Abstract
To evaluate the inhomogeneity of the solvation environment at the air/water interface, we quantitatively analyzed the shape of the electronic spectra at the air/water interface for the first time. We measured the interface-selective electronic χ(2) (second-order nonlinear susceptibility) spectra of solvatochromic coumarin molecules at the air/water interface by heterodyne-detected electronic sum frequency generation (HD-ESFG) spectroscopy. The observed imaginary χ(2) (Im[χ(2)]) spectra were well reproduced by the convolution of a line shape function with a Gaussian distribution of a frequency shift, which enabled us to quantitatively determine the peak position and bandwidth of the Im[χ(2)] spectra. The effective polarity of the air/water interface, which was determined by the peak position, was found to be dependent on each coumarin, which agreed with our previous homodyne-detected ESFG study. Interestingly, the spectra at the air/water interface showed substantially broader bandwidths than those in equa...
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