Density functional computation revealed that in YOH solvation (Y = Li, Na, and K), the Y+ cation locates eccentrically at the interstitial hollow site to form the 4H(2)O unit, and the hydroxyl adds an excessive electron lone pair ":" to form a OH-center dot H2O unit where the hydroxide stays in the the center. The surrounding four oriented H2O neighbors interact with the Y+ through Y+ <-> H+ repulsion and Y+ :O2- attraction, causing the Y+ eccentric dislocation by some 0.80 angstrom. The ":" turns one O:H-O bond into the O:double left right arrow :O super hydrogen bond by altering H2O center dot 4H(2)O into HO-center dot 4H(2)O. The repulsive Y+ <-> H+ enlarges its separation and the attractive Y+:O shortens itself, showing the anisotropic polarization of the Y+ cation. The anisotropic Y+ polarizability, O: double left right arrow :O compressibility, and the H-O bond contraction of the solute OH- distorts the solute bonding network and disperses the O:H-O segmental phonon frequencies, as confirmed spectroscopically.