Spectroscopic investigation on intermolecular and intramolecular motions of concentrated aqueous KSCN solution

► Intermolecular and intramolecular motions of aqueous KSCN solution are studied. ► Concentrated aqueous KSCN solutions present large anisotropic hyperpolarizability. ► The 45 cm−1 vibration in aqueous KSCN solution is the librational motion of SCN−. ► SCN− severely distorts intermolecular hydrogen bond of water.