Trejo Marisol, Clifford Andrew, Alfonso Ernesto Garcia, Halberstadt Nadine, Xue Lan, Kong Wei
Department of Chemistry, Oregon State University, Corvallis, Oregon 97331, USA.
Labo Collisions, Agrégats, Réactivité (LCAR) Université de Toulouse and CNRS, 118 route de Narbonne, 31062 CEDEX 09 Toulouse, France.
J Chem Phys. 2024 Aug 7;161(5). doi: 10.1063/5.0221682.
We report electron diffraction results of xenon clusters formed in superfluid helium droplets, with droplet sizes in the range of 105-106 atoms/droplet and xenon clusters from a few to a few hundred atoms. Under four different experimental conditions, the diffraction profiles can be fitted using four atom pairs of Xe. For the two experiments performed with higher helium contributions, the fittings with one pair of Xe-He and three pairs of Xe-Xe distances are statistically preferred compared with four pairs of Xe-Xe distances, while the other two experiments exhibit the opposite preference. In addition to the shortest pair distances corresponding to the van der Waals distances of Xe-He and Xe-Xe, the longer distances are in the range of the different arrangements of Xe-He-Xe and Xe-He-He-Xe. The number of independent atom pairs is too many for the small xenon clusters and too few for the large clusters. We consider these results evidence of xenon foam structures, with helium atoms stuck between Xe atoms. This possibility is confirmed by helium time-dependent density functional calculations. When the impact parameter of the second xenon atom is a few Angstroms or longer, the second xenon atom fails to penetrate the solvation shell of the first atom, resulting in a dimer with a few He atoms in between the two Xe atoms. In addition, our results for larger droplets point toward a multi-center growth process of dopant atoms or molecules, which is in agreement with previous proposals from theoretical calculations and experimental results.
我们报告了在超流氦滴中形成的氙团簇的电子衍射结果,液滴大小在105 - 106个原子/液滴范围内,氙团簇含有几个到几百个原子。在四种不同的实验条件下,衍射图谱可以用四对Xe原子对来拟合。对于氦贡献较高的两个实验,与四对Xe - Xe距离相比,用一对Xe - He和三对Xe - Xe距离进行拟合在统计上更受青睐,而另外两个实验则表现出相反的偏好。除了对应于Xe - He和Xe - Xe范德华距离的最短原子对距离外,较长的距离处于Xe - He - Xe和Xe - He - He - Xe不同排列的范围内。对于小的氙团簇,独立原子对的数量太多,而对于大团簇则太少。我们认为这些结果证明了氙泡沫结构的存在,其中氦原子夹在Xe原子之间。氦的含时密度泛函计算证实了这种可能性。当第二个氙原子的碰撞参数为几埃或更长时,第二个氙原子无法穿透第一个原子的溶剂化壳层,从而形成一个在两个Xe原子之间有几个He原子的二聚体。此外,我们对较大液滴的结果表明掺杂原子或分子的多中心生长过程,这与理论计算和实验结果之前的提议一致。