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Interaction of long-living solvated electrons with adsorbates at the surface of ice

长寿命溶剂化电子与冰表面吸附物的相互作用

基本信息

批准号：
189957355
负责人：
Professor Dr. Michel Bockstedte
金额：
--
依托单位：
Lehrstuhl für Physikalische Chemie I
依托单位国家：
德国
项目类别：
Research Grants
财政年份：
2011
资助国家：
德国
起止时间：
2010-12-31 至 2014-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/189957355?language=en
关键词：
Interaction long living solvated electrons

项目摘要

Fluid water, water clusters, and water ice possess the fascinating ability to solvate ions and electrons. On ice, these solvated electrons facilitate electron-induced reactions via dissociative electron attachment as, for example, takes place in atmospheric chemistry. Such process enhances the cross section as compared to the gas phase. The current understanding of the physical mechanisms at work remains rather incomplete. In particular, no molecular-scale picture exists that describes the underlying solvation dynamics of the solvated electron state or the interaction of the adsorbate with the solvated electron at the ice surface. Such a picture shall be developed for a model system. For this aim, we combine highly complementary approaches, namely, time-resolved two-photon photoelectron spectroscopy, high-resolution scanning tunneling microscopy, and theoretical approaches on the basis of first-principles and empirical methods. We will exploit the long-living solvated electron states at crystalline ice structures prepared on a metal surface and the dissociation of adsorbed halogenated benzene molecules C6H5F, C6H5Cl, and C6H5Br, i.e. of molecules with different electron afinity. The insight gained on this model system will in general contribute to the understanding of the phenomena of electron solvation in polar solvents and electron-induced processes by these solvated electrons.

液态水、水团簇和水冰具有溶解离子和电子的迷人能力。在冰上，这些溶剂化电子通过解离电子附着促进电子诱导的反应，例如，在大气化学中发生的。与气相相比，这种方法增强了横截面。目前对工作中的物理机制的理解仍然相当不完整。特别是，没有分子尺度的图片存在，描述的溶剂化电子状态或在冰表面的溶剂化电子的吸附物的相互作用的溶剂化动力学。应针对模型系统绘制此类图像。为此，我们结合联合收割机高度互补的方法，即时间分辨双光子光电子能谱，高分辨率扫描隧道显微镜，和理论方法的基础上的第一性原理和经验方法。我们将利用长寿命的溶剂化电子状态在金属表面上制备的结晶冰结构和吸附的卤代苯分子C6H5F，C6H5Cl，和C6H5Br，即具有不同的电子亲合性的分子的解离。在这个模型系统上获得的洞察力将在一般情况下有助于理解的现象，在极性溶剂中的电子溶剂化和电子诱导的过程，这些溶剂化的电子。