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La ; Rocca, P. La ; Lai, Yue Shi ; Langoy, Rune ; Lapidus, Kirill ; Lardeux, Antoine Xavier ; Larionov, Pavel ; Laudi, Elisa ; Lavicka, Roman ; Lazareva, Tatiana V. ; Lea, Ramona ; Leardini, Lucia ; Lee, S. ; Lehas, Fatiha ; Lehner, Sebastian ; Lehrbach, Johannes ; Lemmon, Roy Crawford ; Monzón, I. León ; Lévai, Péter ; Li, X. ; Li, Xing Long ; Lien, Jørgen André ; Lietava, Roman ; Lim, Bong-Hwi ; Lindal, Svein ; Lindenstruth, Volker ; Lindsay, Scott William ; Lippmann, Christian ; Lisa, Michael A. ; Litichevskyi, Vladyslav ; Liu, Alwina Ruixin ; Ljunggren, Hans Martin ; Llope, William Joseph ; Lodato, Davide Francesco ; Loginov, Vitaly ; Loizides, Constantinos ; Lončar, Petra ; Lopez, Xavier Bernard ; Torres, E. 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Martinez ; Masciocchi, Silvia ; Masera, Massimo ; Masoni, Alberto ; Massacrier, Laure Marie ; Masson, Erwann ; Mastroserio, Annalisa ; Mathis, Andreas Michael ; Matuoka, Paula Fernanda Toledo ; Matyja, Adam Tomasz ; Mayer, Christoph ; Mazzilli, Marianna ; Mazzoni, Alessandra Maria ; Meddi, Franco ; Melikyan, Yury ; Menchaca-Rocha, Arturo Alejandro ; Meninno, Elisa ; Meres, Michal ; Mhlanga, Sibaliso ; Miake, Yasuo ; Micheletti, Luca ; Mieskolainen, Matti Mikael ; Mihaylov, Dimitar Lubomirov ; Mikhaylov, Konstantin ; Mischke, André ; Mishra, Aditya Nath ; Miśkowiec, Dariusz Czesław ; Mitu, Ciprian Mihai ; Mohammadi, Naghmeh ; Mohanty, Auro Prasad ; Mohanty, Bedangadas ; Khan, M. Mohisin ; Mondal, Mriganka Mouli ; Mordasini, Cindy ; Godoy, D.A. Moreira De ; Perez Moreno, Luis Alberto ; Moretto, Sandra ; Morreale, Astrid ; Morsch, Andreas ; Mrnjavac, Teo ; Muccifora, Valeria ; Mudnic, Eugen ; Mühlheim, Daniel ; Muhuri, Sanjib ; Mukherjee, Maitreyee ; Mulligan, James Declan ; Munhoz, Marcelo Gameiro ; Münning, Konstantin ; Munzer, Robert Helmut ; Murakami, Hikari ; Murray, Sean ; Musa, Luciano ; Musinsky, Jan ; Myers, Corey James ; Myrcha, Julian Wojciech ; Naik, Bharati ; Nair, Rahul Ramachandran ; Nandi, Basanta Kumar ; Nania, Rosario ; Nappi, Eugenio ; Naru, Muhammad Umair ; Nassirpour, Adrian Fereydon ; Luz, H. Natal da ; Nattrass, Christine ; Rosado Navarro, Sebastian ; Nayak, Kishora ; Nayak, Ranjit ; Nayak, Tapan Kumar ; Nazarenko, Sergey ; Oliveira, R.A. Negrao De ; Nellen, Lukas ; Nesbo, Simon Voigt ; Nešković, Gvozden ; Ng, Fabian ; Nielsen, Borge Svane ; Nikolaev, Sergey ; Nikulin, Sergey ; Nikulin, Vladimir ; Noferini, Francesco ; Nomokonov, Petr V. ; Nooren, Gerardus ; Cabanillas Noris, Juan Carlos ; Norman, Jaime ; Nyanin, Alexander ; Nystrand, Joakim Ingemar ; Ogino, Masanori ; Ohlson, Alice ; Oleniacz, Janusz ; Silva, A.C. Oliveira Da ; Oliver, Michael Henry ; Onderwaater, Jacobus ; Oppedisano, Chiara ; Orava, Risto ; Velasquez, A. Ortiz ; Oskarsson, Anders Nils Erik ; Otwinowski, Jacek Tomasz ; Oyama, Ken ; Pachmayer, Yvonne C. ; Pacik, Vojtěch ; Pagano, Davide ; Paić, Guy ; Palni, Prabhakar ; Pan, Jinjin ; Pandey, Ashutosh Kumar ; Panebianco, Stefano Matthias ; Papikyan, Vardanush ; Pareek, Pooja ; Park, Jonghan ; Parkkila, Jasper Elias ; Parmar, Sonia ; Passfeld, Annika ; Pathak, Surya Prakash ; Patra, Rajendra Nath ; Paul, Biswarup ; Pei, Hua ; Peitzmann, Thomas ; Peng, Xinye ; Pereira, Luis Gustavo ; Costa, H. Pereira Da ; Peresunko, Dmitry Yurevich ; Mesa Perez, Guillermo ; Lezama, E. Perez ; Peskov, Vladimir ; Pestov, Yury N. ; Petráček, Vojtech ; Petrovici, Mihai A. ; Pezzi, Rafael Peretti ; Piano, Stefano ; Pikna, Miroslav ; Pillot, Philippe ; Ozelin de Lima Pimentel, Laís ; Pinazza, Ombretta ; Pinsky, Lawrence ; Pisano, Silvia ; Piyarathna, Danthasinghe B. ; Płoskoń, Mateusz ; Planinic, Mirko ; Pliquett, Fabian ; Pluta, Jan Marian ; Pochybova, Sona ; Podesta Lerma, Pedro Luis Manuel ; Poghosyan, Martin G. ; Polichtchouk, Boris ; Poljak, Nikola ; Poonsawat, Wanchaloem ; Pop, Amalia ; Poppenborg, Hendrik ; Porteboeuf-Houssais, Sarah Julie ; Pozdniakov, Valeriy ; Prasad, Sidharth Kumar ; Preghenella, Roberto ; Prino, Francesco ; Pruneau, Claude A. ; Pshenichnov, Igor A. ; Puccio, Maximiliano ; Punin, Valery ; Puranapanda, Kalyana ; Putschke, Jörn H. ; Quishpe, Raquel Estefania ; Ragoni, Simone ; Raha, Sibaji ; Rajput, Sonia ; Rak, Jan ; Rakotozafindrabe, Andry Malala ; Ramello, Luciano ; Rami, Fouad ; Raniwala, Rashmi ; Raniwala, Sudhir ; Räsänen, Sami Sakari ; Rascanu, Bogdan Theodor ; Rath, Rutuparna ; Ratza, Viktor ; Ravasenga, Ivan ; Read, Kenneth Francis ; Redlich, Krzysztof ; Rehman, Attiq ur ; Reichelt, Patrick ; Reidt, Felix ; Ren, Xiaowen ; Renfordt, Rainer Arno Ernst ; Reshetin, Andrey ; Revol, Jean-Pierre ; Reygers, Klaus ; Riabov, Viktor G. ; Richert, Tuva Ora Herenui ; Richter, Matthias ; Riedler, Petra ; Riegler, Werner ; Riggi, Francesco ; Ristea, Cătălin-Lucian ; Rode, Sudhir Pandurang ; Cahuantzi, M. Rodríguez ; Røed, Ketil ; Rogalev, Roman ; Rogochaya, Elena ; Rohr, David ; Röhrich, Dieter ; Rokita, Przemyslaw Stefan ; Ronchetti, Federico ; Dominguez Rosas, Edgar ; Rosłon, Krystian ; Rosnet, Philippe ; Rossi, Andrea ; Rotondi, Alberto ; Roukoutakis, Filimon ; Roy, Ankhi ; Roy, Pradip Kumar ; Vazquez Rueda, Omar ; Rui, Rinaldo ; Rumyantsev, Boris ; Rustamov, Anar ; Ryabinkin, Evgeny ; Ryabov, Yury ; Rybicki, Andrzej ; Saarinen, Sampo ; Sadhu, Samrangy ; Sadovskiy, Sergey ; Šafařík, Karel ; Saha, Sumit Kumar ; Sahoo, Baidyanath ; Sahoo, Pragati ; Sahoo, Raghunath ; Sahoo, Sarita ; Sahu, Pradip Kumar ; Saini, Jogender ; Sakai, Shingo ; Sambyal, Sanjeev Singh ; Samsonov, Vladimir ; Sandoval, Andres ; Sarkar, Amal ; Sarkar, Debojit ; Sarkar, Nachiketa ; Sarma, Pranjal ; Mantovani Sarti, Valentina ; Sas, Mike Henry Petrus ; Scapparone, Eugenio ; Schaefer, Brennan ; Schambach, Joachim ; Scheid, Horst Sebastian ; Schiaua, Claudiu Cornel ; Schicker, Rainer ; Schmah, Alexander ; Schmidt, Christian Joachim ; Schmidt, Hans Rudolf ; Schmidt, Marten Ole ; Schmidt, M. ; Schmidt, Nicolas ; Schmier, Austin Robert ; Schukraft, Jürgen ; Schutz, Yves Roland ; Schwarz, Kilian ; Schweda, Kai ; Scioli, Gilda ; Scomparin, Enrico ; Šefčík, Michal ; Seger, Janet Elizabeth ; Sekiguchi, Yuko ; Sekihata, Daiki ; Selyuzhenkov, Ilya ; Senyukov, Serhiy ; Serradilla, Eulogio ; Sett, Priyanka ; Sevcenco, Adrian ; Shabanov, Arseniy ; Shabetai, Alexandre ; Shahoyan, Ruben ; Shaikh, Wadut ; Shangaraev, Artem ; Sharma, A. ; Sharma, A. ; Sharma, M. ; Sharma, Natasha ; Sheikh, Ashik Ikbal ; Shigaki, Kenta ; Shimomura, Maya ; Shirinkin, Sergey ; Shou, Qiye ; Sibiriak, Yury ; Siddhanta, Sabyasachi ; Siemiarczuk, Teodor ; Silvermyr, David Olle Rickard ; Simatovic, Goran ; Simonetti, Giuseppe ; Singh, R. ; Singh, R. ; Singh, V.K. ; Singhal, Vikas ; Sarkar-Sinha, Tinku ; Sitar, Branislav ; Sitta, Mario ; Skaali, Toralf Bernhard ; Slupecki, Maciej ; Smirnov, Nikolai ; Snellings, Raimond ; Snellman, Tomas Wilhelm ; Sochan, Jaroslav ; Soncco Meza, Carlos ; Song, J. ; Songmoolnak, Arnon ; Soramel, Francesca ; Sorensen, Soren Pontoppidan ; Sozzi, Federica ; Sputowska, Iwona Anna ; Stachel, Johanna ; Stan, Ionel ; Stankus, Paul William ; Stenlund, Evert Anders ; Stocco, Diego ; Storetvedt, Maksim Melnik ; Strmen, Peter ; Suaide, Alexandre Alarcon do Passo ; Sugitate, Toru ; Suire, Christophe Pierre ; Suleymanov, Mais Kazim Oglu ; Šuljić, Miljenko ; Sultanov, Rishat ; Šumbera, Michal ; Sumowidagdo, Suharyo ; Suzuki, Ken ; Swain, Sagarika ; Szabo, Alexander ; Szarka, Imrich ; Tabassam, Uzma ; Takahashi, Jun ; Tambave, Ganesh ; Tanaka, Naoto ; Tang, S. ; Tarhini, Mohamad ; Tarzila, Madalina-Gabriela ; Tauro, Arturo ; Muñoz, G. Tejeda ; Telesca, Adriana ; Terrevoli, Cristina ; Thakur, Dhananjaya ; Thakur, Sanchari ; Thomas, Deepa ; Thoresen, Freja ; Tieulent, Raphael Noel ; Tikhonov, Anatoly ; Timmins, Anthony Robert ; Toia, Alberica ; Topilskaya, Nataliya ; Toppi, Marco ; Rojas Torres, Solangel ; Tripathy, Sushanta ; Tripathy, Tulika ; Trogolo, Stefano ; Trombetta, Giuseppe ; Tropp, Lukas ; Trubnikov, Victor ; Trzaska, Wladyslaw Henryk ; Trzcinski, Tomasz Piotr ; Trzeciak, Barbara Antonina ; Tsuji, Tomoya ; Tumkin, Alexandr ; Turrisi, Rosario ; Tveter, Trine Spedstad ; Ullaland, Kjetil ; Umaka, Ejiro Naomi ; Uras, Antonio ; Usai, Gianluca ; Utrobicic, Antonija ; Vala, Martin ; Palomo, L. Valencia ; Valle, Nicolò ; Kolk, Naomi van der ; Doremalen, Lennart Vincent Rogier van ; Hoorne, J.W. Van ; Leeuwen, Marco van ; Vyvre, P. Vande ; Varga, Dezsö ; Vargas Treviño, Maria Aurora Diozcora ; Vargyas, Márton ; Varma, Raghava ; Vasileiou, Maria ; Vasiliev, Andrey ; Doce, O. Vázquez ; Vechernin, Vladimir ; Veen, Annelies Marianne ; Vercellin, Ermanno ; Limón, S. Vergara ; Vermunt, Lucas Anne ; Vernet, Renaud ; Vértesi, Róbert ; Vicković, Linda ; Viinikainen, Jussi Samuli ; Vilakazi, Zabulon ; Baillie, O. Villalobos ; Tello, A. Villatoro ; Vino, Gioacchino ; Vinogradov, Alexander A. ; Virgili, Tiziano ; Vislavicius, Vytautas ; Vodopyanov, Alexander ; Völkel, Benedikt ; Völkl, Martin Andreas ; Voloshin, Kirill ; Voloshin, Sergei ; Volpe, Giacomo ; Haller, B. von ; Vorobyev, Ivan ; Voscek, Dominik ; Vrláková, Janka ; Wagner, Boris ; Wang, M. ; Watanabe, Yosuke ; Weber, Michael ; Weber, Steffen Georg ; Wegrzynek, Adami Tadeusz ; Weiser, Dennis ; Wenzel, Sandro Christian ; Wessels, Johannes P. ; Westerhoff, Uwe ; Whitehead, Andile Mothegi ; Widmann, Eberhard ; Wiechula, Jens ; Wikne, Jon ; Wilk, Grzegorz Andrzej ; Wilkinson, Jeremy ; Willems, Guido Alexander ; Willsher, Emily Jade ; Windelband, Bernd ; Witt, William Edward ; Wu, Y. ; Xu, Ran ; Yalcin, Serpil ; Yamakawa, Kosei ; Yang, S. ; Yano, Satoshi ; Yin, Zhongbao ; Yokoyama, Hiroki ; Yoo, In-Kwon ; Yoon, Jin-Hee ; Yuan, S. ; Yurchenko, Volodymyr ; Zaccolo, Valentina ; Zaman, Ali ; Zampolli, Chiara ; Correia Zanoli, Henrique Jose ; Zardoshti, Nima ; Zarochentsev, Andrey ; Závada, Petr ; Zaviyalov, Nikolaj ; Zbroszczyk, Hanna Paulina ; Zhalov, Mikhail ; Zhang, X. ; Zhang, Y. ; Zhang, Z. ; Zhao, C. ; Zherebchevskii, Vladimir ; Zhigareva, Natalia ; Zhou, D. ; Zhou, Y. ; Zhou, Z. ; Zhu, H. ; Zhu, J. ; Zhu, Y. ; Zichichi, Antonino ; Zimmermann, Markus ; Zinovjev, Gennady M. ; Zurlo, Nicola
The procedure for the energy calibration of the high granularity electromagnetic calorimeter PHOS of the ALICE experiment is presented. The methods used to perform the relative gain calibration, to evaluate the geometrical alignment and the corresponding correction of the absolute energy scale, to obtain the nonlinearity correction coefficients and finally, to calculate the time-dependent calibration corrections, are discussed and illustrated by the PHOS performance in proton-proton (pp) collisions at √s=13 TeV. After applying all corrections, the achieved mass resolutions for π0 and η mesons for pT > 1.7 GeV/c are σmπ0 = 4.56 ± 0.03 MeV/c2 and σmη = 15.3 ± 1.0 MeV/c2, respectively.
Wang, Mingyi ; Xiao, Mao ; Bertozzi, Barbara ; Marie, Guillaume ; Rörup, Birte ; Schulze, Benjamin ; Bardakov, Roman ; He, Xu-Cheng ; Shen, Jiali ; Scholz, Wiebke ; Marten, Ruby ; Dada, Lubna ; Baalbaki, Rima ; Lopez, Brandon ; Lamkaddam, Houssni ; Manninen, Hanna E. ; Amorim, Antonio ; Ataei, Farnoush ; Bogert, Pia ; Brasseur, Zoé ; Caudillo, Lucía ; De Menezes, Louis-Philippe ; Duplissy, Jonathan ; Ekman, Annica M. L. ; Finkenzeller, Henning ; Gonzalez Carracedo, Loïc ; Granzin, Manuel ; Guida, Roberto ; Heinritzi, Martin ; Hofbauer, Victoria ; Höhler, Kristina ; Korhonen, Kimmo ; Krechmer, Jordan E. ; Kürten, Christoph Andreas ; Lehtipalo, Katrianne ; Mahfouz, Naser G. A. ; Makhmutov, Vladimir ; Massabò, Dario ; Mathot, Serge ; Mauldin, Roy L. ; Mentler, Bernhard ; Müller, Tatjana ; Onnela, Antti ; Petäjä, Tuukka ; Philippov, Maxim ; Piedehierro, Ana A. ; Pozzer, Andrea ; Ranjithkumar, Ananth ; Schervish, Meredith ; Schobesberger, Siegfried ; Simon, Mario ; Stozhkov, Yuri ; Tomé, António ; Umo, Nsikanabasi Silas ; Vogel, Franziska ; Wagner, Robert ; Wang, Dongyu S. ; Weber, Stefan K. ; Welti, André ; Wu, Yusheng ; Zauner-Wieczorek, Marcel ; Sipilä, Mikko ; Winkler, Paul M. ; Hansel, Armin ; Baltensperger, Urs ; Kulmala, Markku ; Flagan, Richard C. ; Curtius, Joachim ; Riipinen, Ilona ; Gordon, Hamish ; Lelieveld, Jos ; El Haddad, Imad ; Volkamer, Rainer ; Worsnop, Douglas R. ; Christoudias, Theodoros ; Kirkby, Jasper ; Möhler, Ottmar ; Donahue, Neil McPherson
New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN)1,2,3,4. However, the precursor vapours that drive the process are not well understood. With experiments performed under upper tropospheric conditions in the CERN CLOUD chamber, we show that nitric acid, sulfuric acid and ammonia form particles synergistically, at rates that are orders of magnitude faster than those from any two of the three components. The importance of this mechanism depends on the availability of ammonia, which was previously thought to be efficiently scavenged by cloud droplets during convection. However, surprisingly high concentrations of ammonia and ammonium nitrate have recently been observed in the upper troposphere over the Asian monsoon region5,6. Once particles have formed, co-condensation of ammonia and abundant nitric acid alone is sufficient to drive rapid growth to CCN sizes with only trace sulfate. Moreover, our measurements show that these CCN are also highly efficient ice nucleating particles—comparable to desert dust. Our model simulations confirm that ammonia is efficiently convected aloft during the Asian monsoon, driving rapid, multi-acid HNO3–H2SO4–NH3 nucleation in the upper troposphere and producing ice nucleating particles that spread across the mid-latitude Northern Hemisphere.
Wang, Mingyi ; Kong, Weimeng ; Marten, Ruby ; He, Xu-Cheng ; Chen, Dexian ; Pfeifer, Joschka ; Heitto, Arto ; Kontkanen, Jenni ; Dada, Lubna ; Kürten, Christoph Andreas ; Yli-Juuti, Taina ; Manninen, Hanna Elina ; Amanatidis, Stavros ; Amorim, Antonio ; Baalbaki, Rima ; Baccarini, Andrea ; Bell, David M. ; Bertozzi, Barbara ; Bräkling, Steffen ; Brilke, Sophia ; Murillo, Lucía Caudillo ; Chiu, Randall ; Chu, Biwu ; De Menezes, Louis-Philippe ; Duplissy, Jonathan ; Finkenzeller, Henning ; Gonzalez Carracedo, Loic ; Granzin, Manuel ; Guida, Roberto ; Hansel, Armin ; Hofbauer, Victoria ; Krechmer, Jordan ; Lehtipalo, Katrianne ; Lamkaddam, Houssni ; Lampimäki, Marku ; Lee, Chuan Ping ; Makhmutov, Vladimir ; Marie, Guillaume ; Mathot, Serge ; Mauldin, Roy Lee ; Mentler, Bernhard ; Müller, Tatjana ; Onnela, Antti ; Partoll, Eva ; Petäjä, Tuukka ; Philippov, Maxim ; Pospisilova, Veronika ; Ranjithkumar, Ananth ; Rissanen, Matti P. ; Rörup, Birte ; Scholz, Wiebke ; Shen, Jiali ; Simon, Mario ; Sipilä, Mikko ; Steiner, Gerhard ; Stolzenburg, Dominik ; Tham, Yee Jun ; Tomé, António ; Wagner, Andrea Christine ; Wang, Dongyu S. ; Wang, Yonghong ; Weber, Stefan K. ; Winkler, Paul M. ; Wlasits, Peter J. ; Wu, Yusheng ; Xiao, Mao ; Ye, Qing ; Zauner-Wieczorek, Marcel ; Zhou, Xueqin ; Volkamer, Rainer ; Riipinen, Ilona ; Dommen, Josef ; Curtius, Joachim ; Baltensperger, Urs ; Kulmala, Markku ; Worsnop, Douglas R. ; Kirkby, Jasper ; Seinfeld, John H. ; El Haddad, Imad ; Flagan, Richard C. ; Donahue, Neil McPherson
A list of authors and their affiliations appears at the end of the paper New-particle formation is a major contributor to urban smog, but how it occurs in cities is often puzzling. If the growth rates of urban particles are similar to those found in cleaner environments (1–10 nanometres per hour), then existing understanding suggests that new urban particles should be rapidly scavenged by the high concentration of pre-existing particles. Here we show, through experiments performed under atmospheric conditions in the CLOUD chamber at CERN, that below about +5 degrees Celsius, nitric acid and ammonia vapours can condense onto freshly nucleated particles as small as a few nanometres in diameter. Moreover, when it is cold enough (below −15 degrees Celsius), nitric acid and ammonia can nucleate directly through an acid–base stabilization mechanism to form ammonium nitrate particles. Given that these vapours are often one thousand times more abundant than sulfuric acid, the resulting particle growth rates can be extremely high, reaching well above 100 nanometres per hour. However, these high growth rates require the gas-particle ammonium nitrate system to be out of equilibrium in order to sustain gas-phase supersaturations. In view of the strong temperature dependence that we measure for the gas-phase supersaturations, we expect such transient conditions to occur in inhomogeneous urban settings, especially in wintertime, driven by vertical mixing and by strong local sources such as traffic. Even though rapid growth from nitric acid and ammonia condensation may last for only a few minutes, it is nonetheless fast enough to shepherd freshly nucleated particles through the smallest size range where they are most vulnerable to scavenging loss, thus greatly increasing their survival probability. We also expect nitric acid and ammonia nucleation and rapid growth to be important in the relatively clean and cold upper free troposphere, where ammonia can be convected from the continental boundary layer and nitric acid is abundant from electrical storms.
Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments
(2015)
Kim, Jaeseok ; Ahlm, Lars ; Yli-Juuti, Taina ; Lawler, Michael Joseph ; Keskinen, Helmi ; Tröstl, Jasmin ; Schobesberger, Siegfried ; Duplissy, Jonathan ; Amorim, Antonio ; Bianchi, Federico ; Donahue, Neil McPherson ; Flagan, Richard C. ; Hakala, Jani ; Heinritzi, Martin ; Jokinen, Tuija ; Kürten, Christoph Andreas ; Laaksonen, Ari ; Lehtipalo, Katrianne ; Miettinen, Pasi ; Petäjä, Tuukka ; Rissanen, Matti P. ; Rondo, Linda ; Sengupta, Kamalika ; Simon, Mario ; Tomé, Antonio ; Williamson, Christina ; Wimmer, Daniela ; Winkler, Paul M. ; Ehrhart, Sebastian ; Ye, Penglin ; Kirkby, Jasper ; Curtius, Joachim ; Kulmala, Markku ; Lehtinen, Kari E. J. ; Smith, James N. ; Riipinen, Ilona ; Virtanen, Annele
Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e. particles that have grown to diameters of 10 and 15nm following nucleation, and measure their water uptake. Water uptake constrains their chemical composition. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90% relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) experiments performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation. The hygroscopicity parameter Κ decreased with increasing particle size indicating decreasing acidity of particles. No clear effect of the sulfuric acid monomer concentrations on the hygroscopicities of 10nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15nm particles sharply decreased with decreasing sulfuric acid monomer concentrations. In 20 particular, when the concentrations of sulfuric acid was 5.1 x 106 molecules cm exp -3 in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured Κ of 15nm particles was 0.3 ± 0.01 close to the value reported for dimethylamine sulfate (DMAS) (Κ DMAS ~ 0.28). Furthermore, the difference in Κ between sulfuric acid and sulfuric acid-dimethylamine experiments increased with increasing particle size. The Κ values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from α-pinene ozonolysis play a significant role in particle growth already at 10nm sizes.
Hygroscopicity of nanoparticles produced from homogeneous
nucleation in the CLOUD experiments
(2016)
Kim, Jaeseok ; Ahlm, Lars ; Yli-Juuti, Taina ; Lawler, Michael Joseph ; Keskinen, Helmi ; Tröstl, Jasmin ; Schobesberger, Siegfried ; Duplissy, Jonathan ; Amorim, Antonio ; Bianchi, Federico ; Donahue, Neil McPherson ; Flagan, Richard C. ; Hakala, Jani ; Heinritzi, Martin ; Jokinen, Tuija ; Kürten, Christoph Andreas ; Laaksonen, Ari ; Lehtipalo, Katrianne ; Miettinen, Pasi ; Petäjä, Tuukka ; Rissanen, Matti P. ; Rondo, Linda ; Sengupta, Kamalika ; Simon, Mario ; Tomé, Antonio ; Williamson, Christina ; Wimmer, Daniela ; Winkler, Paul M. ; Ehrhart, Sebastian ; Ye, Penglin ; Kirkby, Jasper ; Curtius, Joachim ; Baltensperger, Urs ; Kulmala, Markku ; Lehtinen, Kari E. J. ; Smith, James N. ; Riipinen, Ilona ; Virtanen, Annele
Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e., particles that have grown to diameters of 10 and 15 nm following nucleation, and measure their water uptake. Water uptake is useful information for indirectly obtaining chemical composition of aerosol particles. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90 % relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) campaign performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid–dimethylamine, and sulfuric acid–organics derived from α-pinene oxidation. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles. No clear effect of the sulfuric acid concentration on the hygroscopicity of 10 nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15 nm particles sharply decreased with decreasing sulfuric acid concentrations. In particular, when the concentration of sulfuric acid was 5.1 × 106 molecules cm−3 in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured κ of 15 nm particles was 0.31 ± 0.01: close to the value reported for dimethylaminium sulfate (DMAS) (κDMAS ∼ 0.28). Furthermore, the difference in κ between sulfuric acid and sulfuric acid–imethylamine experiments increased with increasing particle size. The κ values of particles in the presence of sulfuric acid and organics were much smaller than those of particles in the presence of sulfuric acid and dimethylamine. This suggests that the organics produced from α-pinene ozonolysis play a significant role in particle growth even at 10 nm sizes.
Keskinen, Helmi ; Virtanen, Annele ; Joutsensaari, Jorma ; Tsagkogeorgas, Georgios ; Duplissy, Jonathan ; Schobesberger, Siegfried ; Gysel, Martin ; Riccobono, Francesco ; Slowik, Jay G. ; Bianchi, Federico ; Yli-Juuti, Taina ; Lehtipalo, Katrianne ; Rondo, Linda ; Breitenlechner, Martin ; Kupc, Agnieszka ; Almeida, Joao ; Amorin, António ; Dunne, Eimear M. ; Downward, Andrew J. ; Ehrhart, Sebastian ; Franchin, Alessandro ; Kajos, Maija K. ; Kirkby, Jasper ; Kürten, Christoph Andreas ; Nieminen, Tuomo ; Makhmutov, Vladimir ; Mathot, Serge ; Miettinen, Pasi ; Onnela, Antti ; Petäjä, Tuukka ; Praplan, Arnaud Patrick ; Santos, Filipe Duarte ; Schallhart, Simon ; Sipilä, Mikko ; Stozhkov, Yuri ; Tomé, Antonio ; Vaattovaara, Petri ; Wimmer, Daniela ; Prévôt, André Stephan Henry ; Dommen, Josef ; Donahue, Neil McPherson ; Flagan, Richard C. ; Weingartner, Ernest ; Viisanen, Yrjö ; Riipinen, Ilona ; Hansel, Armin ; Curtius, Joachim ; Kulmala, Markku ; Worsnop, Douglas R. ; Baltensperger, Urs ; Wex, Heike ; Stratmann, Frank ; Laaksonen, Ari
Sulphuric acid, ammonia, amines, and oxidised organics play a crucial role in nanoparticle formation in the atmosphere. In this study, we investigate the composition of nucleated nanoparticles formed from these compounds in the CLOUD chamber experiments at CERN. The investigation is carried out via analysis of the particle hygroscopicity, ethanol affinity, oxidation state, and ion composition. Hygroscopicity was studied by a hygroscopic tandem differential mobility analyser and a cloud condensation nuclei counter, ethanol affinity by an organic differential mobility analyser and particle oxidation level by a high-resolution time-of-flight aerosol mass spectrometer. The ion composition was studied by an atmospheric pressure interface time-of-flight mass spectrometer. The volume fraction of the organics in the particles during their growth from sizes of a few nanometers to tens of nanometers was derived from measured hygroscopicity assuming the Zdanovski-Stokes-Robinson relationship, and compared to values gained from the spectrometers. The ZSR-relationship was also applied to obtain the measured ethanol affinities during the particle growth, which were used to derive the volume fractions of sulphuric acid and the other inorganics (e.g. ammonium salts). In the presence of sulphuric acid and ammonia, particles with a mobility diameter of 150 nm were chemically neutralised to ammonium sulphate. In the presence of oxidation products of pinanediol, the organic volume fraction of freshly nucleated particles increased from 0.4 to ∼0.9, with an increase in diameter from 2 to 63 nm. Conversely, the sulphuric acid volume fraction decreased from 0.6 to 0.1 when the particle diameter increased from 2 to 50 nm. The results provide information on the composition of nucleated aerosol particles during their growth in the presence of various combinations of sulphuric acid, ammonia, dimethylamine and organic oxidation products.
Keskinen, Helmi ; Virtanen, Annele ; Joutsensaari, Jorma ; Tsagkogeorgas, Georgios ; Duplissy, Jonathan ; Schobesberger, Siegfried ; Gysel, Martin ; Riccobono, Francesco ; Slowik, Jay G. ; Bianchi, Federico ; Yli-Juuti, Taina ; Lehtipalo, Katrianne ; Rondo, Linda ; Breitenlechner, Martin ; Kupc, Agnieszka ; Almeida, Joao ; Amorin, António ; Dunne, Eimear M. ; Downward, Andrew J. ; Ehrhart, Sebastian ; Franchin, Alessandro ; Kajos, Maija K. ; Kirkby, Jasper ; Kürten, Christoph Andreas ; Nieminen, Tuomo ; Makhmutov, Vladimir ; Mathot, Serge ; Miettinen, Pasi ; Onnela, Antti ; Petäjä, Tuukka ; Praplan, Arnaud Patrick ; Santos, Filipe Duarte ; Schallhart, Simon ; Sipilä, Mikko ; Stozhkov, Yuri ; Tomé, Antonio ; Vaattovaara, Petri ; Wimmer, Daniela ; Prévôt, André Stephan Henry ; Dommen, Josef ; Donahue, Neil McPherson ; Flagan, Richard C. ; Weingartner, Ernest ; Viisanen, Yrjö ; Riipinen, Ilona ; Hansel, Armin ; Curtius, Joachim ; Kulmala, Markku ; Worsnop, Douglas R. ; Baltensperger, Urs ; Wex, Heike ; Stratmann, Frank ; Laaksonen, Ari
Sulphuric acid, ammonia, amines, and oxidised organics play a crucial role in nanoparticle formation in the atmosphere. In this study, we investigate the composition of nucleated nanoparticles formed from these compounds in the CLOUD (Cosmics Leaving Outdoor Droplets) chamber experiments at CERN (Centre européen pour la recherche nucléaire). The investigation was carried out via analysis of the particle hygroscopicity, ethanol affinity, oxidation state, and ion composition. Hygroscopicity was studied by a hygroscopic tandem differential mobility analyser and a cloud condensation nuclei counter, ethanol affinity by an organic differential mobility analyser and particle oxidation level by a high-resolution time-of-flight aerosol mass spectrometer. The ion composition was studied by an atmospheric pressure interface time-of-flight mass spectrometer. The volume fraction of the organics in the particles during their growth from sizes of a few nanometers to tens of nanometers was derived from measured hygroscopicity assuming the Zdanovskii–Stokes–Robinson relationship, and compared to values gained from the spectrometers. The ZSR-relationship was also applied to obtain the measured ethanol affinities during the particle growth, which were used to derive the volume fractions of sulphuric acid and the other inorganics (e.g. ammonium salts). In the presence of sulphuric acid and ammonia, particles with a mobility diameter of 150 nm were chemically neutralised to ammonium sulphate. In the presence of oxidation products of pinanediol, the organic volume fraction of freshly nucleated particles increased from 0.4 to ~0.9, with an increase in diameter from 2 to 63 nm. Conversely, the sulphuric acid volume fraction decreased from 0.6 to 0.1 when the particle diameter increased from 2 to 50 nm. The results provide information on the composition of nucleated aerosol particles during their growth in the presence of various combinations of sulphuric acid, ammonia, dimethylamine and organic oxidation products.
Almeida, Joao ; Schobesberger, Siegfried ; Kürten, Christoph Andreas ; Ortega, Ismael K. ; Kupiainen-Määttä, Oona ; Praplan, Arnaud Patrick ; Adamov, Alexey ; Amorim, Antonio ; Bianchi, Federico ; Breitenlechner, Martin ; David, André ; Dommen, Josef ; Donahue, Neil McPherson ; Downard, Andrew ; Dunne, Eimear M. ; Duplissy, Jonathan ; Ehrhart, Sebastian ; Flagan, Richard C. ; Franchin, Alessandro ; Guida, Roberto ; Hakala, Jani ; Hansel, Armin ; Heinritzi, Martin ; Henschel, Henning ; Jokinen, Tuija ; Junninen, Heikki ; Kajos, Maija ; Kangasluoma, Juha ; Keskinen, Helmi ; Kupc, Agnieszka ; Kurtén, Theo ; Kvashin, Alexander N. ; Laaksonen, Ari ; Lehtipalo, Katrianne ; Leiminger, Markus ; Leppä, Johannes ; Loukonen, Ville ; Makhmutov, Vladimir ; Mathot, Serge ; McGrath, Matthew J. ; Nieminen, Tuomo ; Olenius, Tinja ; Onnela, Antti ; Petäjä, Tuukka ; Riccobono, Francesco ; Riipinen, Ilona ; Rissanen, Matti P. ; Rondo, Linda ; Ruuskanen, Taina ; Santos, Filipe Duarte ; Sarnela, Nina ; Schallhart, Simon ; Schnitzhofer, Ralf ; Seinfeld, John H. ; Simon, Mario ; Sipilä, Mikko ; Stozhkov, Yuri ; Stratmann, Frank ; Tomé, Antonio ; Tröstl, Jasmin ; Tsagkogeorgas, Georgios ; Vaattovaara, Petri ; Viisanen, Yrjo ; Virtanen, Annele ; Vrtala, Aron ; Wagner, Paul E. ; Weingartner, Ernest ; Wex, Heike ; Williamson, Christina ; Wimmer, Daniela ; Ye, Penglin ; Yli-Juuti, Taina ; Carslaw, Kenneth S. ; Kulmala, Markku ; Curtius, Joachim ; Baltensperger, Urs ; Worsnop, Douglas R. ; Vehkamäki, Hanna ; Kirkby, Jasper
Nucleation of aerosol particles from trace atmospheric vapours is thought to provide up to half of global cloud condensation nuclei. Aerosols can cause a net cooling of climate by scattering sunlight and by leading to smaller but more numerous cloud droplets, which makes clouds brighter and extends their lifetimes. Atmospheric aerosols derived from human activities are thought to have compensated for a large fraction of the warming caused by greenhouse gases. However, despite its importance for climate, atmospheric nucleation is poorly understood. Recently, it has been shown that sulphuric acid and ammonia cannot explain particle formation rates observed in the lower atmosphere. It is thought that amines may enhance nucleation, but until now there has been no direct evidence for amine ternary nucleation under atmospheric conditions. Here we use the CLOUD (Cosmics Leaving Outdoor Droplets) chamber at CERN and find that dimethylamine above three parts per trillion by volume can enhance particle formation rates more than 1,000-fold compared with ammonia, sufficient to account for the particle formation rates observed in the atmosphere. Molecular analysis of the clusters reveals that the faster nucleation is explained by a base-stabilization mechanism involving acid–amine pairs, which strongly decrease evaporation. The ion-induced contribution is generally small, reflecting the high stability of sulphuric acid–dimethylamine clusters and indicating that galactic cosmic rays exert only a small influence on their formation, except at low overall formation rates. Our experimental measurements are well reproduced by a dynamical model based on quantum chemical calculations of binding energies of molecular clusters, without any fitted parameters. These results show that, in regions of the atmosphere near amine sources, both amines and sulphur dioxide should be considered when assessing the impact of anthropogenic activities on particle formation.
Schobesberger, Siegfried ; Franchin, Alessandro ; Bianchi, Federico ; Rondo, Linda ; Duplissy, Jonathan ; Kürten, Christoph Andreas ; Ortega, Ismael K. ; Metzger, Axel ; Schnitzhofer, Ralf ; Almeida, Joao ; Amorim, Antonio ; Dommen, Josef ; Dunne, Eimear M. ; Ehn, Mikael ; Gagné, Stéphanie ; Ickes, Luisa ; Junninen, Heikki ; Hansel, Armin ; Kerminen, Veli-Matti ; Kirkby, Jasper ; Kupc, Agnieszka ; Laaksonen, Ari ; Lehtipalo, Katrianne ; Mathot, Serge ; Onnela, Antti ; Petäjä, Tuukka ; Riccobono, Francesco ; Santos, Filipe Duarte ; Sipilä, Mikko ; Tomé, Antonio ; Tsagkogeorgas, Georgios ; Viisanen, Yrjo ; Wagner, Paul E. ; Wimmer, Daniela ; Curtius, Joachim ; Donahue, Neil McPherson ; Baltensperger, Urs ; Kulmala, Markku ; Worsnop, Douglas R.
The formation of particles from precursor vapors is an important source of atmospheric aerosol. Research at the Cosmics Leaving OUtdoor Droplets (CLOUD) facility at CERN tries to elucidate which vapors are responsible for this new-particle formation, and how in detail it proceeds. Initial measurement campaigns at the CLOUD stainless-steel aerosol chamber focused on investigating particle formation from ammonia (NH3) and sulfuric acid (H2SO4). Experiments were conducted in the presence of water, ozone and sulfur dioxide. Contaminant trace gases were suppressed at the technological limit. For this study, we mapped out the compositions of small NH3–H2SO4 clusters over a wide range of atmospherically relevant environmental conditions. We covered [NH3] in the range from < 2 to 1400 pptv, [H2SO4] from 3.3 × 106 to 1.4 × 109 cm−3 (0.1 to 56 pptv), and a temperature range from −25 to +20 °C. Negatively and positively charged clusters were directly measured by an atmospheric pressure interface time-of-flight (APi-TOF) mass spectrometer, as they initially formed from gas-phase NH3 and H2SO4, and then grew to larger clusters containing more than 50 molecules of NH3 and H2SO4, corresponding to mobility-equivalent diameters greater than 2 nm. Water molecules evaporate from these clusters during sampling and are not observed. We found that the composition of the NH3–H2SO4 clusters is primarily determined by the ratio of gas-phase concentrations [NH3] / [H2SO4], as well as by temperature. Pure binary H2O–H2SO4 clusters (observed as clusters of only H2SO4) only form at [NH3] / [H2SO4] < 0.1 to 1. For larger values of [NH3] / [H2SO4], the composition of NH3–H2SO4 clusters was characterized by the number of NH3 molecules m added for each added H2SO4 molecule n (Δm/Δ n), where n is in the range 4–18 (negatively charged clusters) or 1–17 (positively charged clusters). For negatively charged clusters, Δ m/Δn saturated between 1 and 1.4 for [NH3] / [H2SO4] > 10. Positively charged clusters grew on average by Δm/Δn = 1.05 and were only observed at sufficiently high [NH3] / [H2SO4]. The H2SO4 molecules of these clusters are partially neutralized by NH3, in close resemblance to the acid–base bindings of ammonium bisulfate. Supported by model simulations, we substantiate previous evidence for acid–base reactions being the essential mechanism behind the formation of these clusters under atmospheric conditions and up to sizes of at least 2 nm. Our results also suggest that electrically neutral NH3–H2SO4 clusters, unobservable in this study, have generally the same composition as ionic clusters for [NH3] / [H2SO4] > 10. We expect that NH3–H2SO4 clusters form and grow also mostly by Δm/Δn > 1 in the atmosphere's boundary layer, as [NH3] / [H2SO4] is mostly larger than 10. We compared our results from CLOUD with APi-TOF measurements of NH3–H2SO4 anion clusters during new-particle formation in the Finnish boreal forest. However, the exact role of NH3–H2SO4 clusters in boundary layer particle formation remains to be resolved.
Schobesberger, Siegfried ; Franchin, Alessandro ; Bianchi, Federico ; Rondo, Linda ; Duplissy, Jonathan ; Kürten, Christoph Andreas ; Ortega, Ismael K. ; Metzger, Axel ; Schnitzhofer, Ralf ; Almeida, Joao ; Amorim, Antonio ; Dommen, Josef ; Dunne, Eimear M. ; Ehn, Mikael ; Gagné, Stéphanie ; Ickes, Luisa ; Junninen, Heikki ; Hansel, Armin ; Kerminen, Veli-Matti ; Kirkby, Jasper ; Kupc, Agnieszka ; Laaksonen, Ari ; Lehtipalo, Katrianne ; Mathot, Serge ; Onnela, Antti ; Petäjä, Tuukka ; Riccobono, Francesco ; Santos, Filipe Duarte ; Sipilä, Mikko ; Tomé, Antonio ; Tsagkogeorgas, Georgios ; Viisanen, Yrjo ; Wagner, Paul E. ; Wimmer, Daniela ; Curtius, Joachim ; Donahue, Neil McPherson ; Baltensperger, Urs ; Kulmala, Markku ; Worsnop, Douglas R.
The formation of particles from precursor vapors is an important source of atmospheric aerosol. Research at the Cosmics Leaving OUtdoor Droplets (CLOUD) facility at CERN tries to elucidate which vapors are responsible for this new particle formation, and how in detail it proceeds. Initial measurement campaigns at the CLOUD stainless-steel aerosol chamber focused on investigating particle formation from ammonia (NH3) and sulfuric acid (H2SO4). Experiments were conducted in the presence of water, ozone and sulfur dioxide. Contaminant trace gases were suppressed at the technological limit. For this study, we mapped out the compositions of small NH3-H2SO4 clusters over a wide range of atmospherically relevant environmental conditions. We covered [NH3] in the range from <2 to 1400 pptv, [H2SO4] from 3.3 × 106 to 1.4 × 109 cm−3, and a temperature range from −25 to +20 °C. Negatively and positively charged clusters were directly measured by an atmospheric pressure interface time-of-flight (APi-TOF) mass spectrometer, as they initially formed from gas-phase NH3 and H2SO4, and then grew to larger clusters containing more than 50 molecules of NH3 and H2SO4, corresponding to mobility-equivalent diameters greater than 2 nm. Water molecules evaporate from these clusters during sampling and are not observed. We found that the composition of the NH3-H2SO4 clusters is primarily determined by the ratio of gas-phase concentrations [NH3] / [H2SO4], as well as by temperature. Pure binary H2O-H2SO4 clusters (observed as clusters of only H2SO4) only form at [NH3] / [H2SO4]<0.1 to 1. For larger values of [NH3] / [H2SO4], the composition of NH3-H2SO4 clusters was characterized by the number of NH3 molecules m added for each added H2SO4 molecule n (Δm / Δn), where n is in the range 4–18 (negatively charged clusters) or 1–17 (positively charged clusters). For negatively charged clusters, Δm / Δn saturated between 1 and 1.4 for [NH3] / [H2SO4]>10. Positively charged clusters grew on average by Δm / Δn = 1.05 and were only observed at sufficiently high [NH3] / [H2SO4]. The H2SO4 molecules of these clusters are partially neutralized by NH3, in close resemblance to the acid-base bindings of ammonium bisulfate. Supported by model simulations, we substantiate previous evidence for acid-base reactions being the essential mechanism behind the formation of these clusters under atmospheric conditions and up to sizes of at least 2 nm. Our results also suggest that yet unobservable electrically neutral NH3-H2SO4 clusters grow by generally the same mechanism as ionic clusters, particularly for [NH3] / [H2SO4]>10. We expect that NH3-H2SO4 clusters form and grow also mostly by Δm / Δn>1 in the atmosphere's boundary layer, as [NH3] / [H2SO4] is mostly larger than 10. We compared our results from CLOUD with APi-TOF measurements of NH3-H2SO4 anion clusters during new particle formation in the Finnish boreal forest. However, the exact role of NH3-H2SO4 clusters in boundary layer particle formation remains to be resolved.