地球低层和高层大气中无机气溶胶的形成和增长

R. Saunders, J. Plane
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引用次数: 1

摘要

本章描述了大气中两个截然不同的区域中气溶胶颗粒的光化学产生:海洋边界层中的氧化碘颗粒,以及由行星际尘埃烧蚀在中层上层形成的大气烟雾颗粒。这两种体系惊人地相似——可冷凝的无机蒸汽的来源在大气之外,是从海洋或太空注入大气的——粒子是通过均匀成核形成的。本章的目的是描述一个实验室和模型研究,以了解在基本水平上粒子的成核和生长是如何发生的。氧化碘颗粒是由o2与o2的光氧化作用产生的,这很可能是在海藻丰富的沿海地区MBL中观测到的产生新颗粒爆发的主要光化学途径。捕获的颗粒被观察到呈分形(即具有开放或非致密结构),并由稳定的氧化物i2o组成。由氧化铁、氧化硅和硅酸铁组成的大气烟雾类似物,在o3存在下由含铁和含硅气相前体的光氧化形成。含铁颗粒的成像显示它们是扩展的分形聚集体。对于每个系统,都建立了模型来阐明颗粒的生长动力学,并根据标准分形参数对其进行表征。在较长的生长时间内,二氧化钛颗粒的分形维数(df)值为2.5,符合颗粒簇扩散限制聚集(DLA)机制,而烟雾类似物的分形维数(df)值较低(1.75),似乎是由磁聚集过程引起的。
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Inorganic aerosol formation and growth in the Earth's lower and upper atmosphere
This chapter describes the photo-chemical production of aerosol particles in two very different regions of the atmosphere: iodine oxide particles in the marine boundary layer (MBL), and meteoric smoke particles that form in the upper mesosphere from the ablation of interplanetary dust. These two systems are surprisingly analogous - the source of the condensable inorganic vapours is external to the atmosphere, being injected into the atmosphere from the ocean or from space - and the particles are formed by homogeneous nucleation. The purpose of the chapter is to describe a laboratory and modelling study to understand at a fundamental level how the nucleation and growth of the particles occurs. Iodine oxide particles were produced from the photo-oxidation of gaseous I 2 with O 3 , which is most likely the primary photo-chemical route to produce the bursts of new particles observed in the MBL at seaweed-rich coastal locations. The captured particles were observed to be fractal-like (i.e., with open or non-compact structures), and to be composed of the stable oxide I 2 O 5 . Meteoric smoke analogues of iron oxide, silicon oxide, and iron silicate composition were similarly formed from the photo-oxidation of iron- and silicon-containing gas-phase precursors in the presence of O 3 . Imaging of the iron-containing particles showed them to be extended, fractal aggregates. For each system, models were developed to elucidate the growth kinetics of the particles and to characterise them in terms of standard fractal parameters. I 2 O 5 particles were found to have a fractal dimension (D f ) value of 2.5 at long growth times, consistent with a particle-cluster diffusion-limited aggregation (DLA) mechanism, whereas smoke analogues had lower D f values (1.75) which appear to result from a magnetic aggregation process.
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