Spectroscopy and Dynamics at the Gas-Liquid Interface (SDynG-LI)

该提案描述了一种共同努力，以阐明在液态水表面的化学相互作用。关于气相分子与液体表面相互作用的详细动力学知之甚少。虽然光谱和散射实验在过去的几十年中已经建立了坚实的理解固体和气相中的化学反应的动力学，液体和气液界面的等效实验在很大程度上missing.In为了触及这些动态的各个方面，我们提出了一个三管齐下的方法，实现了位于莱比锡，柏林和洛桑的三个节点之间的合作努力。这些实验的核心工具将是液体微射流，在每个节点将使用一个这样的设备。通过将液体射流与不同的分子束和探测方法相结合，我们将解决气-液相互作用的不同方面，如下：在柏林的Helmholtz-Zentrum进行的第一个实验中，通过气体气氛传播的液体射流将用于同步加速器芯级电子光谱实验，以检测在表面产生的物质;第二项实验位于莱比锡大学和莱比锡莱布尼茨表面改性研究所，将通过分子束撞击射流，在液体表面上沉积存款气相分子，然后使用高次谐波产生进行光电子能谱分析;最后，在洛桑联邦理工学院进行的第三个实验中，（EPFL，瑞士），液体平面射流将与分子束交叉，以阐明气液散射动力学。这项合作汇集了分子束，液态水射流，X射线光电子能谱和高次谐波产生能谱。这三个团队结合起来提供了一个专门知识库，精确地组装了解决液体界面分子散射动力学研究所需的成分。在本提案的框架内，我们将在三个原型系统上展示我们不同但互补的方法的潜力：卤素离子，我们将解决水溶液表面氢交换动力学的根本重要问题;氮氧化物分子，在那里我们探测大气化学，特别是酸雨的基石分子之一的反应动力学;和NH3，它结合了氢交换背景下的基本兴趣与大气相关性，特别是与一氧化氮分子的结合。我们预计，这项合作将不亚于踢-开创化学物理学的一个新分支，使我们对气液化学的理解达到与我们对气体表面化学和纯气相化学的理解相同的水平。

This proposal describes a joint effort to elucidate chemical interactions at liquid water surfaces. Little is known about the detailed dynamics of gas-phase molecules interacting with a liquid surface. While spectroscopy and scattering experiments in the past decades have established a firm understanding of the dynamics of chemical reactions on solids and in the gas-phase, equivalent experiments on liquids and the gas-liquid interface are largely missing.In order to touch on various aspects of these dynamics, we propose a three-pronged approach, realized by a collaborative effort between three nodes located in Leipzig, Berlin, and Lausanne. The central tool in these experiments will be liquid microjets, and at each node one such device will be used. By combining the liquid jets with different molecular beam and probing methods, we will address different aspects of gas-liquid interactions as follows: In a first experiment, conducted at the Helmholtz-Zentrum in Berlin, the liquid jet, propagating through a gas atmosphere, will be used in synchrotron core level electron spectroscopy experiments to detect the species produced at the surface; the second experiment, located at the University of Leipzig and the Leibniz Institute of Surface Modification, Leipzig, will deposit gas-phase molecules on a liquid surface by impinging a molecular beam on the jet, followed by photoelectron spectroscopy using higher harmonic generation; finally, in the third experiment, conducted at the Ecole Polytechnique Fédérale de Lausanne (EPFL, Switzerland), a liquid flat-jet will be crossed with a molecular beam in order to elucidate the gas-liquid scattering dynamics.This collaboration brings together leading groups in the fields of molecular beams, liquid water jets, X-Ray photoelectron spectroscopy, and high-harmonic generation spectroscopy. The three teams combined provide a pool of know-how that assembles precisely those ingredients required to tackle the investigation of molecular scattering dynamics at liquid interfaces.In the framework of this proposal we will demonstrate the potential of our different but complementary approaches on three prototypical systems: halogen hydrides, where we will address the fundamentally important issue of hydrogen exchange dynamics at the surface of an aqueous solution; NOx molecules, where we probe the reaction dynamics of one of the cornerstone molecules in atmospheric chemistry and in particular acid rain; and NH3, which combines fundamental interest in the context of hydrogen exchange with atmospheric relevance, in particular in combination with the nitric oxide molecules.We expect that this collaboration will do no less than to kick-start a new branch of chemical physics that will allow us to reach the same level of understanding of gas-liquid chemistry that we already have of gas-surface and pure gas-phase chemistry.