Curtius Joachim, Heinritzi Martin, Beck Lisa J, Pöhlker Mira L, Tripathi Nidhi, Krumm Bianca E, Holzbeck Philip, Nussbaumer Clara M, Hernández Pardo Lianet, Klimach Thomas, Barmpounis Konstantinos, Andersen Simone T, Bardakov Roman, Bohn Birger, Cecchini Micael A, Chaboureau Jean-Pierre, Dauhut Thibaut, Dienhart Dirk, Dörich Raphael, Edtbauer Achim, Giez Andreas, Hartmann Antonia, Holanda Bruna A, Joppe Philipp, Kaiser Katharina, Keber Timo, Klebach Hannah, Krüger Ovid O, Kürten Andreas, Mallaun Christian, Marno Daniel, Martinez Monica, Monteiro Carolina, Nelson Carolina, Ort Linda, Raj Subha S, Richter Sarah, Ringsdorf Akima, Rocha Fabio, Simon Mario, Sreekumar Sreedev, Tsokankunku Anywhere, Unfer Gabriela R, Valenti Isabella D, Wang Nijing, Zahn Andreas, Zauner-Wieczorek Marcel, Albrecht Rachel I, Andreae Meinrat O, Artaxo Paulo, Crowley John N, Fischer Horst, Harder Hartwig, Herdies Dirceu L, Machado Luiz A T, Pöhlker Christopher, Pöschl Ulrich, Possner Anna, Pozzer Andrea, Schneider Johannes, Williams Jonathan, Lelieveld Jos
Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, Frankfurt am Main, Germany.
Atmospheric Microphysics Department, Leibniz Institute for Tropospheric Research, Leipzig, Germany.
Nature. 2024 Dec;636(8041):124-130. doi: 10.1038/s41586-024-08192-4. Epub 2024 Dec 4.
New particle formation (NPF) in the tropical upper troposphere is a globally important source of atmospheric aerosols. It is known to occur over the Amazon basin, but the nucleation mechanism and chemical precursors have yet to be identified. Here we present comprehensive in situ aircraft measurements showing that extremely low-volatile oxidation products of isoprene, particularly certain organonitrates, drive NPF in the Amazonian upper troposphere. The organonitrates originate from OH-initiated oxidation of isoprene from forest emissions in the presence of nitrogen oxides from lightning. Nucleation bursts start about 2 h after sunrise in the outflow of nocturnal deep convection, producing high aerosol concentrations of more than 50,000 particles cm. We report measurements of characteristic diurnal cycles of precursor gases and particles. Our observations show that the interplay between biogenic isoprene, deep tropical convection with associated lightning, oxidation photochemistry and the low ambient temperature uniquely promotes NPF. The particles grow over time, undergo long-range transport and descend through subsidence to the lower troposphere, in which they can serve as cloud condensation nuclei (CCN) that influence the Earth's hydrological cycle, radiation budget and climate.
热带对流层上部的新粒子形成(NPF)是全球大气气溶胶的一个重要来源。已知这种现象发生在亚马逊盆地,但成核机制和化学前体尚未确定。在此,我们展示了全面的飞机原位测量结果,表明异戊二烯的极低挥发性氧化产物,尤其是某些有机硝酸盐,驱动了亚马逊对流层上部的新粒子形成。这些有机硝酸盐源自森林排放的异戊二烯在闪电产生的氮氧化物存在下被OH引发的氧化反应。在夜间深对流的流出区域,成核爆发在日出后约2小时开始,产生超过50,000个粒子/立方厘米的高气溶胶浓度。我们报告了前体气体和粒子特征性日循环的测量结果。我们的观测表明,生物源异戊二烯、伴有相关闪电的热带深对流、氧化光化学以及低环境温度之间的相互作用独特地促进了新粒子形成。这些粒子随时间增长,经历长距离传输,并通过下沉作用降至对流层下部,在那里它们可以作为云凝结核(CCN),影响地球的水文循环、辐射收支和气候。