Room temperature ionic liquids (RTILs) are fluids composed entirely of ions. Their liquid-state dynamics are expected to be very complex because of the molecular structure of the ions and the nature of the intermolecular interactions. The properties of RTILs make them potential replacements for many volatile organic liquids currently in use as solvents. Moreover, the negligible volatility of RTILs eliminates the health and environmental risks posed by fugitive solvent emissions. The understanding of the structure-function relationships developed with regards to the microscopic dynamics in the proposed study will be of great value to those seeking to understand RTILs and to tailor them for specific applications. Computer simulations have recently shown that RTILs based on the 1-alkyl-3-methylimidazolium cation ([Cnmim]+) with alkyl chains C4 and longer are nanostructurally organized with polar regions arising from charge ordering and nonpolar regions arising from clustering of the alkyl chains. The polar regions are in the form of three-dimensional networks which are permeated by the nonpolar regions. Nanostructural organization is a promising development in the field of ionic liquids because it provides a conceptual framework for interpreting not only the physical properties but the microscopic dynamics of RTILs as well. Using femtosecond optical heterodyne-detected Raman-induced Kerr effect spectroscopy (OHD-RIKES), we have studied the low-frequency intermolecular or optical Kerr effect (OKE) spectra of various RTIL systems. The OKE spectra provide further insights into the nature of the nanostructural organization in these fascinating materials.