Probing the Chemistry of Reactive Molecules with Synchrotron Radiation

用同步辐射探测反应分子的化学

• 批准号: 342738563
• 负责人: Professor Dr. Ingo Fischer
• 金额: --
• 依托单位: Institut für Physikalische und Theoretische Chemie
• 依托单位国家: 德国
• 项目类别: Research Grants
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/342738563?language=en
• 关键词: Probing; Chemistry; Reactive; Molecules; Synchrotron

In this project we will employ synchrotron radiation (SR) in the vacuum-ultraviolet and soft X-ray regime to probe the chemistry of reactive molecules. This includes (a) unimolecular reactions like dissociative photoionization, (b) bimolecular reactions of open-shell species with stable molecules, and (c) reactions that lead to the formation of hitherto unexplored molecules. We will focus on species and reactions that are of interest in combustion, interstellar and atmospheric chemistry, but also on boron-containing molecules of fundamental interest in inorganic chemistry. Measurements will be conducted at the storage rings Swiss Light Source (SLS) at the Paul Scherrer Institute (Villigen/CH) and the Synchrotron SOLEIL in St. Aubin/Paris. The experiments will rely on the detection of ions and electrons. For data analysis and interpretation we will continue to cooperate with theory groups.In addition to pyrolysis, i.e. thermal radical generation we will employ a new photolysis flow reactor setup available at the SLS. It permits to produce radicals in bimolecular reactions that are not easily accessible by thermal processes, for example oxyradicals. Furthermore this reactor permits to investigate the kinetics of radical/molecule reactions and to determine reaction rates. We will start with the reaction of allyl, C3H5 + O2 and then proceed to other hydrocarbon radicals and carbenes. We will also expand our research program to the soft X-ray regime and explore the fragmentation dynamics after excitation of core electrons in isocyanic acid, HNCO. This molecule contains the major atoms of organic molecules and combines the advantages of a small few-atom molecule with a considerable degree of complexity. As a first step we will record resonant Auger-spectra of HNCO and in the next step study the site-selectivity of fragmentation upon excitation of the various resonances. The VUV photoionization and dissociative photoionization of reactive molecules will continue to be an important part of our research. We will determine the ionization energies of reactive molecules and the appearance energies AE0K of relevant dissociative photoionization channels. We will focus on species with heteroatoms, for example the isomers of picolyl, C6H6N. Furthermore we are interested in boron-containing molecules like BH3 and B2Hx. For generating boron compounds, we will employ a discharge flow reactor available at Soleil in addition to pyrolysis and photolysis sources.

在这个项目中，我们将在真空-紫外线和软X射线区域使用同步辐射(SR)来探索反应分子的化学。这包括(A)像解离光电离这样的单分子反应，(B)开壳物种与稳定分子的双分子反应，以及(C)导致迄今未被探索的分子的形成的反应。我们将专注于燃烧、星际和大气化学中感兴趣的物种和反应，但也将关注无机化学中基本感兴趣的含硼分子。测量将在保罗谢勒研究所(维利根/CH)的存储环瑞士光源(SLS)和圣奥宾/巴黎的同步加速器太阳上进行。这些实验将依赖于离子和电子的探测。对于数据分析和解释，我们将继续与理论小组合作。除了热解，即热自由基生成，我们还将使用SLS提供的新的光解流动反应器装置。它允许在双分子反应中产生热过程不易获得的自由基，例如氧自由基。此外，该反应器还允许研究自由基/分子反应的动力学并确定反应速率。我们将从烯丙基、C3H5+O2的反应开始，然后继续进行其他碳氢自由基和卡宾的反应。我们还将把我们的研究项目扩展到软X射线区域，并探索在异氰酸(HNCO)中激发核心电子后的碎裂动力学。这种分子包含有机分子中的主要原子，并结合了小原子分子的优点和相当程度的复杂性。作为第一步，我们将记录HNCO的共振俄歇谱，并在下一步研究在各种共振激发下碎裂的位置选择性。反应分子的真空紫外光电离和解离光电离将继续是我们研究的重要部分。我们将测定反应分子的电离能和相关解离光离通道的出现能AE0K。我们将集中在具有杂原子的物种上，例如吡啶甲酰的异构体，C6H6N。此外，我们还对BH3和B2Hx等含硼分子感兴趣。为了产生硼化合物，除了热解和光解来源外，我们还将使用Soleil提供的放电流动反应器。