When salts are added to water, the viscosity generally increases suggesting the ions increase the strength of the water's hydrogen-bond network. However, infrared pump-probe measurements on electrolyte solutions have found that ions have no influence on the rotational dynamics of water molecules implying no enhancement or breakdown of the hydrogen-bond network. Here we report optical Kerr-effect and dielectric relaxation spectroscopic measurements, which have enabled us to separate the effects of rotational and transitional motions of the water molecules. These data show that electrolyte solutions behave like a supercooled liquid approaching a glass transition in which rotational and translational molecular motions are decoupled. It is now possible to understand previously conflicting viscosity data, nuclear magnetic resonance relaxation, and ultrafast infrared spectroscopy in a single unified picture.It is well known that when salts are added to water the viscosity typically increases, suggesting that the ions alter the hydrogen-bond network of the water, 1 which appears to be confirmed by, for example, neutron diffraction experiments. 2 However, recent ultrafast infrared pump-probe measurements on electrolyte solutions have found that ions do not influence the rotational dynamics of water molecules suggesting that there is no enhancement or breakdown of the hydrogen-bond network in liquid water. 3 As the effect of ions and ionic moieties on the structure of water is important for understanding protein stability, enzymatic reactions, and substrate binding, it is crucial to resolve this paradox. 4 Here we report ultrafast optical Kerr effect 5 (OKE) and dielectric relaxation 6 (DR) spectroscopy measurements, which show that salt solutions behave like a supercooled liquid approaching a glass transition, where rotational and translational molecular motions become decoupled. The rotational motions of bulk water molecules -observed as an -relaxation in DR -are essentially independent of concentration. The translational motions seen in OKE spectroscopy can be understood as a -relaxation 7 and their dynamics become increasingly inhomogeneous with increasing salt concentration. This insight reconciles previously conflicting viscosity data, 8 nuclear magnetic resonance relaxation, 9 and ultrafast infrared spectroscopy 3 data in a single unifying picture.When simple inorganic salts are added to water, the viscosity typically increases ( see FIG. 1). In the relatively low concentration range (up to ~0.5 M), this is described by the semi-empirical Jones-Dole equation, 1 , which expresses the shear viscosity in terms of the viscosity of pure water 0 , salt concentration c, and parameters A and B. For many salts additional terms have to be added to describe the rapid increase in viscosity at higher concentrations. The obvious conclusion to draw from this behavior is that ions alter the structure of water. Indeed, the empirical Jones-Dole B coefficient is often used to classify ions as either structure makers (kosmotropes...