Miura Shinichi
Institute for Molecular Science, 38 Myodaiji, Okazaki 444-8585, Japan.
J Chem Phys. 2007 Mar 21;126(11):114309. doi: 10.1063/1.2713397.
In this paper, quantum fluctuations of a carbonyl sulfide molecule in helium-4 clusters are studied as a function of cluster size N in a small-to-large size regime (2<or=N<or=64). The molecular rotation of the dopant shows nonmonotonic size dependence in the range of 10<or=N<or=20, reflecting the density distribution of the helium atoms around the molecule. The size dependence on the rotational constant shows a plateau for N>or=20, which is larger than the experimental nanodroplet value. Superfluid response of the doped cluster is found to show remarkable anisotropy especially for N<or=20. The superfluid fraction regarding the axis perpendicular to the molecular axis shows a steep increase at N=10, giving the significant enhancement of the rotational fluctuation of the molecule. On the other hand, the superfluid fraction regarding the axis parallel to the molecular axis reaches 0.9 at N=5, arising from the bosonic exchange cycles of the helium atoms around the molecular axis. The anisotropy in the superfluid response is found to be the direct consequence of the configurations of the bosonic exchange cycles.
在本文中,研究了在从小到大规模范围(2≤N≤64)内,羰基硫分子在氦 - 4团簇中的量子涨落随团簇大小N的变化情况。掺杂剂的分子旋转在10≤N≤20范围内呈现出非单调的尺寸依赖性,这反映了分子周围氦原子的密度分布。对于N≥20,旋转常数的尺寸依赖性呈现出一个平台期,该值大于实验测得的纳米液滴值。发现掺杂团簇的超流响应表现出显著的各向异性,特别是对于N≤20的情况。关于垂直于分子轴的轴的超流分数在N = 10时急剧增加,这使得分子的旋转涨落显著增强。另一方面,关于平行于分子轴的轴的超流分数在N = 5时达到0.9,这是由分子轴周围氦原子的玻色子交换循环引起的。超流响应中的各向异性被发现是玻色子交换循环构型的直接结果。