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• W2016136602 abstract "High-resolution infrared absorption spectroscopy has been used to study the roto-vibrational spectra of cyanide ions doped into KCl for the two isotopes $^{12}mathrm{C}$ $^{14}mathrm{N}^{mathrm{ensuremath{-}}}$ and $^{13}mathrm{C}$ $^{15}mathrm{N}^{mathrm{ensuremath{-}}}$ in the temperature range 1.7--300 K. At the lowest temperature studied, new structure has been resolved in the spectra for low dopant concentrations (0.01 mol %). This structure is observed to merge into a single peak when strains are introduced into the crystal, confirming the association of these lines with tunneling by isolated cyanide ions. The structure is only partially explained by the Devonshire potential. Above 100 K, the isotopic variation in the experimental data is quantified in terms of a single global parameter, an integrated ratio of the widths of the entire roto-vibrational manifolds for the two isotopes, at each temperature. The values of this parameter turn out to be much smaller than what is predicted by a straightforward model of a cyanide dipole freely rotating in a crystalline host, but are consistent with a dressed-rotor model.By allowing a rotating cyanide ion to elastically distort the equilibrium structure of the surrounding lattice, and by using an adiabatic approximation and suitable averaging procedures, it is explicitly shown that an enhanced value for the moment of inertia of the dipole results. This model is fitted to the KCl:K $^{12}mathrm{C}$ $^{14}mathrm{N}$ spectra with the following free parameters: the rotational constant (in both the ground and excited vibrational levels), the Devonshire-potential-barrier parameter, and the widths of the roto-vibrational lines, with the result that the computed isotope effect is in good agreement with the experimental values. The best-fit values for these fitting parameters are found to be temperature dependent; the dressed moment of inertia of the ${mathrm{CN}}^{mathrm{ensuremath{-}}}$ ion increases with increasing temperature, in contrast to a naive expectation that the rotor should become more nearly free as the average lattice cage size increases. In similar fashion, for the fits to the room-temperature spectra measured for cyanide doped in eight other alkali halide hosts, the dressed moment of inertia tends, on average, to increase with increasing lattice spacing. Our model correctly predicts this trend in the data, although it fails to explain the observed magnitude of the effect. Furthermore, even after allowing these parameters to vary with temperature, detailed agreement between theory and experiment for the roto-vibrational manifold shape was not obtained." @default.
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• W2016136602 date "1991-01-01" @default.
• W2016136602 modified "2023-09-27" @default.
• W2016136602 title "Infrared spectroscopic study of the dressed rotations of<mml:math xmlns:mml=http://www.w3.org/1998/Math/MathML display=inline><mml:mrow><mml:msup><mml:mrow><mml:mi mathvariant=normal>CN</mml:mi></mml:mrow><mml:mrow><mml:mi mathvariant=normal>−</mml:mi></mml:mrow></mml:msup></mml:mrow></mml:math>isotopes in alkali halide crystals" @default.
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• W2016136602 doi "https://doi.org/10.1103/physrevb.43.43" @default.
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