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In a series of previously published works the phenomenon of collision inducednonlinear hyper-Rayleigh scattering of light (CIHRS) was studied on the basis of the numericalquantum chemistry (QC) methods confronted with a theoretical approach. A class of super-molecular systems composed of hydrogen (H 2 ) and lighter inert gas atoms (Rg) was considered.In this report a development of this research work is presented with more massive and highlypolarizable, Kr and Xe, perturbers involved. The collision-induced hyperpolarizability tensorialvalues, Δβ obtained by means of the QC ab initio methods are applied in order to producethe CIHRS spectral distributions; the inuence of Δβ features on the line shapes is comparedwith the earlier theoretical predictions. Namely, the validity of the multipole-induced-multipole(MIM) mechanism is assessed. In particular, its relevance to reproduce long-range functionalbehavior of the so-called symmetry adapted (SA) components of the hyperpolarizability tensorΔβ(R) is discussed. A thorough analysis of the translational CIHRS spectra is then performedto identify the role of the hyperpolarizability spatial distribution in forming particular sectionsof the line shapes. An extension of the dipole-induced-quadrupole analytical model is suggestedand tested with regard to its ability to reproduce more accurate proles

Nonlinear properties and collisional spectra in hydrogen-(heavy) noble-gas-atom mixtures