2023, Royer, Haley M., Pöhlker, Mira L., Krüger, Ovid, Blades, Edmund, Sealy, Peter, Lata, Nurun Nahar, Cheng, Zezhen, China, Swarup, Ault, Andrew P., Quinn, Patricia K., Zuidema, Paquita, Pöhlker, Christopher, Pöschl, Ulrich, Andreae, Meinrat, Gaston, Cassandra J.

The number concentration and properties of aerosol particles serving as cloud condensation nuclei (CCN) are important for understanding cloud properties, including in the tropical Atlantic marine boundary layer (MBL), where marine cumulus clouds reflect incoming solar radiation and obscure the low-albedo ocean surface. Studies linking aerosol source, composition, and water uptake properties in this region have been conducted primarily during the summertime dust transport season, despite the region receiving a variety of aerosol particle types throughout the year. In this study, we compare size-resolved aerosol chemical composition data to the hygroscopicity parameter κ derived from size-resolved CCN measurements made during the Elucidating the Role of Clouds-Circulation Coupling in Climate (EUREC4A) and Atlantic Tradewind Ocean-Atmosphere Mesoscale Interaction Campaign (ATOMIC) campaigns from January to February 2020. We observed unexpected periods of wintertime long-range transport of African smoke and dust to Barbados. During these periods, the accumulation-mode aerosol particle and CCN number concentrations as well as the proportions of dust and smoke particles increased, whereas the average κ slightly decreased (κCombining double low line0.46±0.10) from marine background conditions (κCombining double low line0.52±0.09) when the submicron particles were mostly composed of marine organics and sulfate. Size-resolved chemical analysis shows that smoke particles were the major contributor to the accumulation mode during long-range transport events, indicating that smoke is mainly responsible for the observed increase in CCN number concentrations. Earlier studies conducted at Barbados have mostly focused on the role of dust on CCN, but our results show that aerosol hygroscopicity and CCN number concentrations during wintertime long-range transport events over the tropical North Atlantic are also affected by African smoke. Our findings highlight the importance of African smoke for atmospheric processes and cloud formation over the Caribbean.

2021, Stevens, Bjorn, Bony, Sandrine, Farrell, David, Ament, Felix, Blyth, Alan, Fairall, Christopher, Karstensen, Johannes, Quinn, Patricia K., Speich, Sabrina, Acquistapace, Claudia, Aemisegger, Franziska, Crewell, Susanne, Cronin, Timothy, Cui, Zhiqiang, Cuypers, Yannis, Daley, Alton, Damerell, Gillian M., Dauhut, Thibaut, Deneke, Hartwig, Desbios, Jean-Philippe, Dörner, Steffen, Albright, Anna Lea, Donner, Sebastian, Douet, Vincent, Drushka, Kyla, Dütsch, Marina, Ehrlich, André, Emanuel, Kerry, Emmanouilidis, Alexandros, Etienne, Jean-Claude, Etienne-Leblanc, Sheryl, Faure, Ghislain, Bellenger, Hugo, Feingold, Graham, Ferrero, Luca, Fix, Andreas, Flamant, Cyrille, Flatau, Piotr Jacek, Foltz, Gregory R., Forster, Linda, Furtuna, Iulian, Gadian, Alan, Galewsky, Joseph, Bodenschatz, Eberhard, Gallagher, Martin, Gallimore, Peter, Gaston, Cassandra, Gentemann, Chelle, Geyskens, Nicolas, Giez, Andreas, Gollop, John, Gouirand, Isabelle, Gourbeyre, Christophe, de Graaf, Dörte, Caesar, Kathy-Ann, de Groot, Geiske E., Grosz, Robert, Güttler, Johannes, Gutleben, Manuel, Hall, Kashawn, Harris, George, Helfer, Kevin C., Henze, Dean, Herbert, Calvert, Holanda, Bruna, Chewitt-Lucas, Rebecca, Ibanez-Landeta, Antonio, Intrieri, Janet, Iyer, Suneil, Julien, Fabrice, Kalesse, Heike, Kazil, Jan, Kellman, Alexander, Kidane, Abiel T., Kirchner, Ulrike, Klingebiel, Marcus, de Boer, Gijs, Körner, Mareike, Kremper, Leslie Ann, Kretzschmar, Jan, Krüger, Ovid, Kumala, Wojciech, Kurz, Armin, L'Hégaret, Pierre, Labaste, Matthieu, Lachlan-Cope, Tom, Laing, Arlene, Delanoë, Julien, Landschützer, Peter, Lang, Theresa, Lange, Diego, Lange, Ingo, Laplace, Clément, Lavik, Gauke, Laxenaire, Rémi, Le Bihan, Caroline, Leandro, Mason, Lefevre, Nathalie, Denby, Leif, Lena, Marius, Lenschow, Donald, Li, Qiang, Lloyd, Gary, Los, Sebastian, Losi, Niccolò, Lovell, Oscar, Luneau, Christopher, Makuch, Przemyslaw, Malinowski, Szymon, Ewald, Florian, Manta, Gaston, Marinou, Eleni, Marsden, Nicholas, Masson, Sebastien, Maury, Nicolas, Mayer, Bernhard, Mayers-Als, Margarette, Mazel, Christophe, McGeary, Wayne, McWilliams, James C., Fildier, Benjamin, Mech, Mario, Mehlmann, Melina, Meroni, Agostino Niyonkuru, Mieslinger, Theresa, Minikin, Andreas, Minnett, Peter, Möller, Gregor, Morfa Avalos, Yanmichel, Muller, Caroline, Musat, Ionela, Forde, Marvin, Napoli, Anna, Neuberger, Almuth, Noisel, Christophe, Noone, David, Nordsiek, Freja, Nowak, Jakub L., Oswald, Lothar, Parker, Douglas J., Peck, Carolyn, Person, Renaud, George, Geet, Philippi, Miriam, Plueddemann, Albert, Pöhlker, Christopher, Pörtge, Veronika, Pöschl, Ulrich, Pologne, Lawrence, Posyniak, Michał, Prange, Marc, Quiñones Meléndez, Estefanía, Radtke, Jule, Gross, Silke, Ramage, Karim, Reimann, Jens, Renault, Lionel, Reus, Klaus, Reyes, Ashford, Ribbe, Joachim, Ringel, Maximilian, Ritschel, Markus, Rocha, Cesar B., Rochetin, Nicolas, Hagen, Martin, Röttenbacher, Johannes, Rollo, Callum, Royer, Haley, Sadoulet, Pauline, Saffin, Leo, Sandiford, Sanola, Sandu, Irina, Schäfer, Michael, Schemann, Vera, Schirmacher, Imke, Hausold, Andrea, Schlenczek, Oliver, Schmidt, Jerome, Schröder, Marcel, Schwarzenboeck, Alfons, Sealy, Andrea, Senff, Christoph J., Serikov, Ilya, Shohan, Samkeyat, Siddle, Elizabeth, Smirnov, Alexander, Heywood, Karen J., Späth, Florian, Spooner, Branden, Stolla, M. Katharina, Szkółka, Wojciech, de Szoeke, Simon P., Tarot, Stéphane, Tetoni, Eleni, Thompson, Elizabeth, Thomson, Jim, Tomassini, Lorenzo, Hirsch, Lutz, Totems, Julien, Ubele, Alma Anna, Villiger, Leonie, von Arx, Jan, Wagner, Thomas, Walther, Andi, Webber, Ben, Wendisch, Manfred, Whitehall, Shanice, Wiltshire, Anton, Jacob, Marek, Wing, Allison A., Wirth, Martin, Wiskandt, Jonathan, Wolf, Kevin, Worbes, Ludwig, Wright, Ethan, Wulfmeyer, Volker, Young, Shanea, Zhang, Chidong, Zhang, Dongxiao, Jansen, Friedhelm, Ziemen, Florian, Zinner, Tobias, Zöger, Martin, Kinne, Stefan, Klocke, Daniel, Kölling, Tobias, Konow, Heike, Lothon, Marie, Mohr, Wiebke, Naumann, Ann Kristin, Nuijens, Louise, Olivier, Léa, Pincus, Robert, Pöhlker, Mira, Reverdin, Gilles, Roberts, Gregory, Schnitt, Sabrina, Schulz, Hauke, Siebesma, A. Pier, Stephan, Claudia Christine, Sullivan, Peter, Touzé-Peiffer, Ludovic, Vial, Jessica, Vogel, Raphaela, Zuidema, Paquita, Alexander, Nicola, Alves, Lyndon, Arixi, Sophian, Asmath, Hamish, Bagheri, Gholamhossein, Baier, Katharina, Bailey, Adriana, Baranowski, Dariusz, Baron, Alexandre, Barrau, Sébastien, Barrett, Paul A., Batier, Frédéric, Behrendt, Andreas, Bendinger, Arne, Beucher, Florent, Bigorre, Sebastien, Blades, Edmund, Blossey, Peter, Bock, Olivier, Böing, Steven, Bosser, Pierre, Bourras, Denis, Bouruet-Aubertot, Pascale, Bower, Keith, Branellec, Pierre, Branger, Hubert, Brennek, Michal, Brewer, Alan, Brilouet, Pierre-Etienne, Brügmann, Björn, Buehler, Stefan A., Burke, Elmo, Burton, Ralph, Calmer, Radiance, Canonici, Jean-Christophe, Carton, Xavier, Cato Jr., Gregory, Charles, Jude Andre, Chazette, Patrick, Chen, Yanxu, Chilinski, Michal T., Choularton, Thomas, Chuang, Patrick, Clarke, Shamal, Coe, Hugh, Cornet, Céline, Coutris, Pierre, Couvreux, Fleur

The science guiding the EUREC4A campaign and its measurements is presented. EUREC4A comprised roughly 5 weeks of measurements in the downstream winter trades of the North Atlantic – eastward and southeastward of Barbados. Through its ability to characterize processes operating across a wide range of scales, EUREC4A marked a turning point in our ability to observationally study factors influencing clouds in the trades, how they will respond to warming, and their link to other components of the earth system, such as upper-ocean processes or the life cycle of particulate matter. This characterization was made possible by thousands (2500) of sondes distributed to measure circulations on meso- (200 km) and larger (500 km) scales, roughly 400 h of flight time by four heavily instrumented research aircraft; four global-class research vessels; an advanced ground-based cloud observatory; scores of autonomous observing platforms operating in the upper ocean (nearly 10 000 profiles), lower atmosphere (continuous profiling), and along the air–sea interface; a network of water stable isotopologue measurements; targeted tasking of satellite remote sensing; and modeling with a new generation of weather and climate models. In addition to providing an outline of the novel measurements and their composition into a unified and coordinated campaign, the six distinct scientific facets that EUREC4A explored – from North Brazil Current rings to turbulence-induced clustering of cloud droplets and its influence on warm-rain formation – are presented along with an overview of EUREC4A's outreach activities, environmental impact, and guidelines for scientific practice. Track data for all platforms are standardized and accessible at https://doi.org/10.25326/165 (Stevens, 2021), and a film documenting the campaign is provided as a video supplement.

2017, Engel, Anja, Bange, Hermann W., Cunliffe, Michael, Burrows, Susannah M., Friedrichs, Gernot, Galgani, Luisa, Herrmann, Hartmut, Hertkorn, Norbert, Johnson, Martin, Liss, Peter S., Quinn, Patricia K., Schartau, Markus, Soloviev, Alexander, Stolle, Christian, Upstill-Goddard, Robert C., van Pinxteren, Manuela, Zäncker, Birthe

Despite the huge extent of the ocean's surface, until now relatively little attention has been paid to the sea surface microlayer (SML) as the ultimate interface where heat, momentum and mass exchange between the ocean and the atmosphere takes place. Via the SML, large-scale environmental changes in the ocean such as warming, acidification, deoxygenation, and eutrophication potentially influence cloud formation, precipitation, and the global radiation balance. Due to the deep connectivity between biological, chemical, and physical processes, studies of the SML may reveal multiple sensitivities to global and regional changes. Understanding the processes at the ocean's surface, in particular involving the SML as an important and determinant interface, could therefore provide an essential contribution to the reduction of uncertainties regarding ocean-climate feedbacks. This review identifies gaps in our current knowledge of the SML and highlights a need to develop a holistic and mechanistic understanding of the diverse biological, chemical, and physical processes occurring at the ocean-atmosphere interface. We advocate the development of strong interdisciplinary expertise and collaboration in order to bridge between ocean and atmospheric sciences. Although this will pose significant methodological challenges, such an initiative would represent a new role model for interdisciplinary research in Earth System sciences.

2016, Bates, Timothy S., Quinn, Patricia K., Covert, David S., Coffman, Derek J., Johnson, James E., Wiedensohler, Alfred

The goals of the IGAC Aerosol Characterization Experiments (ACE) are to determine and understand the properties and controlling processes of the aerosol in a globally representative range of natural and anthropogenically perturbed environments. ACE-1 was conducted in the remote marine atmosphere south of Australia while ACE-2 was conducted in the anthropogenically modified atmosphere of the Eastern North Atlantic. In-situ shipboard measurements from the RV Discoverer(ACE-1) and the RV Professor Vodyanitskiy(ACE-2), combined with calculated back trajectories can be used to define the physical properties of the sub-micron aerosol in marine boundary layer (MBL) air masses from the remote Southern Ocean, Western Europe, the Iberian coast, the Mediterranean and the background Atlantic Ocean. The differences in these aerosol properties, combined with dimethylsulfide, sulfur dioxide and meteorological measurements provide a means to assess processes that affect the aerosol distribution. The background sub-micron aerosol measured over the Atlantic Ocean during ACE-2 was more abundant (number and volume) and appeared to be more aged than that measured over the Southern Ocean during ACE-1. Based on seawater DMS measurements and wind speed, the oceanic source of non-sea-salt sulfur and sea-salt to the background marine atmosphere during ACE-1 and ACE-2 was similar. However, the synoptic meteorological pattern was quite different during ACE-1 and ACE-2. The frequent frontal passages during ACE-1 resulted in the mixing of nucleation mode particles into the marine boundary layer from the free troposphere and relatively short aerosol residence times. In the more stable meteorological setting of ACE-2, a significant nucleation mode aerosol was observed in the MBL only for a half day period associated with a weak frontal system. As a result of the longer MBL aerosol residence times, the average background ACE-2 accumulation mode aerosol had a larger diameter and higher number concentration than during ACE-1. The sub-micron aerosol number size distributions in the air masses that passed over Western Europe, the Mediterranean, and coastal Portugal were distinctly different from each other and the background aerosol. The differences can be attributed to the age of the air mass and the degree of cloud processing.

2018, Benedetti, Angela, Reid, Jeffrey S., Knippertz, Peter, Marsham, John H., Di Giuseppe, Francesca, Rémy, Samuel, Basart, Sara, Boucher, Olivier, Brooks, Ian M., Menut, Laurent, Mona, Lucia, Laj, Paolo, Pappalardo, Gelsomina, Wiedensohler, Alfred, Baklanov, Alexander, Brooks, Malcolm, Colarco, Peter R., Cuevas, Emilio, da Silva, Arlindo, Escribano, Jeronimo, Flemming, Johannes, Huneeus, Nicolas, Jorba, Oriol, Kazadzis, Stelios, Kinne, Stefan, Popp, Thomas, Quinn, Patricia K., Sekiyama, Thomas T., Tanaka, Taichu, Terradellas, Enric

Numerical prediction of aerosol particle properties has become an important activity at many research and operational weather centers. This development is due to growing interest from a diverse set of stakeholders, such as air quality regulatory bodies, aviation and military authorities, solar energy plant managers, climate services providers, and health professionals. Owing to the complexity of atmospheric aerosol processes and their sensitivity to the underlying meteorological conditions, the prediction of aerosol particle concentrations and properties in the numerical weather prediction (NWP) framework faces a number of challenges. The modeling of numerous aerosol-related parameters increases computational expense. Errors in aerosol prediction concern all processes involved in the aerosol life cycle including (a) errors on the source terms (for both anthropogenic and natural emissions), (b) errors directly dependent on the meteorology (e.g., mixing, transport, scavenging by precipitation), and (c) errors related to aerosol chemistry (e.g., nucleation, gas-aerosol partitioning, chemical transformation and growth, hygroscopicity). Finally, there are fundamental uncertainties and significant processing overhead in the diverse observations used for verification and assimilation within these systems. Indeed, a significant component of aerosol forecast development consists in streamlining aerosol-related observations and reducing the most important errors through model development and data assimilation. Aerosol particle observations from satellite- and ground-based platforms have been crucial to guide model development of the recent years and have been made more readily available for model evaluation and assimilation. However, for the sustainability of the aerosol particle prediction activities around the globe, it is crucial that quality aerosol observations continue to be made available from different platforms (space, near surface, and aircraft) and freely shared. This paper reviews current requirements for aerosol observations in the context of the operational activities carried out at various global and regional centers. While some of the requirements are equally applicable to aerosol-climate, the focus here is on global operational prediction of aerosol properties such as mass concentrations and optical parameters. It is also recognized that the term "requirements" is loosely used here given the diversity in global aerosol observing systems and that utilized data are typically not from operational sources. Most operational models are based on bulk schemes that do not predict the size distribution of the aerosol particles. Others are based on a mix of "bin" and bulk schemes with limited capability of simulating the size information. However the next generation of aerosol operational models will output both mass and number density concentration to provide a more complete description of the aerosol population. A brief overview of the state of the art is provided with an introduction on the importance of aerosol prediction activities. The criteria on which the requirements for aerosol observations are based are also outlined. Assimilation and evaluation aspects are discussed from the perspective of the user requirements.

2016, Johnson, Doug W., Osborne, Simon, Wood, Robert, Suhre, Karsten, Johnson, Randy, Businger, Steven, Quinn, Patricia K., Wiedensohler, Alfred, Durkee, Philip A., Russell, Lynn M., Andreae, Meinrat O., O’Dowd, Colin, Noone, Kevin J., Bandy, Brian, Rudolph, J., Rapsomanikis, Spyros

One of the primary aims of the North Atlantic regional Aerosol Characterisation Experiment (ACE-2) was to quantify the physical and chemical processes affecting the evolution of the major aerosol types over the North Atlantic. The best, practical way of doing this is in a Lagrangian framework where a parcel of air is sampled over several tens of hours and its physical and chemical properties are intensively measured. During the intensive observational phase of ACE-2, between 15 June 1997 and 24 July 1997, 3 cloudy Lagrangian experiments and 3 cloud-free, Lagrangian experiments were undertaken between the south west tip of the Iberian Peninsula and the Canary Islands. This paper gives an overview of the aims and logistics of all of the Lagrangian experiments and compares and contrasts them to provide a framework for the more focused Lagrangian papers in this issue and future process modelling studies and parametrisation development. The characteristics of the cloudy Lagrangian experiments were remarkably different, enabling a wide range of different physical and chemical processes to be studied. In the 1st Lagrangian, a clean maritime air mass was sampled in which salt particle production, due to increased wind speed, dominated the change in the accumulation mode concentrations. In the 2nd Lagrangian, extensive cloud cover resulted in cloud processing of the aerosol in a polluted air mass, and entrainment of air from the free troposphere influenced the overall decrease in aerosol concentrations in the marine boundary layer (MBL). Very little change in aerosol characteristics was measured in the 3rd Lagrangian, where the pollution in the MBL was continually being topped up by entraining air from a residual continental boundary layer (CBL) above. From the analysis of all the Lagrangian experiments, it has been possible to formulate, and present here, a generalised description of a European continental outbreak of pollution over the sub-tropical North Atlantic.