Several optical techniques are used to characterize the ultrafast solvation dynamics of two structurally different molecules, LD690 and LDS750. Linear absorption, fluorescence, resonance Raman, and time-resolved four-wave mixing experiments have been performed on both molecules in a variety of solvents. The combination of different experiments is necessary to characterize the femtosecond dynamics. We find that both molecules exhibit very fast dephasing, due to sub-100 fs decays of the solvation correlation function M(t). The LD690 data is analyzed in depth, using a multimode oscillator model to treat both intramolecular vibrations and the solvent coordinates. The dynamics are solvent-dependent, but this dependence cannot be explained in a straightforward manner using quantities such as inertial solvent rotational motion or a simple dielectric continuum response. Various aspects of the spectroscopy, both linear and nonlinear, provide clues that the dynamics are influenced by molecular-level interactions that are not taken into account by theories that only consider bulk solvent properties.