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Brief Description of SFG

Second-order NLO processes, including SFG, are strictly forbidden in media with inversion symmetry under the electric dipole approximation and are allowed only at the interface between these media where the inversion symmetry is necessarily broken. In the IR-Visible SFG measurement, a visible laser beam (covis) and a tunable infrared laser beam (cOir) are overlapped at an interface and the SFG signal is measured by scanning cOir while keeping cOvis constant. The SFG intensity (Isfg) is enhanced when coir becomes equal to the vibration levels of the molecules at the interface. Thus, one can obtain surface-specific vibrational spectra at an interface [Pg.72]

In addition to the surface/interface selectivity, IR-Visible SFG spectroscopy provides a number of attractive features since it is a coherent process (i) Detection efficiency is very high because the angle of emission of SFG light is strictly determined by the momentum conservation of the two incident beams, together with the fact that SFG can be detected by a photomultiplier (PMT) or CCD, which are the most efficient light detectors, because the SFG beam is in the visible region, (ii) The polarization feature that NLO intrinsically provides enables us to obtain information about a conformational and lateral order of adsorbed molecules on a flat surface, which cannot be obtained by traditional vibrational spectroscopy [29-32]. (iii) A pump and SFG probe measurement can be used for an ultra-fast dynamics study with a time-resolution determined by the incident laser pulses [33-37]. (iv) As a photon-in/photon-out method, SFG is applicable to essentially any system as long as one side of the interface is optically transparent. [Pg.73]


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