Time-resolved surface second harmonic generation has been used to study the picosecond rotational relaxation dynamics of free Rhodamine 6G molecules at the air/water interface. It was found that different elements of the second-order nonlinear susceptibility, chi-(2)ijk, show different kinetics, which indicates that rotational motions have been observed. The data also suggest that the observed rotational relaxation is due chiefly to the out-of-plane motions at the interface and that the ground- and excited-state molecules have different equilibrium orientational distributions.
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页码:6752 / 6753
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Alfano R. R., 1973, Optics Communications, V7, P191, DOI 10.1016/0030-4018(73)90007-2