In situ characterization of cloud condensation nuclei, interstitial, and background particles using the single particle mass spectrometer, SPLAT II.

In situ characterization of cloud condensation nuclei, interstitial, and background particles using the single particle mass spectrometer, SPLAT II.
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DOI:
10.1021/ac1013892
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发表时间:
2010-08
影响因子:
7.4
通讯作者:
A. Zelenyuk;D. Imre;M. Earle;R. Easter;A. Korolev;R. Leaitch;Peter S. K. Liu;A. Macdonald;M. Ovchinnikov;W. Strapp
A. Zelenyuk;D. Imre;M. Earle;R. Easter;A. Korolev;R. Leaitch;Peter S. K. Liu;A. Macdonald;M. Ovchinnikov;W. Strapp
中科院分区:
化学1区
文献类型:
--
作者:
A. Zelenyuk;D. Imre;M. Earle;R. Easter;A. Korolev;R. Leaitch;Peter S. K. Liu;A. Macdonald;M. Ovchinnikov;W. Strapp

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气溶胶间接影响仍然是气候变化模型中最不确定的方面,需要以高空间和时间分辨率来表征单个颗粒的大小和成分。我们首次部署了在双数据采集模式下运行的单颗粒质谱仪 (SPLAT II),以同时测量颗粒数浓度、密度、非球面度以及单个颗粒尺寸和定量成分,时间分辨率优于 60 秒,从而产生在此示例案例中明确表征气溶胶-云相互作用所需的所有特性。我们发现颗粒由含氧有机物组成,许多与硫酸盐、生物质燃烧颗粒混合,有些与硫酸盐和加工过的海盐混合。发现云残留物比背景颗粒含有更多的硫酸盐,这解释了它们作为云凝结核(CCN)的效率更高。此外,由于云内液滴处理,CCN 硫酸盐含量随着时间的推移而增加。背景、CCN 和间隙颗粒的尺寸分布之间的比较表明,虽然几乎所有 CCN 颗粒都大于 100 nm,但超过 80% 的间隙颗粒小于 100 nm。我们得出的结论是,对于这种云,粒径是气溶胶活化成云滴的控制因素,较高的硫酸盐含量起着次要作用。
The aerosol indirect effect remains the most uncertain aspect of climate change modeling, calling for characterization of individual particles sizes and compositions with high spatial and temporal resolution. We present the first deployment of our single particle mass spectrometer (SPLAT II) operated in dual data acquisition mode to simultaneously measure particle number concentrations, density, asphericity, and individual particle size and quantitative composition, with temporal resolution better than 60 s, thus yielding all the required properties to definitively characterize the aerosol-cloud interaction in this exemplary case. We find that particles are composed of oxygenated organics, many mixed with sulfates, biomass burning particles, some with sulfates, and processed sea-salt. Cloud residuals are found to contain more sulfates than background particles, explaining their higher efficiency to serve as cloud condensation nuclei (CCN). Additionally, CCN sulfate content increased with time due to in-cloud droplet processing. A comparison between the size distributions of background, CCN, and interstitial particles shows that while nearly all CCN particles are larger than 100 nm, over 80% of interstitial particles are smaller than 100 nm. We conclude that for this cloud, particle size is the controlling factor on aerosol activation into cloud-droplets, with higher sulfate content playing a secondary role.