Ultrafast time resolution would be required for the study of strongly H-bonded systems, where H-bonded OH or NH groups often display surprisingly broad transitions even under cryogenic conditions. This spectral breadth is predicted to arise from strong anharmonic coupling to lower-frequency modes, which will result in rapid relaxation dynamics of the excited OH/NH stretch. TA and 2D-CIVS can be used to track the vibrational energy relaxation pathways in these systems. Further, 2D-CIVS would be able to reveal homogeneous vs. inhomogeneous contributions to broad OH/NH stretch lineshapes and track frequency-frequency correlation dynamics (spectral diffusion) as energy relaxes into low-frequency soft modes. Finally, vibrational dynamics on excited electronic states can be measured using UV/Vis pump-IR probe TA-CIVS, providing an exciting possible avenue for the study of photoinduced reaction dynamics and mechanisms.