Shen Jiali, Russell Douglas M, DeVivo Jenna, Kunkler Felix, Baalbaki Rima, Mentler Bernhard, Scholz Wiebke, Yu Wenjuan, Caudillo-Plath Lucía, 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, Große 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
Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland.
Helsinki Institute of Physics, University of Helsinki, Helsinki, Finland.
Nature. 2024 Dec;636(8041):115-123. doi: 10.1038/s41586-024-08196-0. Epub 2024 Dec 4.
Aircraft observations have revealed ubiquitous new particle formation in the tropical upper troposphere over the Amazon and the Atlantic and Pacific oceans. 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 troposphere. 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 10 cm, reaching rates around 30 cm s at acid concentrations of 10 cm. 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. We find that rapid nucleation and growth rates persist in the presence of NO 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, resulting in tens of thousands of particles per cubic centimetre.
飞机观测显示,在亚马逊地区以及大西洋和太平洋上空的热带对流层上部普遍存在新粒子形成现象。尽管其中涉及的蒸汽成分尚不清楚,但最近的卫星观测显示,热带对流层上部夜间异戊二烯混合比高达十亿分之一体积比(ppbv),这一数值令人惊讶。在此,我们在欧洲核子研究组织的CLOUD(宇宙射线产生户外水滴)实验舱中进行了实验,报告了在对流层上部-30°C和-50°C的温度下,羟基自由基与异戊二烯反应引发的新粒子形成情况。我们发现,异戊二烯氧化有机分子(IP-OOM)在对流层上部发现的浓度下成核,无需其他蒸汽。此外,在高于10⁻⁵厘米的极低硫酸或碘含氧酸浓度下,成核速率提高了100倍,在酸浓度为10⁻⁵厘米时达到约30厘米⁻³秒⁻¹的速率。我们的测量表明,成核过程涉及IP-OOM的顺序添加,以及胚胎分子簇中零个或一个酸分子。IP-OOM还能在3 - 60纳米/小时的速度下驱动粒子快速生长。我们发现,在对流层上部闪电产生的一氧化氮浓度存在的情况下,快速成核和生长速率依然存在。我们的实验室测量表明,雨林排放的异戊二烯可能在热带对流层上部的广阔区域驱动快速的新粒子形成,导致每立方厘米产生数万个粒子。