Vibrational Anharmonicities Revealed by Coherent Two-Dimensional Infrared Spectroscopy

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Abstract
Two-dimensional infrared photon echo spectroscopy has been used to describe the anharmonic nuclear potential of two coupled molecular vibrations. The two-dimensional spectrum shows diagonal and off-diagonal features, each composed of two peaks. The splitting between these peaks is directly related to the anharmonicity, while the relative amplitude of the diagonal and off-diagonal features describes the projection angle between interacting dipoles.