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使用高分辨率冷光电子成像探测SO3和SO3的电子结构和键解离

Dao-Fu Yuan¹, Tarek Trabelsi², Yue-Rou Zhang¹

¹Department of Chemistry, Brown University, Providence, Rhode Island 02912, United States.

Journal of the American Chemical Society

|July 20, 2022

概括

这项研究首次准确地确定了三氧化硫 (SO3) 的电子亲和力及其基离子 (SO3-) 的键解离能. 这些发现为涉及SO3和SO3的大气化学提供了关键的热力学数据.

科学领域:

大气化学
量子化学
光谱学

背景情况:

三氧化硫 (SO3) 和它的基离子 (SO3-) 是大气相关的物种.
它们的实验热力学特性和电子结构尚未得到充分证实.
需要准确的数据来了解SO3在大气氧化还原反应中的作用.

研究的目的:

通过实验确定SO3的电子亲和力 (EA).
测量SO3- → SO2 + O- 的键解离能.
为SO3和SO3-提供基本的分子数据.

主要方法:

低温冷却的SO3离子的高分辨率光电子成像
使用ab initio计算,将实验光谱与计算的弗兰克-康登因子 (FCF) 配合.
监测O信号的出现以确定键解离能.

主要成果:

确定SO3的电子亲和力为2.126 6 eV.
SO3- → SO2 + O- 的结合解离能被测定为 4. 259 ± 0. 006 eV.
SO3 → SO2 + O 的自旋禁止解离能量是3.594(6) eV.

结论:

这项研究为SO3和SO3-提供了首次准确的实验测量.
这些发现增强了我们对这些大气物种基本分子特性的理解.
这些数据将有助于模拟大气中涉及SO3和SO3的氧化还原反应.

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