An alkylsilane monolayer functionalized with a metal carbonyl complex was prepared on a planar SiO2 surface. The CO stretching mode of the complex was used as a vibrational probe for nonlinear infrared spectroscopy. The interfacial solvent dynamics were indirectly observed when two-dimensional infrared (2D IR) spectroscopy was applied to the functionalized monolayer immersed in several solvents. Ultrafast in-plane and out-of-plane motions of the planar monolayer were studied by polarization-resolved heterodyne-detected transient grating (HDTG) spectroscopy. The same strategy was employed to probe the dynamics inside the pores of porous silica (SBA-15) particles. The wall inside the pores was functionalized with the same metal complex. With the use of phase cycling and polarization filtering, 2D IR spectra free from the contamination by scattered pump beams were obtained to report on the unique molecular dynamics inside the pores.

Ultrafast molecular dynamics at functionalized interfaces probed by nonlinear infrared spectroscopy

248th National Meeting (2014)

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