Electrostatic interactions are pivotal in applications ranging from industrial rare earth separations to ion exchange membranes for batteries, and fuel cells. Historically from the inception of vibrational stark effect(VSE), molecular vibrations are long known to characterize electrostatic interactions at the atomic scale. Advanced spectroscopic tools such as pump-probe (PP) and two-dimensional infrared (2DIR) spectroscopy interrogate high frequency molecular vibrations on the picosecond timescale making them ideal tools to probe fluctuating electrostatic interactions in the condensed phase. In this talk I will discuss two studies using PP and 2DIR to probe electrostatic interactions. I will first discuss how vibrational anisotropy extracted from polarizationdependent pump-probe spectroscopy can measure the strength of the electrostatic interactions between the metal ion and ligand upon lanthanide binding. These studies demonstrate how vibrational dynamics of the ligand carboxylate groups can sense the large-scale conformational change of the ligand subjected to ion binding. I will then discuss how 2DIR can be used to sense the local environment of novel self-assembled ion exchange membranes, where the membranes are suitable for ion transport and filtration. Ionic interaction and associated water dynamics control the bulk scale transport properties through these membranes. From 2DIR spectra we extract ion specific spectral diffusion dynamics of the transporting ions. The spectra diffusion can be further linked to their activation barrier for ionic conductivity.