Aircraft observations have revealed ubiquitous new particle formation in the tropical upper troposphere over the Amazon(1,2) and the Atlantic and Pacific oceans(3,4). Although the vapours involved remain unknown, recent satellite observations have revealed surprisingly high night-time isoprene mixing ratios of up to 1âpart per billion by volume (ppbv) in the tropical upper troposphere(5). 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 -30â°C and -50â°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 10(5)âcm(-3), reaching rates around 30âcm(-3)âs(-1) at acid concentrations of 10(6)âcm(-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 3-60ânmâh(-1). We find that rapid nucleation and growth rates persist in the presence of NO(x) 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 troposphere(1,2), resulting in tens of thousands of particles per cubic centimetre.
New particle formation from isoprene under upper-tropospheric conditions.
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作者:Shen Jiali, Russell Douglas M, DeVivo Jenna, Kunkler Felix, Baalbaki Rima, Mentler Bernhard, Scholz Wiebke, Yu Wenjuan, Caudillo-Plath LucÃa, Sommer Eva, Ahongshangbam Emelda, Alfaouri Dina, Almeida João, 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, GroÃe Schute Lena, Heinritzi Martin, Iyer Siddharth, Klebach Hannah, Krüger Timm, Kürten Andreas, Lampimäki Markus, Liu Lu, Lopez Brandon, Martinez Monica, Morawiec Aleksandra, Onnela Antti, Peltola Maija, Rato Pedro, Reza Mago, Richter Sarah, Rörup Birte, Sebastian Milin Kaniyodical, Simon Mario, Surdu Mihnea, Tamme Kalju, Thakur Roseline C, Tomé António, 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, Möhler 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
| 期刊: | Nature | 影响因子: | 48.500 |
| 时间: | 2024 | 起止号: | 2024 Dec;636(8041):115-123 |
| doi: | 10.1038/s41586-024-08196-0 | ||
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