Synergistic HNO3–H2SO4–NH3 upper tropospheric particle formation
Author:
Wang MingyiORCID, Xiao Mao, Bertozzi BarbaraORCID, Marie GuillaumeORCID, Rörup Birte, Schulze Benjamin, Bardakov Roman, He Xu-ChengORCID, Shen Jiali, Scholz Wiebke, Marten RubyORCID, Dada Lubna, Baalbaki RimaORCID, Lopez Brandon, Lamkaddam Houssni, Manninen Hanna E., Amorim António, Ataei Farnoush, Bogert Pia, Brasseur ZoéORCID, Caudillo Lucía, De Menezes Louis-Philippe, Duplissy JonathanORCID, Ekman Annica M. L.ORCID, Finkenzeller Henning, Carracedo Loïc Gonzalez, Granzin Manuel, Guida Roberto, Heinritzi Martin, Hofbauer Victoria, Höhler KristinaORCID, Korhonen Kimmo, Krechmer Jordan E.ORCID, Kürten Andreas, Lehtipalo KatrianneORCID, Mahfouz Naser G. A.ORCID, Makhmutov Vladimir, Massabò Dario, Mathot Serge, Mauldin Roy L., Mentler BernhardORCID, Müller TatjanaORCID, Onnela Antti, Petäjä TuukkaORCID, Philippov MaximORCID, Piedehierro Ana A., Pozzer AndreaORCID, 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.ORCID, Welti AndréORCID, Wu Yusheng, Zauner-Wieczorek MarcelORCID, Sipilä Mikko, Winkler Paul M., Hansel ArminORCID, Baltensperger Urs, Kulmala MarkkuORCID, Flagan Richard C.ORCID, Curtius JoachimORCID, Riipinen Ilona, Gordon HamishORCID, Lelieveld JosORCID, El-Haddad ImadORCID, Volkamer RainerORCID, Worsnop Douglas R., Christoudias TheodorosORCID, Kirkby JasperORCID, Möhler Ottmar, Donahue Neil M.ORCID
Abstract
AbstractNew particle formation in the upper free troposphere is a major global source of cloud condensation nuclei (CCN)1–4. 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–NH3nucleation in the upper troposphere and producing ice nucleating particles that spread across the mid-latitude Northern Hemisphere.
Publisher
Springer Science and Business Media LLC
Subject
Multidisciplinary
Reference90 articles.
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