New particle formation from isoprene under upper-tropospheric conditions

• 成果类型: Article
• 署名作者: Shen, Jiali; Russell, Douglas M.; Devivo, Jenna; Kunkler, Felix; Baalbaki, Rima; Mentler, Bernhard; Scholz, Wiebke; Yu, Wenjuan; Caudillo-Plath, Lucia; Sommer, Eva; Ahongshangbam, Emelda; Alfaouri, Dina; Almeida, Joao; Amorim, Antonio; Beck, Lisa J.; Beckmann, Hannah; Berntheusel, Moritz; Bhattacharyya, Nirvan; Canagaratna, Manjula R.; Chassaing, Anouck; Cruz-Simbron, Romulo; Dada, Lubna; Duplissy, Jonathan; Gordon, Hamish; Granzin, Manuel; Grosse Schute, Lena; Heinritzi, Martin; Iyer, Siddharth; Klebach, Hannah; Krueger, Timm; Kuerten, Andreas; Lampimaeki, Markus; Liu, Lu; Lopez, Brandon; Martinez, Monica; Morawiec, Aleksandra; Onnela, Antti; Peltola, Maija; Rato, Pedro; Reza, Mago; Richter, Sarah; Roerup, Birte; Sebastian, Milin Kaniyodical; Simon, Mario; Surdu, Mihnea; Tamme, Kalju; Thakur, Roseline C.; Tome, Antonio; Tong, Yandong; Top, Jens; Umo, Nsikanabasi Silas; Unfer, Gabriela; Vettikkat, Lejish; Weissbacher, Jakob; Xenofontos, Christos; Yang, Boxing; Zauner-Wieczorek, Marcel; Zhang, Jiangyi; Zheng, Zhensen; Baltensperger, Urs; Christoudias, Theodoros; Flagan, Richard C.; El Haddad, Imad; Junninen, Heikki; Moehler, Ottmar; Riipinen, Ilona; Rohner, Urs; Schobesberger, Siegfried; Volkamer, Rainer; Winkler, Paul M.; Hansel, Armin; Lehtipalo, Katrianne; Donahue, Neil M.; Lelieveld, Jos; Harder, Hartwig; Kulmala, Markku; Worsnop, Doug R.; Kirkby, Jasper; Curtius, Joachim; He, Xu-Cheng
• 署名单位: University of Helsinki; University of Helsinki; Helsinki Institute of Physics; Goethe University Frankfurt; Carnegie Mellon University; Max Planck Society; University of Innsbruck; European Organization for Nuclear Research (CERN); University of Vienna; University of Helsinki; University of Tartu; Aerodyne Research; Stockholm University; University of Colorado System; University of Colorado Boulder; University of Colorado System; University of Colorado Boulder; Swiss Federal Institutes of Technology Domain; Paul Scherrer Institute; Tampere University; Carnegie Mellon University; Helmholtz Association; Karlsruhe Institute of Technology; Universidade da Beira Interior; Leibniz Association; Leibniz Institut fur Tropospharenforschung (TROPOS); University of Eastern Finland; California Institute of Technology; TOFWERK AG; Finnish Meteorological Institute; Carnegie Mellon University; Carnegie Mellon University; Nanjing University; Beijing University of Chemical Technology; University of Cambridge
• 刊物名称: Nature
• ISSN/ISSBN: 0028-3767
• DOI: 10.1038/s41586-024-08196-0
• 发表日期: 2024-12-05
• 关键词: secondary organic aerosol; sulfuric-acid; mass-spectrometer; basis-sets; iodine; photooxidation; chemistry; size; gas; ion

摘要

Aircraft observations have revealed ubiquitous new particle formation in the tropical upper troposphere over the Amazon1,2 and the Atlantic and Pacific oceans3,4. Although the vapours involved remain unknown, recent satellite observations have revealed surprisingly high night-time isoprene mixing ratios of up to 1 part per billion by volume (ppbv) in the tropical upper troposphere5. Here, in experiments performed with the CERN CLOUD (Cosmics Leaving Outdoor Droplets) chamber, we report new particle formation initiated by the reaction of hydroxyl radicals with isoprene at upper-tropospheric temperatures of -30 degrees C and -50 degrees C. We find that isoprene-oxygenated organic molecules (IP-OOM) nucleate at concentrations found in the upper troposphere, without requiring any more vapours. Moreover, the nucleation rates are enhanced 100-fold by extremely low concentrations of sulfuric acid or iodine oxoacids above 105 cm-3, reaching rates around 30 cm-3 s-1 at acid concentrations of 106 cm-3. Our measurements show that nucleation involves sequential addition of IP-OOM, together with zero or one acid molecule in the embryonic molecular clusters. IP-OOM also drive rapid particle growth at 3-60 nm h-1. We find that rapid nucleation and growth rates persist in the presence of NOx at upper-tropospheric concentrations from lightning. Our laboratory measurements show that isoprene emitted by rainforests may drive rapid new particle formation in extensive regions of the tropical upper troposphere1,2, resulting in tens of thousands of particles per cubic centimetre.