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由生物源新粒子形成导致的人为气溶胶辐射强迫降低。

Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation.

作者信息

Gordon Hamish, Sengupta Kamalika, Rap Alexandru, Duplissy Jonathan, Frege Carla, Williamson Christina, Heinritzi Martin, Simon Mario, Yan Chao, Almeida João, Tröstl Jasmin, Nieminen Tuomo, Ortega Ismael K, Wagner Robert, Dunne Eimear M, Adamov Alexey, Amorim Antonio, Bernhammer Anne-Kathrin, Bianchi Federico, Breitenlechner Martin, Brilke Sophia, Chen Xuemeng, Craven Jill S, Dias Antonio, Ehrhart Sebastian, Fischer Lukas, Flagan Richard C, Franchin Alessandro, Fuchs Claudia, Guida Roberto, Hakala Jani, Hoyle Christopher R, Jokinen Tuija, Junninen Heikki, Kangasluoma Juha, Kim Jaeseok, Kirkby Jasper, Krapf Manuel, Kürten Andreas, Laaksonen Ari, Lehtipalo Katrianne, Makhmutov Vladimir, Mathot Serge, Molteni Ugo, Monks Sarah A, Onnela Antti, Peräkylä Otso, Piel Felix, Petäjä Tuukka, Praplan Arnaud P, Pringle Kirsty J, Richards Nigel A D, Rissanen Matti P, Rondo Linda, Sarnela Nina, Schobesberger Siegfried, Scott Catherine E, Seinfeld John H, Sharma Sangeeta, Sipilä Mikko, Steiner Gerhard, Stozhkov Yuri, Stratmann Frank, Tomé Antonio, Virtanen Annele, Vogel Alexander Lucas, Wagner Andrea C, Wagner Paul E, Weingartner Ernest, Wimmer Daniela, Winkler Paul M, Ye Penglin, Zhang Xuan, Hansel Armin, Dommen Josef, Donahue Neil M, Worsnop Douglas R, Baltensperger Urs, Kulmala Markku, Curtius Joachim, Carslaw Kenneth S

机构信息

Department of Experimental Physics, CERN (European Organization for Nuclear Research), CH-1211 Geneva, Switzerland;

School of Earth and Environment, University of Leeds, Leeds LS2 9JT, United Kingdom.

出版信息

Proc Natl Acad Sci U S A. 2016 Oct 25;113(43):12053-12058. doi: 10.1073/pnas.1602360113. Epub 2016 Oct 10.

Abstract

The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol-cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20-100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by [Formula: see text] (27%) to [Formula: see text] Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.

摘要

人为排放造成的气溶胶辐射强迫的强度取决于工业化前原始条件下大气的基线状态。测量表明,在大气条件下,仅由生物源蒸汽就可发生颗粒物形成。在此,我们评估了这种颗粒物来源对工业化时期前工业化云凝结核(CCN)浓度和气溶胶 - 云辐射强迫的潜在影响。模型模拟表明,由于气溶胶浓度较低,纯生物源颗粒物形成机制对前工业化大气中CCN浓度的相对影响比对当前大气中的影响大得多。因此,前工业化时期云的反照率比当前条件下增加得更多,从而人为气溶胶的冷却强迫降低。该机制使前工业化低层大气的很大一部分区域内CCN浓度增加20% - 100%,自1750年以来由云反照率变化引起的年全球平均辐射强迫幅度降低了[公式:见原文](27%)至[公式:见原文]。模型的不确定性、相对较慢的形成速率以及有限的可用环境测量数据使得难以确定在工业化前条件下起主导作用的一种机制的重要性。我们的模拟预测亚马逊地区的颗粒物形成比观测到的更多。然而,现在已经报道了在自由对流层首次观测到纯有机成核现象。鉴于其对人为强迫可能产生的重大影响,应努力更好地理解这种自然驱动的气溶胶过程。

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