The nonlinear optical process of second harmonic generation (SHG) possesses an intrinsic sensitivity to the asymmetry present at the interface between two centrosymmetric media. We present results from our studies of equilibrium and time-dependent processes at the liquid-vapor interface using the method of SHG. Information on the orientational structure, concentration of solute molecules, and chemical equilibria at the water-vapor interface are discussed. Results from dynamic processes at the interface, such as excited- state relaxation, photoisomerization, and intermolecular energy transfer, are presented.

© 1989 Optical Society of America

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