H3(+) as a trap for noble gases-3: multiple trapping of neon, argon, and krypton in X(n)H3(+) (n = 1-3).
H3(+) as a trap for noble gases-3: multiple trapping of neon, argon, and krypton in X(n)H3(+) (n = 1-3).
复制标题
H3( ) 作为稀有气体-3 的陷阱：在 X(n)H3( ) (n = 1-3) 中多重捕获氖气、氩气和氪气。
DOI：
10.1063/1.3126777
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发表时间：
2009
期刊：
影响因子：
--
通讯作者：
O. Mousis
中科院分区：
文献类型：
--
作者：
F. Pauzat;Y. Ellinger;J. Pilmé;O. Mousis
最近对 XH(3)(+) 稀有气体复合物形成的研究表明，它对巨行星大气成分以及彗星的成分具有战略意义。天体物理过程中的一个关键因素是稀有气体与 H(3)(+) 的相对丰度。在此背景下，研究了从氖气到氪气的稀有气体 X 与一种以上稀有气体（X(n)H(3)(+) 至 n = 3）聚集的可能性。为了证实我们的结果，使用了多种方法，包括从头算耦合簇 CCSD 和 CCSD(T)、MP2 以及密度泛函 BH&HLYP 水平的理论。发现所有含有一种、两种和三种惰性气体的配合物在氖、氩和氪族中都是稳定的。这些稳定的结构是平面的，稀有气体附着在 H(3)(+) 三角形的顶点。第 n 个原子的结合能（定义为 X(n)H(3)(+) --> X(n-1)H(3)(+) + X 反应能）在氖系列中随着 n 从 1 变化到 3 略有增加，而在氩系列中则降低，并且在氪系列中当 n = 2 时显示最小值。这种现象的根源在于各自振动能量的变化。电子局域化函数的拓扑分析显示了从惰性气体到 H(3)(+) 的电荷转移作为沿系列键合的驱动力的重要性。这也与从氖到氪的原子极化率的增加一致。报告旋转常数和谐波频率，以便在空间观测之前提供用于实验室检测的大量数据。这项研究强烈表明，即使在 H(3)(+) 丰度较小的环境中，惰性气体也可以被隔离。
Recent studies on the formation of XH(3)(+) noble gas complexes have shown strategic implications for the composition of the atmospheres of the giant planets as well as for the composition of comets. One crucial factor in the astrophysical process is the relative abundances of the noble gases versus H(3)(+). It is the context in which the possibility for clustering with more than one noble gas (X(n)H(3)(+) up to n = 3) has been investigated for noble gases X ranging from neon to krypton. In order to assert our results, a variety of methods have been used including ab initio coupled cluster CCSD and CCSD(T), MP2, and density functional BH&HLYP levels of theory. All complexes with one, two, and three noble gases are found to be stable in the Ne, Ar, and Kr families. These stable structures are planar with the noble gases attached to the apices of the H(3)(+) triangle. The binding energy of the nth atom, defined as the X(n)H(3)(+) --> X(n-1)H(3)(+) + X reaction energy, increases slightly with n varying from 1 to 3 in the neon series, while it decreases in the argon series and shows a minimum for n = 2 in the krypton series. The origin of this phenomenon is to be found in the variations in the respective vibrational energies. A topological analysis of the electron localization function shows the importance of the charge transfer from the noble gases toward H(3)(+) as a driving force in the bonding along the series. It is also consistent with the increase in the atomic polarizabilities from neon to krypton. Rotational constants and harmonic frequencies are reported in order to provide a body of data to be used for the detection in laboratory prior to space observations. This study strongly suggests that the noble gases could be sequestered even in an environment where the H(3)(+) abundance is small.