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

Wang, Mingyi; Xiao, Mao; Bertozzi, Barbara 1; 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 ORCID iD icon 2; ... mehr

Abstract:

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 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.


Verlagsausgabe §
DOI: 10.5445/IR/1000148964
Veröffentlicht am 25.07.2022
Originalveröffentlichung
DOI: 10.1038/s41586-022-04605-4
Scopus
Zitationen: 32
Web of Science
Zitationen: 34
Dimensions
Zitationen: 38
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Meteorologie und Klimaforschung Atmosphärische Aerosolforschung (IMKAAF)
Publikationstyp Zeitschriftenaufsatz
Publikationsdatum 19.05.2022
Sprache Englisch
Identifikator ISSN: 0028-0836, 1476-4687
KITopen-ID: 1000148964
HGF-Programm 12.11.26 (POF IV, LK 01) Aerosol-Cloud-Climate-Interaction
Erschienen in Nature
Verlag Nature Research
Band 605
Heft 7910
Seiten 483–489
Vorab online veröffentlicht am 18.05.2022
Nachgewiesen in Dimensions
Web of Science
Scopus
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