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Synergistic HNO$_{3}$–H$_{2}$SO$_{4}$–NH$_{3}$ upper tropospheric particle formation

New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN). 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 nitr...

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Autores principales: 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, António, Ataei, Farnoush, Bogert, Pia, Brasseur, Zoé, Caudillo, Lucía, De Menezes, Louis-Philippe, Duplissy, Jonathan, Ekman, Annica M L, Finkenzeller, Henning, Carracedo, Loïc Gonzalez, Granzin, Manuel, Guida, Roberto, Heinritzi, Martin, Hofbauer, Victoria, Höhler, Kristina, Korhonen, Kimmo, Krechmer, Jordan E, Kürten, 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 M
Lenguaje:eng
Publicado: 2022
Acceso en línea:https://dx.doi.org/10.1038/s41586-022-04605-4
http://cds.cern.ch/record/2816486
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author 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, António
Ataei, Farnoush
Bogert, Pia
Brasseur, Zoé
Caudillo, Lucía
De Menezes, Louis-Philippe
Duplissy, Jonathan
Ekman, Annica M L
Finkenzeller, Henning
Carracedo, Loïc Gonzalez
Granzin, Manuel
Guida, Roberto
Heinritzi, Martin
Hofbauer, Victoria
Höhler, Kristina
Korhonen, Kimmo
Krechmer, Jordan E
Kürten, 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 M
author_facet 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, António
Ataei, Farnoush
Bogert, Pia
Brasseur, Zoé
Caudillo, Lucía
De Menezes, Louis-Philippe
Duplissy, Jonathan
Ekman, Annica M L
Finkenzeller, Henning
Carracedo, Loïc Gonzalez
Granzin, Manuel
Guida, Roberto
Heinritzi, Martin
Hofbauer, Victoria
Höhler, Kristina
Korhonen, Kimmo
Krechmer, Jordan E
Kürten, 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 M
author_sort Wang, Mingyi
collection CERN
description New particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN). 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 region. 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 HNO$_{3}$–H$_{2}$SO$_{4}$–NH$_{3}$ nucleation in the upper troposphere and producing ice nucleating particles that spread across the mid-latitude Northern Hemisphere.
id cern-2816486
institution Organización Europea para la Investigación Nuclear
language eng
publishDate 2022
record_format invenio
spelling cern-28164862023-03-30T15:29:22Zdoi:10.1038/s41586-022-04605-4http://cds.cern.ch/record/2816486engWang, MingyiXiao, MaoBertozzi, BarbaraMarie, GuillaumeRörup, BirteSchulze, BenjaminBardakov, RomanHe, Xu-ChengShen, JialiScholz, WiebkeMarten, RubyDada, LubnaBaalbaki, RimaLopez, BrandonLamkaddam, HoussniManninen, Hanna EAmorim, AntónioAtaei, FarnoushBogert, PiaBrasseur, ZoéCaudillo, LucíaDe Menezes, Louis-PhilippeDuplissy, JonathanEkman, Annica M LFinkenzeller, HenningCarracedo, Loïc GonzalezGranzin, ManuelGuida, RobertoHeinritzi, MartinHofbauer, VictoriaHöhler, KristinaKorhonen, KimmoKrechmer, Jordan EKürten, AndreasLehtipalo, KatrianneMahfouz, Naser G AMakhmutov, VladimirMassabò, DarioMathot, SergeMauldin, Roy LMentler, BernhardMüller, TatjanaOnnela, AnttiPetäjä, TuukkaPhilippov, MaximPiedehierro, Ana APozzer, AndreaRanjithkumar, AnanthSchervish, MeredithSchobesberger, SiegfriedSimon, MarioStozhkov, YuriTomé, AntónioUmo, Nsikanabasi SilasVogel, FranziskaWagner, RobertWang, Dongyu SWeber, Stefan KWelti, AndréWu, YushengZauner-Wieczorek, MarcelSipilä, MikkoWinkler, Paul MHansel, ArminBaltensperger, UrsKulmala, MarkkuFlagan, Richard CCurtius, JoachimRiipinen, IlonaGordon, HamishLelieveld, JosEl-Haddad, ImadVolkamer, RainerWorsnop, Douglas RChristoudias, TheodorosKirkby, JasperMöhler, OttmarDonahue, Neil MSynergistic HNO$_{3}$–H$_{2}$SO$_{4}$–NH$_{3}$ upper tropospheric particle formationNew particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN). 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 region. 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 HNO$_{3}$–H$_{2}$SO$_{4}$–NH$_{3}$ nucleation in the upper troposphere and producing ice nucleating particles that spread across the mid-latitude Northern Hemisphere.oai:cds.cern.ch:28164862022
spellingShingle 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, António
Ataei, Farnoush
Bogert, Pia
Brasseur, Zoé
Caudillo, Lucía
De Menezes, Louis-Philippe
Duplissy, Jonathan
Ekman, Annica M L
Finkenzeller, Henning
Carracedo, Loïc Gonzalez
Granzin, Manuel
Guida, Roberto
Heinritzi, Martin
Hofbauer, Victoria
Höhler, Kristina
Korhonen, Kimmo
Krechmer, Jordan E
Kürten, 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 M
Synergistic HNO$_{3}$–H$_{2}$SO$_{4}$–NH$_{3}$ upper tropospheric particle formation
title Synergistic HNO$_{3}$–H$_{2}$SO$_{4}$–NH$_{3}$ upper tropospheric particle formation
title_full Synergistic HNO$_{3}$–H$_{2}$SO$_{4}$–NH$_{3}$ upper tropospheric particle formation
title_fullStr Synergistic HNO$_{3}$–H$_{2}$SO$_{4}$–NH$_{3}$ upper tropospheric particle formation
title_full_unstemmed Synergistic HNO$_{3}$–H$_{2}$SO$_{4}$–NH$_{3}$ upper tropospheric particle formation
title_short Synergistic HNO$_{3}$–H$_{2}$SO$_{4}$–NH$_{3}$ upper tropospheric particle formation
title_sort synergistic hno$_{3}$–h$_{2}$so$_{4}$–nh$_{3}$ upper tropospheric particle formation
url https://dx.doi.org/10.1038/s41586-022-04605-4
http://cds.cern.ch/record/2816486
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