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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...
Autores principales: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
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Lenguaje: | eng |
Publicado: |
2022
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Acceso en línea: | https://dx.doi.org/10.1038/s41586-022-04605-4 http://cds.cern.ch/record/2816486 |
_version_ | 1780973594769096704 |
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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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