The main experimental techniques used in the research include ultrafast two dimensional infrared 2D IR vibrational echo experiments, IR polarization selective pump-probe PP and heterodyne detected transient grating HDTG experiments, and optical heterodyne detected optical Kerr effect OHD-OKE experiments. The first 2D IR experiments on functionalized SiO2 planar surface monolayers of alkyl chains with a vibrational probe head group were performed. Room temperature ionic liquids were also investigated. Room temperature ionic liquids RTIL are intrinsically interesting because they simultaneously have properties that are similar to organic liquids and liquid salts. In addition, RTILs are increasingly being considered for and used in technological applications. Metal-organic frame works were also investigated. A unique aspect of metal-organic frameworks MOFs is their structural flexibility coexisting with a degree of regularity. We showed that two-dimensional infrared2D IR spectroscopy with pulse-shaping techniques can probe the ultrafast structural fluctuations of MOFs in spite of seeming insurmountable experimental problems and obtained the first measurements of framework dynamics.