Photoionization and Dissoziative Photoionization of Reactive Molecules Using Synchrotron Radiation

在本项目中，我们将继续利用同步辐射对活性分子的光致电离和解离光离进行研究。这些分子将由合适的前体通过热解产生。分子参数，如电离能和出现能，将被确定，以便得出热化学性质，如结合能和生成热。此外，这些数据将有助于在线识别火焰中的自由基。该项目的另一个令人兴奋的方面是有可能通过光谱鉴定迄今未知的活性中间体。我们将扩展我们对含有杂原子的活性分子的研究，特别是氮，因为含氮的自由基还没有被很好地探索。我们将研究NH2和NH，两个与天体化学相关的小自由基，N-杂环自由基吡啶和吡咯基，预计它们存在于生物燃料燃烧和CNN自由基中。另一种候选者是氮杂波利定，一种含有B和N原子的杂环。另一个令人感兴趣的体系是重氮蓝鼓酸的热解。初步实验表明，从这种前体中形成了几个不寻常的和尚未表征的物种，其中包括直链NNCCO和恶唑-叶立烯。我们将在进一步的实验中验证这些物种的世代。活性碳氢化合物的光致电离研究将继续进行。一些不太稳定的C7H6异构体还没有被成功地表征，将重新修饰。该项目下一阶段的主题也是丁烯基异构体C4H7。最后，我们将确定几种可能与碳烟形成有关的由五元环和六元环组成的多环芳烃(PAH)的电离能。

In this project we will continue our research on the photoionization and dissociative photoionization of reactive molecules using synchrotron radiation. The molecules will be generated by pyrolysis from suitable precursors. Molecular parameters like ionization and appearance energies will be determined in order to derive thermochemical properties like binding energies and heats of formation. Furthermore the data will aid in the on-line identification of radicals in flames. A further exciting aspect of this project is the possibility to spectroscopically identify hitherto unknown reactive intermediates. We will extend our studies of reactive molecules containing heteroatoms, in particular nitrogen, because N-containing radicals are not well explored. We will investigate NH2 and NH, two small radicals of astrochemical relevance, the N-heterocyclic radicals pyridyl and pyrrolyl, which are expected to be present in biofuel combustion and the CNN radical. Another candidate is azaboridine, a heterocycle that contains B and N atoms. A further system of interest is the pyrolysis of diazomeldrums acid. Preliminary experiments indicate the formation of several unusual and not yet characterized species from this precursor, among them the linear chain NNCCO and an oxazole-ylidene. We will verify the generation of these species in further experiments. Studies on the photoionization of reactive hydrocarbons will be continued. Some of the less stable isomer of C7H6 have not yet been successfully characterized and will be readdressed. Subject of the next phase of the project are also the isomers of butenyl, C4H7. Finally we will determine the ionization energies of several polycyclic aromatic hydrocarbons (PAH) composed of five- and six-membered rings that are possibly involved in soot formation.