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Concentration studies of collision-induced fundamental absorption of hydrogen dissolved in liquid neon.

We report further and more detailed results of our recent investigation [W. A. Herrebout, B. J. van der Veken, and A. P. Kouzov, Phys. Rev. Lett. 101, 093001 (2008)] on the collision-induced fundamental absorption by hydrogen dissolved in liquid neon (T ≈ 25 K). The band shapes were studied in a wide range of concentrations (0.003-0.05 mole fractions) as well as for different ortho/para ratios and at much higher level of accuracy and resolution than before. Due to almost unhindered rotation of the hydrogen molecule and low temperature, an unprecedently rich frequency-domain picture produced by different terms of the interaction-induced polarization was observed. While some of them are conspicuous via fast intracell motion of a light guest (H(2)), others--induced by the electrostatic field of the guest--give rise to lines whose shapes are imprinted by fluctuations of the nearest surrounding. Strong motional narrowing observed on the guest-guest induced lines shows up in their Lorentzian shapes which are signatures of microscopic-scale diffusion. Near-Lorentzian peaks were also detected at the tops of the diffuse lines induced by isolated guests. Their formation may be associated with a long-living defect (vacancy) emerging in the vicinity of the polarization inductor. Altogether, our results give the first unambiguous spectroscopic evidence on the diffusional evolution of isolated binary interactions that emerge in dense chaotic media.