Nonadditive three-body polarizabilities of molecules interacting at long range: Theory and numerical results for the inert gases, H2,N2,CO2, and CH4
Nonadditive three-body polarizabilities of molecules interacting at long range: Theory and numerical results for the inert gases, H2,N2,CO2, and CH4
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远距离相互作用分子的非加和三体极化率：惰性气体 H2、N2、CO2 和 CH4 的理论和数值结果
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发表时间：
2000
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通讯作者：
K. L. Hunt
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作者：
M. H. Champagne;Xiaoping Li;K. L. Hunt
惰性气体和氢在高密度下的碰撞光散射光谱提供了非加性三体相互作用效应的证据，这需要一个定量的理论。在这项工作中，我们推导和评估了电子重叠可忽略的相互作用分子的三体极化率Δα(3)。我们的结果基于非局域响应理论，解释了偶极诱导偶极(DID)相互作用、四极感应、色散和协同感应-色散效应。先导顺序的贡献来自DID项，该DID项在分子极化率α中标度为DID 3d−6和簇内分子之间的代表性距离d。然而，四极诱导效应也很大，在大约1A.U的间隔下，在本工作中研究的物种的等边三角形构型的主要DID项的∼在35%到104%之间。在各向同性对势中的范德华极小值之外。对于相同的配置，发现...
Collision-induced light scattering spectra of the inert gases and hydrogen at high densities provide evidence of nonadditive three-body interaction effects, for which a quantitative theory is needed. In this work, we derive and evaluate the three-body polarizability Δα(3) for interacting molecules with negligible electronic overlap. Our results, based on nonlocal response theory, account for dipole-induced-dipole (DID) interactions, quadrupolar induction, dispersion, and concerted induction-dispersion effects. The contribution of leading order comes from a DID term that scales as α3d−6 in the molecular polarizability α and a representative distance d between the molecules in a cluster. Quadrupolar induction effects are also large, however, ranging from ∼35% to 104% of the leading DID terms for equilateral triangular configurations of the species studied in this work, at separations approximately 1 a.u. beyond the van der Waals minima in the isotropic pair potentials. For the same configurations, the dispe...