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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Calculated electronic transitions in sulfuric acid and implications for its photodissociation in the atmosphere
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Calculated electronic transitions in sulfuric acid and implications for its photodissociation in the atmosphere

机译：硫酸中的电子跃迁及其对大气中光解离的影响

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摘要

We have calculated electronic transitions for sulfuric acid in the ultraviolet region using a hierarchy of coupled cluster response functions and correlation consistent basis sets. Our calculations indicate that the lowest energy singlet transition occurs at 8.42 eV with an oscillator strength of 0.01. The lowest energy triplet state occurs at 8.24 eV. Thus, the cross section of sulfuric acid in the actinic region is likely to be very small and smaller than the upper limit put on this cross section by previous experimental investigations. We estimate the cross section of sulfuric acid in the atmospherically relevant Lyman-alpha region (similar to 10.2 eV) to be similar to 6 x 10(-17) cm(2) molecule(-1), a value approximately 30 times larger than the speculative value used in previous atmospheric simulations. We have calculated the J values for photodissociation of sulfuric acid with absorption of visible, UV, and Lyman-alpha radiation, at altitudes between 30 and 100 km. We find that the dominant photodissociation mechanism of sulfuric acid below 70 km is absorption in the visible region by OH stretching overtone transitions, whereas above 70 km, absorption of Lyman-alpha radiation by high energy Rydberg excited states is the favored mechanism. The low lying electronic transitions of sulfuric acid in the UV region do not contribute significantly to its dissociation at any altitude.
机译：我们已经使用耦合簇响应函数和相关一致基集的层次结构计算了紫外线区域中硫酸的电子跃迁。我们的计算表明，最低能量单重态跃迁发生在8.42 eV且振荡器强度为0.01时。最低能量三重态出现在8.24 eV。因此，光化区域中硫酸的横截面可能非常小，并且小于先前实验研究对该横截面施加的上限。我们估计与大气相关的Lyman-alpha区域（类似于10.2 eV）中的硫酸截面类似于6 x 10（-17）cm（2）分子（-1），其值大约是大30倍在先前的大气模拟中使用的推测值。我们已经计算出在30至100 km之间的高度，硫酸与可见光，UV和Lyman-α辐射吸收后光解离的J值。我们发现，低于70 km的硫酸的主要光解离机理是通过OH拉伸泛音跃迁在可见光区吸收，而高于70 km，高能里德堡激发态对Lyman-α辐射的吸收是有利的机理。硫酸在紫外区的低电子跃迁在任何高度下都不会对其分解产生重大影响。

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