Abstract
Novel interface-selective second-(χ(2)) and fourth-order (χ(4)) nonlinear spectroscopic techniques were developed to study liquid interfaces. χ(2) electronic sum frequency generation (ESFG) spectroscopy enabled us to obtain interfacial electronic spectra with an unprecedented high signal-to-noise ratio and dense wavelength data points, whereas frequency-domain χ(4) Raman spectroscopy provided vibrational spectra of solute molecules adsorbed at interfaces for the whole fingerprint region. Because these new even-order electronic and vibrational nonlinear spectroscopies utilize only visible and near-infrared laser pulses, they are applicable to the study of a variety of “buried” interfaces.
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