Formation Dynamics and Spectroscopy of Novel Rare-Gas Atom Containing Molecules

R.加州大学欧文分校的Benny Gerber在理论和计算化学项目的支持下，利用分子动力学模拟探索含新型稀有气体分子的形成机制，包括可能涉及的不同势能表面之间的“表面跳跃”。 这些稀有气体分子，如HXeCl和HXeOH，最近被实验发现，并具有典型化学强度的稳定键。 模拟将计算这些化合物的形成产率及其对辐射波长和温度的依赖性，包括稀有气体团簇和基质中的物种。 计算的另一个目的是预测是否可以通过从团簇物种中蒸发稀有气体原子来制备新的但仍然未知的含稀有气体的化合物。 这项研究将追求新的含氩分子的形成，以及制备含氖和氦分子的可能性。 最后，模拟将用于测试HRgX分子的纯晶体是否稳定。 除了动力学模拟外，还将使用振动自洽场（VSCF）方法计算新分子的振动光谱，其中包括非谐性和模式之间的耦合效应。 这一努力的成果预计将大大扩展有关一类新的有趣分子的知识，能够发现该家族中的新物种，并鼓励对非稀有气体化学惰性分子的类似化合物的研究。 直到最近，人们普遍认为稀有气体原子（氦、氖、氩、氪、氙和氡）不能在中性分子的电子基态形成化学键，含有稀有气体原子的化合物属于有限的一类。 在这项研究中探索的新的稀有气体分子家族最终可能在包括大气化学和材料化学在内的各个科学领域具有重要的应用。

R. Benny Gerber of the University of California, Irvine, is supported by the Theoretical and Computational Chemistry Program to explore the formation mechanism of novel rare gas containing molecules using molecular dynamics simulations, including "surface hopping" between the different potential energy surfaces that may be involved. These rare gas molecules, such as HXeCl and HXeOH, have recently been discovered experimentally, and have stable bonds of typical chemical strength. The simulations will compute the formation yield of these compounds and its dependence on radiation wavelength and temperature, both for the rare gas clusters and for species in matrices. Another objective of the calculations is to predict if new but still unknown rare gas containing compounds can be made by evaporation of rare gas atoms from clusters species. This research will pursue the formation of new argon-containing molecules, and the possibility of preparing neon and helium containing molecules. Finally, simulations will be used to test whether pure crystals of HRgX molecules can be stable. In addition to the dynamics simulations, calculations of the vibrational spectroscopy of the new molecules will be carried out using the Vibrational Self-Consistent Field (VSCF) method, which includes effects of anharmonicities and coupling between modes. The outcomes of this effort are expected to greatly expand knowledge about a new and interesting class of molecules, enable discovery of new species within this family, and encourage studies of analogous compounds for non-rare gas chemically inert molecules. Until recently, it was widely assumed that rare gas atoms (helium, neon, argon, krypton, xenon, and radon) could not form chemical bonds in the electronic ground state of neutral molecules, and chemical compounds containing rare gas atoms have belonged to a limited class. The new family of rare gas molecules that will be explored in this research could ultimately have significant applications in various areas of science, including atmospheric chemistry and materials chemistry.