Ion-induced nucleation of pure biogenic particles.
Ion-induced nucleation of pure biogenic particles.
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DOI：
10.1038/nature17953
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发表时间：
2016-05-26
期刊：
影响因子：
64.8
通讯作者：
Curtius J
中科院分区：
文献类型：
--
作者：
Kirkby J;Duplissy J;Sengupta K;Frege C;Gordon H;Williamson C;Heinritzi M;Simon M;Yan C;Almeida J;Tröstl J;Nieminen T;Ortega IK;Wagner R;Adamov A;Amorim A;Bernhammer AK;Bianchi F;Breitenlechner M;Brilke S;Chen X;Craven J;Dias A;Ehrhart S;Flagan RC;Franchin A;Fuchs C;Guida R;Hakala J;Hoyle CR;Jokinen T;Junninen H;Kangasluoma J;Kim J;Krapf M;Kürten A;Laaksonen A;Lehtipalo K;Makhmutov V;Mathot S;Molteni U;Onnela A;Peräkylä O;Piel F;Petäjä T;Praplan AP;Pringle K;Rap A;Richards NA;Riipinen I;Rissanen MP;Rondo L;Sarnela N;Schobesberger S;Scott CE;Seinfeld JH;Sipilä M;Steiner G;Stozhkov Y;Stratmann F;Tomé A;Virtanen A;Vogel AL;Wagner AC;Wagner PE;Weingartner E;Wimmer D;Winkler PM;Ye P;Zhang X;Hansel A;Dommen J;Donahue NM;Worsnop DR;Baltensperger U;Kulmala M;Carslaw KS;Curtius J
在没有硫酸的情况下，气溶胶粒子可以通过高度氧化的生物蒸汽成核在大气中形成，来自银河宇宙射线的离子与中性成核相比，成核率增加了一到两个数量级。本文的在线版本(doi：10.1038/Nature17953)包含补充材料，授权用户可以使用。在没有硫酸的情况下，气溶胶粒子可以通过高度氧化的生物蒸汽成核在大气中形成，来自银河宇宙射线的离子与中性成核相比，成核率增加了一到两个数量级。本文的在线版本(doi：10.1038/Nature17953)包含补充材料，授权用户可以使用。大气气溶胶对云的影响和气候系统的辐射强迫仍然知之甚少。人们认为，在没有硫酸的情况下，大气蒸气中的气溶胶粒子很少成核。本周发表在《自然》杂志上的两篇论文指出，高氧分子(HOMS)在促进新粒子的形成和生长方面发挥了以前没有得到重视的作用，本质上是一种在没有污染的情况下产生气溶胶的机制。Jasper Kirkby等人。结果表明，在与欧洲核子研究中心云室中的大气相关的条件下，在没有硫酸的情况下，由于离子诱导HOMS成核，可以形成气溶胶粒子。Jasmin Tröstl等人。研究了在大气条件下，在欧洲核子研究中心云室中没有硫酸的情况下，有机蒸气在成核有机颗粒初始生长中的作用。他们发现，推动初始增长的有机蒸气的挥发性极低。随着颗粒大小的增加，随后的增长主要是由于挥发度略高的更丰富的有机蒸气。本文的在线版本(doi：10.1038/Nature17953)包含补充材料，授权用户可以使用。大气气溶胶及其对云的影响被认为对气候的人为辐射强迫很重要，但仍然知之甚少。在全球范围内，大约一半的云凝结核来自大气水蒸气的成核。人们认为，硫酸是启动大气中大多数颗粒物形成的关键因素，而离子的作用相对较小。然而，一些实验室研究报告称，在没有故意添加硫酸的情况下形成了有机颗粒，尽管不能排除污染。在这里，我们提出了在大气条件下，在没有硫酸的情况下，从高度氧化的生物蒸汽中形成气溶胶颗粒的证据。高氧分子(HOMS)是由α-Pinene臭氧化生成的。我们发现，与中性成核相比，来自银河系宇宙射线的离子使成核速率提高了一到两个数量级。我们的实验结果得到了具有代表性的HOMS团簇结合能的量子化学计算的支持。在低硫酸污染的陆地环境中，离子诱导的纯有机颗粒成核可能是气溶胶颗粒的一个潜在的广泛来源。本文的在线版本(doi：10.1038/Nature17953)包含补充材料，授权用户可以使用。
Aerosol particles can form in the atmosphere by nucleation of highly oxidized biogenic vapours in the absence of sulfuric acid, with ions from Galactic cosmic rays increasing the nucleation rate by one to two orders of magnitude compared with neutral nucleation. The online version of this article (doi:10.1038/nature17953) contains supplementary material, which is available to authorized users. Aerosol particles can form in the atmosphere by nucleation of highly oxidized biogenic vapours in the absence of sulfuric acid, with ions from Galactic cosmic rays increasing the nucleation rate by one to two orders of magnitude compared with neutral nucleation. The online version of this article (doi:10.1038/nature17953) contains supplementary material, which is available to authorized users. The effect of atmospheric aerosols on clouds and the radiative forcing of the climate system remains poorly understood. It is thought that nucleation of aerosol particles from atmospheric vapours rarely proceeds in the absence of sulfuric acid. Now two papers in this week’s Nature point to a previously unappreciated role for highly oxygenated molecules (HOMs) in promoting new particle formation and growth, essentially a mechanism that produces aerosols in the absence of pollution. Jasper Kirkby et al. show that aerosol particles can form as a result of ion-induced nucleation of HOMs in the absence of sulfuric acid under conditions relevant to the atmosphere in the CLOUD chamber at CERN. Jasmin Tröstl et al. examined the role of organic vapours in the initial growth of nucleated organic particles in the absence of sulfuric acid in the CERN CLOUD chamber under atmospheric conditions. They find that the organic vapours driving initial growth have extremely low volatilities. With increasing particle size, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility. The online version of this article (doi:10.1038/nature17953) contains supplementary material, which is available to authorized users. Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere, and that ions have a relatively minor role. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution. The online version of this article (doi:10.1038/nature17953) contains supplementary material, which is available to authorized users.
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影响因子：
56.9
作者：
Bianchi, F.;Trostl, J.;Baltensperger, U.
通讯作者：
Baltensperger, U.
影响因子：
5.2
作者：
Enghoff, Martin B.;Pedersen, Jens Olaf Pepke;Svensmark, Henrik
通讯作者：
Svensmark, Henrik
影响因子：
4.5
作者：
Kerminen, VM;Kulmala, M
通讯作者：
Kulmala, M
DOI：
10.1017/cbo9781107415324.016
发表时间：
2014-01-01
期刊：
CLIMATE CHANGE 2013: THE PHYSICAL SCIENCE BASIS
影响因子：
--
作者：
Boucher, Olivier;Randall, David;Wyant, Matthew
通讯作者：
Wyant, Matthew
影响因子：
4.4
作者：
DITCHFIELD, R;HEHRE, WJ;POPLE, JA
通讯作者：
POPLE, JA