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New particle formation from isoprene under upper-tropospheric conditions
Nature ( IF 50.5 ) Pub Date : 2024-12-04 , DOI: 10.1038/s41586-024-08196-0
Jiali Shen, Douglas M. Russell, Jenna DeVivo, Felix Kunkler, Rima Baalbaki, Bernhard Mentler, Wiebke Scholz, Wenjuan Yu, Lucía Caudillo-Plath, Eva Sommer, Emelda Ahongshangbam, Dina Alfaouri, João Almeida, Antonio Amorim, Lisa J. Beck, Hannah Beckmann, Moritz Berntheusel, Nirvan Bhattacharyya, Manjula R. Canagaratna, Anouck Chassaing, Romulo Cruz-Simbron, Lubna Dada, Jonathan Duplissy, Hamish Gordon, Manuel Granzin, Lena Große Schute, Martin Heinritzi, Siddharth Iyer, Hannah Klebach, Timm Krüger, Andreas Kürten, Markus Lampimäki, Lu Liu, Brandon Lopez, Monica Martinez, Aleksandra Morawiec, Antti Onnela, Maija Peltola, Pedro Rato, Mago Reza, Sarah Richter, Birte Rörup, Milin Kaniyodical Sebastian, Mario Simon, Mihnea Surdu, Kalju Tamme, Roseline C. Thakur, António Tomé, Yandong Tong, Jens Top, Nsikanabasi Silas Umo, Gabriela Unfer, Lejish Vettikkat, Jakob Weissbacher, Christos Xenofontos, Boxing Yang, Marcel Zauner-Wieczorek, Jiangyi Zhang, Zhensen Zheng, Urs Baltensperger, Theodoros Christoudias, Richard C. Flagan, Imad El Haddad, Heikki Junninen, Ottmar Möhler, Ilona Riipinen, Urs Rohner, Siegfried Schobesberger, Rainer Volkamer, Paul M. Winkler, Armin Hansel, Katrianne Lehtipalo, Neil M. Donahue, Jos Lelieveld, Hartwig Harder, Markku Kulmala, Doug R. Worsnop, Jasper Kirkby, Joachim Curtius, Xu-Cheng He

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 °C and −50 °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.



中文翻译:


对流层上层条件下异戊二烯形成新颗粒



飞机观测显示,在亚马逊 1,2 、大西洋和太平洋上空的热带对流层上层,无处不在的新粒子形成 3,4 。尽管所涉及的蒸气仍然未知,但最近的卫星观测显示,热带对流层 5 上层的夜间异戊二烯混合比高达十亿分之一 (ppbv)。在这里,在使用 CERN CLOUD(离开室外液滴的宇宙学)室进行的实验中,我们报道了羟基自由基与 -30 °C 和 -50 °C 的对流层上部温度下异戊二烯反应引发的新颗粒形成。 我们发现异戊二烯含氧有机分子 (IP-OOM) 以对流层上部发现的浓度成核,不需要更多的蒸汽。此外,100 5 cm −3 以上的极低浓度硫酸或碘氧酸的成核速率提高了 10 倍,在 30 6 cm 的酸浓度下达到 10 cm −3 −3 左右 −1 的成核速率。我们的测量表明,成核涉及 IP-OOM 的连续添加,以及胚胎分子簇中的零个或一个酸分子。IP-OOM 还驱动颗粒在 3–60 nm h −1 处快速生长。我们发现,在闪电产生的对流层上层浓度的 NO x 存在下,快速成核和生长速率持续存在。我们的实验室测量表明,热带雨林排放的异戊二烯可能会推动热带对流层 1,2 上部的广泛区域迅速形成新的颗粒,导致每立方厘米产生数万个颗粒。

更新日期:2024-12-05
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