke, Lewis, Ally, Richmond, Ben, Passant, Neil, Murrells, Tim, Henderson, Barron, Bates, Kelvin H., Helmig, Detlev, and Evans, Mat J.

Abstract

Non-Methane Volatile Organic Compounds (NMVOCs) generate ozone (O3) when they are oxidized in the presence of oxides of nitrogen, modulate the oxidative capacity of the atmosphere and can lead to the formation of aerosol. Here, we assess the capability of a chemical transport model (GEOS-Chem) to simulate NMVOC concentrations by comparing ethane, propane and higher alkane observations in remote regions from the NOAA Flask Network and the World Meteorological Organization's 5 Global Atmosphere Watch (GAW) network. Using the Community Emissions Data System (CEDS) inventory we find a significant underestimate in the simulated concentration of both ethane (35%) and propane (64%), consistent with previous studies. We run a new simulation where the total mass of anthropogenic NMVOC emitted in a grid box is the same as that used in CEDS, but with the NMVOC speciation derived from regional inventories. For US emissions we use the National Emissions Inventory (NEI), for Europe we use the UK National Atmospheric Emissions Inventory (NAEI), and for China, the Multi-resolution Emission Inventory for China (MEIC). These changes lead to a large increase in the modelled concentrations of ethane, improving the mean model bias from -35% to -3.8%. Simulated propane also improves (from -64% to -48.0% mean model bias), but there remains a substantial model underestimate. There were relatively minor changes to other NMVOCs. The low bias in simulated global ethane concentration is essentially removed, resolving one long-term issue in global simulations. Propane concentrations are improved but remain significantly underestimated, suggesting the potential for a missing global propane source. The change in the NMVOC emission speciation results in only minor changes in tropospheric O3 and OH concentrations. [ABSTRACT FROM AUTHOR]

Published
2023
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13. Extensive field evidence for the release of HONO from the photolysis of nitrate aerosols

Author

Andersen, Simone T., primary, Carpenter, Lucy J., additional, Reed, Chris, additional, Lee, James D., additional, Chance, Rosie, additional, Sherwen, Tomás, additional, Vaughan, Adam R., additional, Stewart, Jordan, additional, Edwards, Pete M., additional, Bloss, William J., additional, Sommariva, Roberto, additional, Crilley, Leigh R., additional, Nott, Graeme J., additional, Neves, Luis, additional, Read, Katie, additional, Heard, Dwayne E., additional, Seakins, Paul W., additional, Whalley, Lisa K., additional, Boustead, Graham A., additional, Fleming, Lauren T., additional, Stone, Daniel, additional, and Fomba, Khanneh Wadinga, additional

Published
2023
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14. Fundamental oxidation processes in the remote marine atmosphere investigated using the NO–NO2–O3 photostationary state

Author

Andersen, Simone T., primary, Nelson, Beth S., additional, Read, Katie A., additional, Punjabi, Shalini, additional, Neves, Luis, additional, Rowlinson, Matthew J., additional, Hopkins, James, additional, Sherwen, Tomás, additional, Whalley, Lisa K., additional, Lee, James D., additional, and Carpenter, Lucy J., additional

Published
2022
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15. Air pollution measurement errors: is your data fit for purpose?

Author

Diez, Sebastian, primary, Lacy, Stuart E., additional, Bannan, Thomas J., additional, Flynn, Michael, additional, Gardiner, Tom, additional, Harrison, David, additional, Marsden, Nicholas, additional, Martin, Nicholas A., additional, Read, Katie, additional, and Edwards, Pete M., additional

Published
2022
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16. Supplementary material to "Fundamental Oxidation Processes in the Remote Marine Atmosphere Investigated Using the NO-NO2-O3 Photostationary State"

Author

Andersen, Simone T., primary, Nelson, Beth S., additional, Read, Katie A., additional, Punjabi, Shalini, additional, Neves, Luis, additional, Rowlinson, Matthew J., additional, Hopkins, James, additional, Sherwen, Tomás, additional, Whalley, Lisa K., additional, Lee, James D., additional, and Carpenter, Lucy J., additional

Published
2022
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17. Observations and modelling of glyoxal in the tropical Atlantic marine boundary layer

Author

Walker, Hannah, primary, Stone, Daniel, additional, Ingham, Trevor, additional, Hackenberg, Sina, additional, Cryer, Danny, additional, Punjabi, Shalini, additional, Read, Katie, additional, Lee, James, additional, Whalley, Lisa, additional, Spracklen, Dominick V., additional, Carpenter, Lucy J., additional, Arnold, Steve R., additional, and Heard, Dwayne E., additional

Published
2022
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20. Observations and modelling of glyoxal in the tropical Atlantic marine boundary layer

Author

Walker, Hannah, primary, Stone, Daniel, additional, Ingham, Trevor, additional, Hackenberg, Sina, additional, Cryer, Danny, additional, Punjabi, Shalini, additional, Read, Katie, additional, Lee, James, additional, Whalley, Lisa, additional, Spracklen, Dominick Vincent, additional, Carpenter, Lucy Jane, additional, Arnold, Steve Robert, additional, and Heard, Dwayne Ellis, additional

Published
2021
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21. Supplementary material to "Observations and modelling of glyoxal in the tropical Atlantic marine boundary layer"

Author

Walker, Hannah, primary, Stone, Daniel, additional, Ingham, Trevor, additional, Hackenberg, Sina, additional, Cryer, Danny, additional, Punjabi, Shalini, additional, Read, Katie, additional, Lee, James, additional, Whalley, Lisa, additional, Spracklen, Dominick Vincent, additional, Carpenter, Lucy Jane, additional, Arnold, Steve Robert, additional, and Heard, Dwayne Ellis, additional

Published
2021
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27. Perspectives and Integration in SOLAS Science

Author

Garçon, Véronique C., primary, Bell, Thomas G., additional, Wallace, Douglas, additional, Arnold, Steve R., additional, Baker, Alex, additional, Bakker, Dorothee C. E., additional, Bange, Hermann W., additional, Bates, Nicholas R., additional, Bopp, Laurent, additional, Boutin, Jacqueline, additional, Boyd, Philip W., additional, Bracher, Astrid, additional, Burrows, John P., additional, Carpenter, Lucy J., additional, de Leeuw, Gerrit, additional, Fennel, Katja, additional, Font, Jordi, additional, Friedrich, Tobias, additional, Garbe, Christoph S., additional, Gruber, Nicolas, additional, Jaeglé, Lyatt, additional, Lana, Arancha, additional, Lee, James D., additional, Liss, Peter S., additional, Miller, Lisa A., additional, Olgun, Nazli, additional, Olsen, Are, additional, Pfeil, Benjamin, additional, Quack, Birgit, additional, Read, Katie A., additional, Reul, Nicolas, additional, Rödenbeck, Christian, additional, Rohekar, Shital S., additional, Saiz-Lopez, Alfonso, additional, Saltzman, Eric S., additional, Schneising, Oliver, additional, Schuster, Ute, additional, Seferian, Roland, additional, Steinhoff, Tobias, additional, Traon, Pierre-Yves Le, additional, and Ziska, Franziska, additional

Published
2013
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28. Fundamental Oxidation Processes in the Remote Marine Atmosphere Investigated Using the NO-NO2-O3 Photostationary State.

Author

Andersen, Simone T., Nelson, Beth S., Read, Katie A., Punjabi, Shalini, Neves, Luis, Rowlinson, Matthew J., Hopkins, James, Sherwen, Tomás, Whalley, Lisa K., Lee, James D., and Carpenter, Lucy J.

Abstract

The photostationary state (PSS) equilibrium between NO and NO2 is reached within minutes in the atmosphere and can be described by the PSS parameter, φ. Deviations from expected values of φ have previously been used to infer missing oxidants in diverse locations, from highly polluted regions to the extremely clean conditions observed in the remote marine boundary layer (MBL), and have been interpreted as missing understanding of fundamental photochemistry. Here, contrary to these previous observations, we observe good agreement between PSS-derived NO2 ([NO2]PSS ext.) calculated from photochemical model predictions of peroxy radicals (RO2 and HO2) and measured NO, O3, and jNO2, and observed NO2 in extremely clean air containing low levels of CO (< 90 ppbV) and VOCs. However, in clean air containing small amounts of aged pollution (CO > 100 ppbV), we observed higher levels of NO2 than inferred from the PSS, with [NO2]Obs./[NO2]PSS ext. of 1.12–1.68 (25th–75th percentile) implying 18.5–104 pptV (25th–75th percentile) of missing RO2 radicals. Potential NO2 measurement artefacts have to be carefully considered when comparing PSS-derived NO2 to observed NO2, but we show that the NO2 artefact required to explain the deviation would have to be ~ 4 times greater than the maximum calculated from known interferences. If the missing RO2 radicals have an ozone production efficiency equivalent to that of methyl peroxy radicals (CH3O2), then the calculated net ozone production including these additional oxidants is similar to that observed, within estimated uncertainties, once halogen oxide chemistry is accounted for. This implies that peroxy radicals cannot be excluded as the missing oxidant in clean marine air containing aged pollution, and that measured and modelled RO2 are both significantly underestimated under these conditions. [ABSTRACT FROM AUTHOR]

Published
2022
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31. Quantifying bioaerosol concentrations in dust clouds through online UV-LIF and mass spectrometry measurements at the Cape Verde Atmospheric Observatory

Author

Morrison, Douglas, primary, Crawford, Ian, additional, Marsden, Nicholas, additional, Flynn, Michael, additional, Read, Katie, additional, Neves, Luis, additional, Foot, Virginia, additional, Kaye, Paul, additional, Stanley, Warren, additional, Coe, Hugh, additional, Topping, David, additional, and Gallagher, Martin, additional

Published
2020
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32. Marine organic matter in the remote environment of the Cape Verde islands – an introduction and overview to the MarParCloud campaign

Author

van Pinxteren, Manuela, primary, Fomba, Khanneh Wadinga, additional, Triesch, Nadja, additional, Stolle, Christian, additional, Wurl, Oliver, additional, Bahlmann, Enno, additional, Gong, Xianda, additional, Voigtländer, Jens, additional, Wex, Heike, additional, Robinson, Tiera-Brandy, additional, Barthel, Stefan, additional, Zeppenfeld, Sebastian, additional, Hoffmann, Erik Hans, additional, Roveretto, Marie, additional, Li, Chunlin, additional, Grosselin, Benoit, additional, Daële, Veronique, additional, Senf, Fabian, additional, van Pinxteren, Dominik, additional, Manzi, Malena, additional, Zabalegui, Nicolás, additional, Frka, Sanja, additional, Gašparović, Blaženka, additional, Pereira, Ryan, additional, Li, Tao, additional, Wen, Liang, additional, Li, Jiarong, additional, Zhu, Chao, additional, Chen, Hui, additional, Chen, Jianmin, additional, Fiedler, Björn, additional, von Tümpling, Wolf, additional, Read, Katie Alana, additional, Punjabi, Shalini, additional, Lewis, Alastair Charles, additional, Hopkins, James Roland, additional, Carpenter, Lucy Jane, additional, Peeken, Ilka, additional, Rixen, Tim, additional, Schulz-Bull, Detlef, additional, Monge, María Eugenia, additional, Mellouki, Abdelwahid, additional, George, Christian, additional, Stratmann, Frank, additional, and Herrmann, Hartmut, additional

Published
2020
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33. Supplementary material to "Quantifying Bioaerosol Concentrations in Dust Clouds through Online UV-LIF and Mass Spectrometry Measurements at the Cape Verde Atmospheric Observatory"

Author

Morrison, Douglas, primary, Crawford, Ian, additional, Marsden, Nicholas, additional, Flynn, Michael, additional, Read, Katie, additional, Neves, Luis, additional, Foot, Virginia, additional, Kaye, Paul, additional, Stanley, Warren, additional, Coe, Hugh, additional, Topping, David, additional, and Gallagher, Martin, additional

Published
2020
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34. Observations and modelling of glyoxal in the tropical Atlantic marine boundary layer.

Author

Walker, Hannah, Stone, Daniel, Ingham, Trevor, Hackenberg, Sina, Cryer, Danny, Punjabi, Shalini, Read, Katie, Lee, James, Whalley, Lisa, Spracklen, Dominick V., Carpenter, Lucy J., Arnold, Steve R., and Heard, Dwayne E.

Abstract

In situ field measurements of glyoxal at the surface in the tropical marine boundary layer have been made with a temporal resolution of a few minutes during two 4-week campaigns in June-July and August-September 2014 at the Cape Verde Atmospheric Observatory (CVAO, 16° 52' N, 24° 52' W). Using laser-induced phosphorescence spectroscopy with an instrumental detection limit of ~ 1 pptv (1 hour averaging), volume mixing ratios up to ~10 pptv were observed, with 24 hour averaged mixing ratios of 4.9 pptv and 6.3 pptv observed during the first and second campaigns, respectively. Some diel behaviour was observed but this was not marked. A box model using the detailed Master Chemical Mechanism (version 3.2) and constrained with detailed observations of a suite of species co-measured at the observatory was used to calculate glyoxal mixing ratios. There is a general model underestimation of the glyoxal observations during both campaigns, with mean midday (1100-1300 hours) observed-to-modelled ratios for glyoxal of 3.2 and 4.2 for the two campaigns, respectively, and higher ratios at night. A rate of production analysis shows the dominant sources of glyoxal in this environment to be the reactions of OH with glycoaldehyde and acetylene, with a significant contribution from the reaction of OH with the peroxide HC(O)CH2OOH, which itself derives from OH oxidation of acetaldehyde. Increased mixing ratios of acetaldehyde, which is unconstrained and potentially underestimated in the base model, can significantly improve the agreement between the observed and modelled glyoxal during the day. Mean midday observed-to-modelled glyoxal ratios decreased to 1.3 and 1.8 for campaigns 1 and 2, respectively, on constraint to a fixed acetaldehyde mixing ratio of 200 pptv, which is consistent with recent airborne measurements near CVAO. However, a significant model underprediction remains at night. The model was sensitive to changes in deposition rates of model intermediates and the uptake of glyoxal onto aerosol. The midday (1100-1300) mean modelled glyoxal mixing ratio decreased by factors of 0.87 and 0.90 on doubling the deposition rates of model intermediates and aerosol uptake of glyoxal, respectively, and increased by factors of 1.10 and 1.06 on halving the deposition rates of model intermediates and aerosol uptake of glyoxal, respectively. Although measured levels of monoterpenes at the site (total of ~ 1 pptv) do not significantly influence the model calculated levels of glyoxal, transport of air from a source region with high monoterpene emissions to the site has the potential to give elevated mixing ratios of glyoxal from monoterpene oxidation products, but the values are highly sensitive to the deposition rates of these oxidised intermediates. A source of glyoxal derived from production in the ocean surface organic microlayer cannot be ruled out on the basis of this work, and may be significant at night. [ABSTRACT FROM AUTHOR]

Published
2021
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35. Global impact of nitrate photolysis in sea-salt aerosol on NOx, OH, and O3 in the marine boundary layer

Author

Kasibhatla, Prasad, Sherwen, Tomás, Evans, Mathew J., Carpenter, Lucy J., Reed, Chris, Alexander, Becky, Chen, Qianjie, Sulprizio, Melissa P., Lee, James D., Read, Katie A., Bloss, William, Crilley, Leigh R., Keene, William C., Pszenny, Alexander A.P., and Hodzic, Alma

Abstract

Recent field studies have suggested that sea-salt particulate nitrate (NITs) photolysis may act as a significant local source of nitrogen oxides (NOx) over oceans. We present a study of the global impact of this process on oxidant concentrations in the marine boundary layer (MBL) using the GEOS-Chem model, after first updating the model to better simulate observed gas-particle phase partitioning of nitrate in the marine boundary layer. Model comparisons with long-term measurements of NOx from the Cape Verde Atmospheric Observatory (CVAO) in the eastern tropical North Atlantic provide support for an in situ source of NOx from NITs photolysis, with NITs photolysis coefficients about 25-50 times larger than corresponding HNO3 photolysis coefficients. Short-term measurements of nitrous acid (HONO) at this location show a clear daytime peak, with average peak mixing ratios ranging from 3 to 6 pptv. The model reproduces the general shape of the diurnal HONO profile only when NITs photolysis is included, but the magnitude of the daytime peak mixing ratio is under-predicted. This under-prediction is somewhat reduced if HONO yields from NITs photolysis are assumed to be close to unity. The combined NOx and HONO analysis suggests that the upper limit of the ratio of NITs : HNO3 photolysis coefficients is about 100. The largest simulated relative impact of NITs photolysis is in the tropical and subtropical marine boundary layer, with peak local enhancements ranging from factors of 5 to 20 for NOx, 1.2 to 1.6 for OH, and 1.1 to 1.3 for ozone. Since the spatial extent of the sea-salt aerosol (SSA) impact is limited, global impacts on NOx, ozone, and OH mass burdens are small ( ∼ 1-3 %). We also present preliminary analysis showing that particulate nitrate photolysis in accumulation-mode aerosols (predominantly over continental regions) could lead to ppbv-level increases in ozone in the continental boundary layer. Our results highlight the need for more comprehensive long-term measurements of NOx, and related species like HONO and sea-salt particulate nitrate, to better constrain the impact of particulate nitrate photolysis on marine boundary layer oxidant chemistry. Further field and laboratory studies on particulate nitrate photolysis in other aerosol types are also needed to better understand the impact of this process on continental boundary layer oxidant chemistry.

Published
2018

36. Impacts of bromine and iodine chemistry on tropospheric OH and HO2 : Comparing observations with box and global model perspectives

Author

Stone, Daniel, Sherwen, Toms, Evans, Mathew J., Vaughan, Stewart, Ingham, Trevor, Whalley, Lisa K., Edwards, Peter M., Read, Katie A., Lee, James D., Moller, Sarah J., Carpenter, Lucy J., Lewis, Alastair C., and Heard, Dwayne E.

Abstract

The chemistry of the halogen species bromine and iodine has a range of impacts on tropospheric composition, and can affect oxidising capacity in a number of ways. However, recent studies disagree on the overall sign of the impacts of halogens on the oxidising capacity of the troposphere. We present simulations of OH and HO2 radicals for comparison with observations made in the remote tropical ocean boundary layer during the Seasonal Oxidant Study at the Cape Verde Atmospheric Observatory in 2009. We use both a constrained box model, using detailed chemistry derived from the Master Chemical Mechanism (v3.2), and the three-dimensional global chemistry transport model GEOS-Chem. Both model approaches reproduce the diurnal trends in OH and HO2. Absolute observed concentrations are well reproduced by the box model but are overpredicted by the global model, potentially owing to incomplete consideration of oceanic sourced radical sinks. The two models, however, differ in the impacts of halogen chemistry. In the box model, halogen chemistry acts to increase OH concentrations (by 9.8% at midday at the Cape Verde Atmospheric Observatory), while the global model exhibits a small increase in OH at the Cape Verde Atmospheric Observatory (by 0.6% at midday) but overall shows a decrease in the global annual mass-weighted mean OH of 4.5%. These differences reflect the variety of timescales through which the halogens impact the chemical system. On short timescales, photolysis of HOBr and HOI, produced by reactions of HO2 with BrO and IO, respectively, increases the OH concentration. On longer timescales, halogen-catalysed ozone destruction cycles lead to lower primary production of OH radicals through ozone photolysis, and thus to lower OH concentrations. The global model includes more of the longer timescale responses than the constrained box model, and overall the global impact of the longer timescale response (reduced primary production due to lower O3 concentrations) overwhelms the shorter timescale response (enhanced cycling from HO2 to OH), and thus the global OH concentration decreases. The Earth system contains many such responses on a large range of timescales. This work highlights the care that needs to be taken to understand the full impact of any one process on the system as a whole.

Published
2018

37. Marine organic matter in the remote environment of the Cape Verde Islands – An introduction and overview to the MarParCloud campaign

Author

van Pinxteren, Manuela, primary, Fomba, Khanneh Wadinga, additional, Triesch, Nadja, additional, Stolle, Christian, additional, Wurl, Oliver, additional, Bahlmann, Enno, additional, Gong, Xianda, additional, Voigtländer, Jens, additional, Wex, Heike, additional, Robinson, Tiera-Brandy, additional, Barthel, Stefan, additional, Zeppenfeld, Sebastian, additional, Hoffmann, Erik H., additional, Roveretto, Marie, additional, Li, Chunlin, additional, Grosselin, Benoit, additional, Daële, Veronique, additional, Senf, Fabian, additional, van Pinxteren, Dominik, additional, Manzi, Malena, additional, Zabalegui, Nicolás, additional, Frka, Sanja, additional, Gašparović, Blaženka, additional, Pereira, Ryan, additional, Li, Tao, additional, Wen, Liang, additional, Li, Jiarong, additional, Zhu, Chao, additional, Chen, Hui, additional, Chen, Jianmin, additional, Fiedler, Björn, additional, von Tümpling, Wolf, additional, Read, Katie A., additional, Punjabi, Shalini, additional, C. Lewis, Alastair C., additional, Hopkins, James R., additional, Carpenter, Lucy J., additional, Peeken, Ilka, additional, Rixen, Tim, additional, Schulz-Bull, Detlef, additional, Monge, María Eugenia, additional, Mellouki, Abdelwahid, additional, George, Christian, additional, Stratmann, Frank, additional, and Herrmann, Hartmut, additional

Published
2019
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38. Supplementary material to "Marine organic matter in the remote environment of the Cape Verde Islands – An introduction and overview to the MarParCloud campaign"

Author

van Pinxteren, Manuela, primary, Fomba, Khanneh Wadinga, additional, Triesch, Nadja, additional, Stolle, Christian, additional, Wurl, Oliver, additional, Bahlmann, Enno, additional, Gong, Xianda, additional, Voigtländer, Jens, additional, Wex, Heike, additional, Robinson, Tiera-Brandy, additional, Barthel, Stefan, additional, Zeppenfeld, Sebastian, additional, Hoffmann, Erik H., additional, Roveretto, Marie, additional, Li, Chunlin, additional, Grosselin, Benoit, additional, Daële, Veronique, additional, Senf, Fabian, additional, van Pinxteren, Dominik, additional, Manzi, Malena, additional, Zabalegui, Nicolás, additional, Frka, Sanja, additional, Gašparović, Blaženka, additional, Pereira, Ryan, additional, Li, Tao, additional, Wen, Liang, additional, Li, Jiarong, additional, Zhu, Chao, additional, Chen, Hui, additional, Chen, Jianmin, additional, Fiedler, Björn, additional, von Tümpling, Wolf, additional, Read, Katie A., additional, Punjabi, Shalini, additional, C. Lewis, Alastair C., additional, Hopkins, James R., additional, Carpenter, Lucy J., additional, Peeken, Ilka, additional, Rixen, Tim, additional, Schulz-Bull, Detlef, additional, Monge, María Eugenia, additional, Mellouki, Abdelwahid, additional, George, Christian, additional, Stratmann, Frank, additional, and Herrmann, Hartmut, additional

Published
2019
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39. Recent multivariate changes in the North Atlantic climate system, with a focus on 2005-2016

Author

Robson, Jon, Sutton, Rowan T., Archibald, Alex, Cooper, Fenwick, Christensen, Matthew, Gray, Lesley J., Holliday, N. Penny, Macintosh, Claire, Mcmillan, Malcolm, Moat, Ben, Russo, Maria, Tilling, Rachel, Carslaw, Ken, Desbruyeres, Damien, Embury, Owen, Feltham, Daniel L., Grosvenor, Daniel P., Josey, Simon, King, Brian, Lewis, Alastair, Mccarthy, Gerard D., Merchant, Chris, New, Adrian L., O'Reilly, Christopher H., Osprey, Scott M., Read, Katie, Scaife, Adam, Shepherd, Andrew, Sinha, Bablu, Smeed, David, Smith, Doug, Ridout, Andrew, Woollings, Tim, Yang, Mingxi, Robson, Jon, Sutton, Rowan T., Archibald, Alex, Cooper, Fenwick, Christensen, Matthew, Gray, Lesley J., Holliday, N. Penny, Macintosh, Claire, Mcmillan, Malcolm, Moat, Ben, Russo, Maria, Tilling, Rachel, Carslaw, Ken, Desbruyeres, Damien, Embury, Owen, Feltham, Daniel L., Grosvenor, Daniel P., Josey, Simon, King, Brian, Lewis, Alastair, Mccarthy, Gerard D., Merchant, Chris, New, Adrian L., O'Reilly, Christopher H., Osprey, Scott M., Read, Katie, Scaife, Adam, Shepherd, Andrew, Sinha, Bablu, Smeed, David, Smith, Doug, Ridout, Andrew, Woollings, Tim, and Yang, Mingxi

Abstract

Major changes are occurring across the North Atlantic climate system, including in the atmosphere, ocean and cryosphere, and many observed changes are unprecedented in instrumental records. As the changes in the North Atlantic directly affect the climate and air quality of the surrounding continents, it is important to fully understand how and why the changes are taking place, not least to predict how the region will change in the future. To this end, this article characterizes the recent observed changes in the North Atlantic region, especially in the period 2005–2016, across many different aspects of the system including: atmospheric circulation; atmospheric composition; clouds and aerosols; ocean circulation and properties; and the cryosphere. Recent changes include: an increase in the speed of the North Atlantic jet stream in winter; a southward shift in the North Atlantic jet stream in summer, associated with a weakening summer North Atlantic Oscillation; increases in ozone and methane; increases in net absorbed radiation in the mid‐latitude western Atlantic, linked to an increase in the abundance of high level clouds and a reduction in low level clouds; cooling of sea surface temperatures in the North Atlantic subpolar gyre, concomitant with increases in the western subtropical gyre, and a decline in the Atlantic Ocean's overturning circulation; a decline in Atlantic sector Arctic sea ice and rapid melting of the Greenland Ice Sheet. There are many interactions between these changes, but these interactions are poorly understood. This article concludes by highlighting some of the key outstanding questions.

Published
2018
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40. Four years (2011–2015) of total gaseous mercury measurements from the Cape Verde Atmospheric Observatory

Author

Read, Katie A., Neves, Luis M., Carpenter, Lucy J., Lewis, Alastair C., Fleming, Zoe F., and Kentisbeer, John

Subjects
13. Climate action, Data and Information, Atmospheric Sciences
Abstract

Mercury is a chemical with widespread anthropogenic emissions that is known to be highly toxic to humans, ecosystems and wildlife. Global anthropogenic emissions are around 20 % higher than natural emissions and the amount of mercury released into the atmosphere has increased since the industrial revolution. In 2005 the European Union and the United States adopted measures to reduce mercury use, in part to offset the impacts of increasing emissions in industrialising countries. The changing regional emissions of mercury have impacts on a range of spatial scales. Here we report 4 years (December 2011–December 2015) of total gaseous mercury (TGM) measurements at the Cape Verde Observatory (CVO), a global WMO-GAW station located in the subtropical remote marine boundary layer. Observed total gaseous mercury concentrations were between 1.03 and 1.33 ng m−3 (10th, 90th percentiles), close to expectations based on previous interhemispheric gradient measurements. We observe a decreasing trend in TGM (−0.05 ± 0.04 ng m−3 yr−1, −4.2 % ± 3.3 % yr−1) over the 4 years consistent with the reported decrease of mercury concentrations in North Atlantic surface waters and reductions in anthropogenic emissions. The decrease was more visible in the summer (July–September) than in the winter (December–February), when measurements were impacted by air from the African continent and Sahara/Sahel regions. African air masses were also associated with the highest and most variable TGM concentrations. We suggest that the less pronounced downward trend inclination in African air may be attributed to poorly controlled anthropogenic sources such as artisanal and small-scale gold mining (ASGM) in West Africa.

Published
2017
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41. Tropospheric Ozone Assessment Report: Database and Metrics Data of Global Surface Ozone Observations

Author

Schultz, Martin G., Schröder, Sabine, Lyapina, Olga, Cooper, Owen, Galbally, Ian, Petropavlovskikh, Irina, von Schneidemesser, Erika, Tanimoto, Hiroshi, Elshorbany, Yasin, Naja, Ma, Seguel, Rodrigo, Dauert, Ute, Eckhardt, Paul, Feigenspahn, Stefan, Fiebig, Ma, Hjellbrekke, Anne-Gunn, Hong, You-Deog, Christian Kjeld, Peter, Koide, Hiroshi, Lear, Gary, Tarasick, David, Ueno, Mikio, Wallasch, Ma, Baumgardner, Darrel, Chuang, Ming-Tung, Gillett, Robert, Lee, Meehye, Molloy, Suzie, Moolla, Raeesa, Wang, Tao, Sharps, Katrina, Adame, Jose A., Ancellet, Gérard, Apadula, Francesco, Artaxo, Paul, Barlasina, Ma, Bogucka, Ma, Bonasoni, Paolo, Chang, Limseok, Colomb, Aurélie, Cuevas, Emilio, Cupeiro, Ma, Degorska, Anna, Ding, Aijun, Fröhlich, Ma, Frolova, Ma, Gadhavi, Harish, GHEUSI, François, Gilge, Stefan, Gonzalez, Ma, Gros, Valérie, Hamad, Samera H., Helmig, Detlev, Henriques, Diamantino, Hermansen, Ove, Holla, Robert, Huber, Jacques, Im, Ulas, Jaffe, Daniel A., Komala, Ninong, Kubistin, Dagmar, Lam, Ka-Se, Laurila, Tuomas, Lee, Haeyoung, Levy, Ilan, Mazzoleni, Claudio, Mazzoleni, Lynn, McClure-Begley, Audra, Mohamad, Maznorizan, Murovic, Marijana, Navarro-Comas, M., Nicodim, Florin, Parrish, David, Read, Katie A., Reid, Nick, Ries, Ludwig, Saxena, Pallavi, Schwab, James J., Scorgie, Yvonne, Senik, Irina, Simmonds, Peter, Sinha, Vinayak, Skorokhod, Andrey, Spain, Gerard, Spangl, Wolfgang, Spoor, Ronald, Springston, Stephen R., Steer, Kelvyn, Steinbacher, Martin, Suharguniyawan, Eka, Torre, Paul, Trickl, Thomas, Weili, Lin, Weller, Rolf, Xu, Xiaobin, Xue, Likun, Zhiqiang, Ma, Institut für Energie- und Klimaforschung - Troposphäre (IEK-8), Forschungszentrum Jülich GmbH | Centre de recherche de Juliers, Helmholtz-Gemeinschaft = Helmholtz Association-Helmholtz-Gemeinschaft = Helmholtz Association, Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado [Boulder]-National Oceanic and Atmospheric Administration (NOAA), CSIRO Climate Science Centre, Commonwealth Scientific and Industrial Research Organisation [Canberra] (CSIRO), NOAA Earth System Research Laboratory (ESRL), National Oceanic and Atmospheric Administration (NOAA), Institute for Advanced Sustainability Studies [Potsdam] (IASS), National Institute for Environmental Studies (NIES), NASA Goddard Space Flight Center (GSFC), Aryabhatta Research Institute of Observational Sciences (ARIES), Centro Nacional de Medio Ambiente (CENMA), German Federal Environmental Agency / Umweltbundesamt (UBA), Norwegian Institute for Air Research (NILU), National Institute of Environmental Research [South Korea] (NIER), European Environmental Agency (EEA), Japan Meteorological Agency (JMA), Office of Air and Radiation (OAR), US Environmental Protection Agency (EPA), Environment and Climate Change Canada, Centro de Ciencias de la Atmosfera [Mexico], Universidad Nacional Autónoma de México = National Autonomous University of Mexico (UNAM), National Central University [Taiwan] (NCU), Department of Earth and Environmental Sciences [Korea], Korea University [Seoul], School of Geography, Archaeology and Environmental Studies [Johannesburg] (GAES), University of the Witwatersrand [Johannesburg] (WITS), Department of Civil and Environmental Engineering [Hong Kong] (CEE), The Hong Kong Polytechnic University [Hong Kong] (POLYU), Centre for Ecology and Hydrology [Bangor] (CEH), Natural Environment Research Council (NERC), Instituto Nacional de Técnica Aeroespacial (INTA), TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Ricerca sul Sistema Energetico (RSE), Instituto de Fisica da Universidade de São Paulo (IFUSP), Universidade de São Paulo = University of São Paulo (USP), Servicio Meteorológico Nacional [Buenos Aires], Institute of Meteorology and Water Management - National Research Institute (IMGW - PIB), CNR Institute of Atmospheric Sciences and Climate (ISAC), National Research Council of Italy | Consiglio Nazionale delle Ricerche (CNR), Laboratoire de Météorologie Physique (LaMP), Institut national des sciences de l'Univers (INSU - CNRS)-Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Centre National de la Recherche Scientifique (CNRS), Izaña Atmospheric Research Center (IARC), Agencia Estatal de Meteorología (AEMet), Iinstitute of Environmental Protection - National Research Institute (IOS-PIB), School of Atmospheric Sciences [Nanjing], Nanjing University (NJU), Umweltbundesamt GmbH = Environment Agency Austria, Latvian Environment Geology and Meteorology Centre (LEGMC), National Atmospheric Research Laboratory [Tirupati] (NARL), Indian Space Research Organisation (ISRO), Centre national de recherches météorologiques (CNRM), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS), Zentrum für Medizin-Meteorologische Forschung (ZMMF), Deutscher Wetterdienst [Offenbach] (DWD), Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Chimie Atmosphérique Expérimentale (CAE), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), UMD School of Public Health, University of Maryland [College Park], University of Maryland System-University of Maryland System, Institute of Arctic Alpine Research [University of Colorado Boulder] (INSTAAR), University of Colorado [Boulder], Portuguese Institute for Sea and Atmosphere (IMPA), Norsk Institutt for Luftforskning (NILU), Meteorologisches Observatorium Hohenpeißenberg (MOHp), Department of Environmental Science [Roskilde] (ENVS), Aarhus University [Aarhus], School of Science, Technology, Engineering and Mathematics [Bothell] (STEM), University of Washington-Bothell, Indonesian National Institute of Aeronautics and Space (LAPAN), Finnish Meteorological Institute (FMI), National Institute of Meteorological Sciences (NIMS), Air Quality and Climate Change Division [Jerusalem], Israël Ministry of Environmental Protection, Michigan Technological University (MTU), Malaysian Meteorological Department (MetMalaysia), Ministry of Science, Technology and Innovation [Malaysia] (MOSTI), Slovenian Environment Agency, Administratia Nationala de Meteorologie, Department of Chemistry [York, UK], University of York [York, UK], Auckland Council, Jawaharlal Nehru University (JNU), Atmospheric Sciences Research Center (ASRC), University at Albany [SUNY], State University of New York (SUNY)-State University of New York (SUNY), New South Wales Office of Environment and Heritage, A.M.Obukhov Institute of Atmospheric Physics (IAP), Russian Academy of Sciences [Moscow] (RAS), School of Chemistry [Bristol], University of Bristol [Bristol], Indian Institute of Science Education and Research Mohali (IISER Mohali), National University of Ireland [Galway] (NUI Galway), National Institute for Public Health and the Environment [Bilthoven] (RIVM), Brookhaven National Laboratory [Upton, NY] (BNL), UT-Battelle, LLC-Stony Brook University [SUNY] (SBU), State University of New York (SUNY)-State University of New York (SUNY)-U.S. Department of Energy [Washington] (DOE), South Australia Environment Protection Authority (EPA), Swiss Federal Laboratories for Materials Science and Technology [Thun] (EMPA), Indonesian Meteorological, Climatologicall and Geophysical Agency (BMKG), Environment Protection Authority Victoria (EPA ), Institut für Meteorologie und Klimaforschung - Atmosphärische Umweltforschung (IMK-IFU), Karlsruher Institut für Technologie (KIT), China Meteorological Administration (CMA), Alfred-Wegener-Institut, Helmholtz-Zentrum für Polar- und Meeresforschung (AWI), Shandong University, Universidad Nacional Autónoma de México (UNAM), Instituto de Fisica [Sao Paulo], Universidade de São Paulo (USP), Consiglio Nazionale delle Ricerche (CNR), Université Clermont Auvergne [2017-2020] (UCA [2017-2020])-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Umweltbundesamt GmbH/Environment Agency Austria, National Atmospheric Research Laboratory [Tirupathi] (NARL), Météo France-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Institute of Arctic and Alpine Research (INSTAAR), U.S. Department of Energy [Washington] (DOE)-UT-Battelle, LLC-Stony Brook University [SUNY] (SBU), and Institut national des sciences de l'Univers (INSU - CNRS)-Météo France-Centre National de la Recherche Scientifique (CNRS)

Subjects
lcsh:GE1-350, tropospheric ozone, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Monitoring, ground-level ozone, monitoring, database, Tropospheric ozone, Ecology and Environment, Atmospheric Sciences, Database, Earth sciences, ddc:550, Data and Information, Ground-level ozone, lcsh:Environmental sciences
Abstract

In support of the first Tropospheric Ozone Assessment Report (TOAR) a relational database of global surface ozone observations has been developed and populated with hourly measurement data and enhanced metadata. A comprehensive suite of ozone data products including standard statistics, health and vegetation impact metrics, and trend information, are made available through a common data portal and a web interface. These data form the basis of the TOAR analyses focusing on human health, vegetation, and climate relevant ozone issues, which are part of this special feature. Cooperation among many data centers and individual researchers worldwide made it possible to build the world’s largest collection of in-situ hourly surface ozone data covering the period from 1970 to 2015. By combining the data from almost 10,000 measurement sites around the world with global metadata information, new analyses of surface ozone have become possible, such as the first globally consistent characterisations of measurement sites as either urban or rural/remote. Exploitation of these global metadata allows for new insights into the global distribution, and seasonal and long-term changes of tropospheric ozone and they enable TOAR to perform the first, globally consistent analysis of present-day ozone concentrations and recent ozone changes with relevance to health, agriculture, and climate. Considerable effort was made to harmonize and synthesize data formats and metadata information from various networks and individual data submissions. Extensive quality control was applied to identify questionable and erroneous data, including changes in apparent instrument offsets or calibrations. Such data were excluded from TOAR data products. Limitations of a posteriori data quality assurance are discussed. As a result of the work presented here, global coverage of surface ozone data for scientific analysis has been significantly extended. Yet, large gaps remain in the surface observation network both in terms of regions without monitoring, and in terms of regions that have monitoring programs but no public access to the data archive. Therefore future improvements to the database will require not only improved data harmonization, but also expanded data sharing and increased monitoring in data-sparse regions. This work is part of the Tropospheric Ozone Assessment Report (TOAR) which was supported by the International Global Atmospheric Chemistry (IGAC) project, the National Oceanic and Atmospheric Administration (NOAA), Forschungszentrum Jülich, and the World Meteorological Organisation (WMO). Many institutions and agencies sup¬ported the implementation of the measurements, and the processing, quality assurance, and submission of the data contained in the TOAR database.

Published
2017
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42. Five-Year Records of Mercury Concentrations Observed at Ground-Based Monitoring Sites in the Framework of the GMOS Global Network

Author

Sprovieri Francesca (1), Pirrone Nicola (2), Bencardino Mariantonia (1), D'Amore Francesco (1), Carbone Francesco (1), Cinnirella Sergio (1), Landis Matthew (3), Ebinghaus Ralf (4), Martin Lynwill (5), Munthe John (6), Wangberg Ingvar (6), Artaxo Paulo (7), Barbante Carlo (8), Cairns Warren (9), Vardè Massimiliano (10), Diéguez María (11), Garcia Patricia (11), Dommergue Aurélien (12), Angot Hélène (12), Magand Olivier (12), Skov Henrik (13), Horvat Milena (14), Kotnik Joze (14), Read Katie (15), Neves Luis (16), Sena Fabrizio (17), Mashyanov Nikolay (18), Wip Dennis (19), Feng Xin (20), Zhang Hui (20), Fu Xuewu (20), Ramachandran Ramesh (21), Knoery Joël (22), Gawlik Bernd (23), Obolkin Vladimir (24), Labuschagne Casper (25), Morais Fernando (7), Barbose Henrique (7), Brito Joel (7), Cossa Daniel (26), and Weigelt Andreas (27)

Subjects
GMOS, Atmospheric Hg, Hg wet deposition, Mercury, ground-based monitoring sites
Abstract

Long-term monitoring data of ambient mercury (Hg) on a global scale to assess its emission, transport, atmospheric chemistry, and deposition processes is vital to understanding the impact of Hg pollution on the environment. The Global Mercury Observation System (GMOS) started in November 2010 with the overall goal to develop a coordinated global observing system to monitor Hg on a global scale, including a large network of ground-based monitoring stations, ad hoc oceanographic cruises and measurement flights in the troposphere and lower stratosphere. To date, more than 40 ground-based monitoring sites constitute the global network covering many regions where little to no observational data were available before GMOS. This work presents atmospheric Hg concentrations recorded worldwide, analyzing Hg measurement results in terms of temporal trends, seasonality and comparability within the network. Major findings highlighted a clear gradient of atmospheric Hg concentrations between the Northern and Southern Hemispheres, confirming that the gradient observed is mostly driven by local and regional sources, which can be anthropogenic, natural or a combination of both. In order to understand the atmospheric cycling and seasonal depositional characteristics of Hg, wet deposition samples were also collected at 17 selected GMOS monitoring sites providing new insight into baseline concentrations of THg concentrations in precipitation particularly in regions, such as the Southern Hemisphere and Tropical areas where wet deposition were never investigated before, opening the way for additional measurements across the GMOS network and new findings in future modeling studies highlighting the need of integrated measurements in ambient air and rainwater samples to improve our understanding of deposition processes and oxidation mechanisms. These new observations in fact, give scientists and modelers some insight into baseline concentrations of Hg concentrations in air and precipitation with the overarching benefit which clearly consists in the advancement of knowledge about Hg processes on global scale.

Published
2017

43. Long-term NOx measurements in the remote marine tropical troposphere.

Author

Andersen, Simone T., Carpenter, Lucy J., Nelson, Beth S., Neves, Luis, Read, Katie A., Reed, Chris, Ward, Martyn, Rowlinson, Matthew J., and Lee, James D.

Subjects
ATMOSPHERIC nitrogen oxides, LIGHT emitting diodes, TROPOSPHERIC aerosols, TROPOSPHERE, TROPOSPHERIC chemistry, NITROGEN dioxide, TIME series analysis
Abstract

Atmospheric nitrogen oxides (NO + NO2 = NO x) have been measured at the Cape Verde Atmospheric Observatory (CVAO) in the tropical Atlantic (16° 51' N, 24° 52' W) since October 2006. These measurements represent a unique time series of NOx in the background remote troposphere. Nitrogen dioxide (NO2) is measured via photolytic conversion to nitric oxide (NO) by ultra violet light emitting diode arrays followed by chemiluminescence detection. Since the measurements began, a blue light converter (BLC) has been used for NO2 photolysis, with a maximum spectral output of 395 nm from 2006-2015 and of 385 nm from 2015. The original BLC used was constructed with a Teflon-like material and appeared to cause an overestimation of NO2 when illuminated. To avoid such interferences, a new additional photolytic converter (PLC) with a quartz photolysis cell (maximum spectral output also 385 nm) was implemented in March 2017. Once corrections are made for the NO2 artefact from the original BLC, the two NO2 converters are shown to give comparable NO2 mixing ratios (PLC = 0.92 x BLC, R2 = 0.92), giving confidence in the quantitative measurement of NOx at very low levels. Data analysis methods for the NOx measurements made at CVAO have been developed and applied to the entire time series to produce an internally consistent and high quality long-term data set. NO has a clear diurnal pattern with a maximum mixing ratio of 2-10 pptV during the day depending on the season and ~0 pptV during the night. NO2 shows a fairly flat diurnal signal, although a small increase in daytime NOx is evident in some months. Monthly average mixing ratios of NO2 vary between 5 and 30 pptV depending on the season. Clear seasonal trends in NO and NO2 levels can be observed with a maximum in autumn/winter and a minimum in spring/summer. [ABSTRACT FROM AUTHOR]

Published
2020
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44. Recent multivariate changes in the North Atlantic climate system, with a focus on 2005–2016

Author

Robson, Jon, primary, Sutton, Rowan T., additional, Archibald, Alex, additional, Cooper, Fenwick, additional, Christensen, Matthew, additional, Gray, Lesley J., additional, Holliday, N. Penny, additional, Macintosh, Claire, additional, McMillan, Malcolm, additional, Moat, Ben, additional, Russo, Maria, additional, Tilling, Rachel, additional, Carslaw, Ken, additional, Desbruyères, Damien, additional, Embury, Owen, additional, Feltham, Daniel L., additional, Grosvenor, Daniel P., additional, Josey, Simon, additional, King, Brian, additional, Lewis, Alastair, additional, McCarthy, Gerard D., additional, Merchant, Chris, additional, New, Adrian L., additional, O'Reilly, Christopher H., additional, Osprey, Scott M., additional, Read, Katie, additional, Scaife, Adam, additional, Shepherd, Andrew, additional, Sinha, Bablu, additional, Smeed, David, additional, Smith, Doug, additional, Ridout, Andrew, additional, Woollings, Tim, additional, and Yang, Mingxi, additional

Published
2018
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45. Global impact of nitrate photolysis in sea-salt aerosol on NO&lt;sub&gt;&lt;i&gt;x&lt;/i&gt;&lt;/sub&gt;, OH, and O&lt;sub&gt;3&lt;/sub&gt; in the marine boundary layer

Author

Kasibhatla, Prasad, primary, Sherwen, Tomás, additional, Evans, Mathew J., additional, Carpenter, Lucy J., additional, Reed, Chris, additional, Alexander, Becky, additional, Chen, Qianjie, additional, Sulprizio, Melissa P., additional, Lee, James D., additional, Read, Katie A., additional, Bloss, William, additional, Crilley, Leigh R., additional, Keene, William C., additional, Pszenny, Alexander A. P., additional, and Hodzic, Alma, additional

Published
2018
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46. Supplementary material to "Global impact of nitrate photolysis in sea-salt aerosol on NOx, OH, and O3 in the marine boundary layer"

Author

Kasibhatla, Prasad, primary, Sherwen, Tomás, additional, Evans, Mathew J., additional, Carpenter, Lucy J., additional, Reed, Chris, additional, Alexander, Becky, additional, Chen, Qianjie, additional, Sulprizio, Melissa, additional, Lee, James D., additional, Read, Katie A., additional, Bloss, William, additional, Crilley, Leigh R., additional, Keene, William C., additional, Pszenny, Alex A. P., additional, and Hodzic, Alma, additional

Published
2018
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47. Impacts of bromine and iodine chemistry on tropospheric OH and HO&lt;sub&gt;2&lt;/sub&gt;: comparing observations with box and global model perspectives

Author

Stone, Daniel, primary, Sherwen, Tomás, additional, Evans, Mathew J., additional, Vaughan, Stewart, additional, Ingham, Trevor, additional, Whalley, Lisa K., additional, Edwards, Peter M., additional, Read, Katie A., additional, Lee, James D., additional, Moller, Sarah J., additional, Carpenter, Lucy J., additional, Lewis, Alastair C., additional, and Heard, Dwayne E., additional

Published
2018
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48. Multi-model study of mercury dispersion in the atmosphere: atmospheric processes and model evaluation

Author

Travnikov, Oleg, Angot, Helene, Artaxo, Paulo, Bencardino, Mariantonia, Bieser, Johannes, D'Amore, Francesco, Dastoor, Ashu, De Simone, Francesco, Diéguez, María del Carmen, Dommergue, Aurélien, Ebinghaus, Ralf, Feng, Xin Bin, Gencarelli, Christian N., Hedgecock, Ian M., Magand, Olivier, Martin, Lynwill, Matthias, Volker, Mashyanov, Nikolay, Pirrone, Nicola, Ramachandran, Ramesh, Read, Katie Alana, Ryjkov, Andrei, Selin, Noelle E., Sena, Fabrizio, Song, Shaojie, Sprovieri, Francesca, Wip, Dennis, Wängberg, Ingvar, Yang, Xin, Travnikov, Oleg, Angot, Helene, Artaxo, Paulo, Bencardino, Mariantonia, Bieser, Johannes, D'Amore, Francesco, Dastoor, Ashu, De Simone, Francesco, Diéguez, María del Carmen, Dommergue, Aurélien, Ebinghaus, Ralf, Feng, Xin Bin, Gencarelli, Christian N., Hedgecock, Ian M., Magand, Olivier, Martin, Lynwill, Matthias, Volker, Mashyanov, Nikolay, Pirrone, Nicola, Ramachandran, Ramesh, Read, Katie Alana, Ryjkov, Andrei, Selin, Noelle E., Sena, Fabrizio, Song, Shaojie, Sprovieri, Francesca, Wip, Dennis, Wängberg, Ingvar, and Yang, Xin

Abstract

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

Published
2017

49. Four years (2011-2015) of total gaseous mercury and other key measurements from the Cape Verde Atmospheric Observatory (CVAO)

Author

Read, Katie, Kentisbeer, John, Neves, Luis, Carpenter, Lucy, Read, Katie, Kentisbeer, John, Neves, Luis, and Carpenter, Lucy

Abstract

The Global GAW Cape Verde Atmospheric Observatory (CVAO) –Humberto Duarte Fonseca is situated in Calhau on the island of São Vicente in Cape Verde (16.848°N, 24.871°W). Measurements were started in October 2006 to further our understanding of atmospheric chemistry within the tropical marine boundary layer. Funding for the UK trace gases is through the Atmospheric Measurement Facility (AMF) which is a subsidiary of NCAS (NaTonal Centre for Atmospheric Science) in the UK. Our partners on the CVAO project are the InsTtuto Naçional de Meteorologia and GeoXsca (INMG), Cape Verde, the Max-Planck InsTtut für Biogeochemie, Germany, and the Leibniz-InsTtut für Troposphärenforschung, Germany (TROPOS). Here we present our Total Gaseous Mercury (TGM) measurements along with some other trace gas measurements from the CVAO.

Published
2017

50. Multi-model study of mercury dispersion in the atmosphere: atmospheric processes and model evaluation

Author

Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences, Selin, Noelle E, Song, Shaojie, Travnikov, Oleg, Angot, Hélène, Artaxo, Paulo, Bencardino, Mariantonia, Bieser, Johannes, D'Amore, Francesco, Dastoor, Ashu, De Simone, Francesco, Diéguez, María del Carmen, Dommergue, Aurélien, Ebinghaus, Ralf, Feng, Xin Bin, Gencarelli, Christian N., Hedgecock, Ian M., Magand, Olivier, Martin, Lynwill, Matthias, Volker, Mashyanov, Nikolay, Pirrone, Nicola, Ramachandran, Ramesh, Read, Katie Alana, Ryjkov, Andrei, Sena, Fabrizio, Sprovieri, Francesca, Wip, Dennis, Wängberg, Ingvar, Yang, Xin, Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences, Selin, Noelle E, Song, Shaojie, Travnikov, Oleg, Angot, Hélène, Artaxo, Paulo, Bencardino, Mariantonia, Bieser, Johannes, D'Amore, Francesco, Dastoor, Ashu, De Simone, Francesco, Diéguez, María del Carmen, Dommergue, Aurélien, Ebinghaus, Ralf, Feng, Xin Bin, Gencarelli, Christian N., Hedgecock, Ian M., Magand, Olivier, Martin, Lynwill, Matthias, Volker, Mashyanov, Nikolay, Pirrone, Nicola, Ramachandran, Ramesh, Read, Katie Alana, Ryjkov, Andrei, Sena, Fabrizio, Sprovieri, Francesca, Wip, Dennis, Wängberg, Ingvar, and Yang, Xin

Abstract

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

Published
2017

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