Molecular assemblies at liquid interfaces probed by optical second-harmonic generation

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Abstract
Surface second harmonic generation (SHG) has recently emerged as a promising new technique capable of probing the molecular organization at liquid interfaces. It provides information on the number of molecules adsorbed, the orientation and local environment of specific residues, and confers the ability to assess the symmetry of the intermolecular arrangement. Previously, SHG had been applied in the study of simple model systems where the major signal contributions originated from dye chromophores. Here we show SHG to be sensitive to submonolayer densities of the aromatic amino acids tryptophan, tyrosine, and phenylalanine adsorbed to the air/water interface, with the strongest resonant enhancement at the second harmonic wavelength of 266 nm being found for tryptophan. This observation opens the door for probing the ordering of peptides at liquid interfaces by exploiting the nonlinear optical properties of the tryptophan residues.

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