Vibrational Anharmonicities Revealed by Coherent Two-Dimensional Infrared Spectroscopy

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.