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Comprehensive investigation of vibrational relaxation of non-hydrogen-bonded water molecules in liquids
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Image of FIG. 1.
FIG. 1.

(a) Vibrational energy levels and relaxation channels of monomeric water molecules after OH bend (left-hand side) and OH stretch excitation (right-hand side). (b) Possible IR transitions observable OH bend (left-hand side) and OH stretch excitation (right-hand side); the anharmonic shift of each transition is given in terms of the respective anharmonic constant .

Image of FIG. 2.
FIG. 2.

Numerical simulations of excess population on the vibrational modes ⟨100∣, ⟨001∣, ⟨020∣, and ⟨100∣ after ⟨001∣ excitation: (a) , (b) , and (c) . (d) Population difference : positive values representing stimulated emission (for details see text).

Image of FIG. 3.
FIG. 3.

Transient spectra of in in the OH bending region, measured after excitation of symmetric OH stretch (circles), antisymmetric OH stretch (squares), and OH bend (triangles); individual curves normalized and vertically shifted for clarity.

Image of FIG. 4.
FIG. 4.

Transient spectrum of in in the OH stretching region after excitation of symmetric OH bending mode: squares represent experimental data and vertical lines specify the position of the four Lorentzian lines of the best fit curve (solid curve).

Image of FIG. 5.
FIG. 5.

Transient time traces obtained after excitation of the antisymmetric OH stretch for in (left-hand side) [(a) and (b)] and in (right-hand side) [(c) and (d)]. The upper panels [(a) and (c)] refer to experiments with identical pump and probe frequency, the lower ones [(b) and (d)] were measured in the individual maximum of induced absorption. Experimental points and calculated curves; for details see text.


Generic image for table
Table I.

(Upper part) Fundamental frequencies and bandwidths of molecule in gas phase (after Ref. 16) and in the solvents and in liquid phase. (Lower part) Anharmonic constants of molecule, as obtained in this work; values for gas phase (also from Ref. 16) for comparison.


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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Comprehensive investigation of vibrational relaxation of non-hydrogen-bonded water molecules in liquids