Abstract
Novel interface-selective second-order (χ (2) ) and fourth-order (χ (4) ) nonlinear spectroscopic techniques were developed to study liquid interfaces. χ (2) electronic sum frequency generation (ESFG) spectroscopy provides interfacial electronic spectra with an unprecedented high signaltonoise ratio in a short measurement time, whereas frequencydomain χ (4) Raman spectroscopy realized observation of vibrational spectra of solute molecules adsorbed at interfaces for the whole fingerprint region. Because these new evenorder electronic and vibrational nonlinear spectroscopies utilize only visible and nearinfrared laser pulses, they are applicable to the study of a variety of “buried” interfaces.
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