The experimental technique and applications of ultrafast two-dimensional infrared (2D IR) vibrational echo spectroscopy are presented. Using ultrashort infrared pulses and optical heterodyne detection to provide phase information, unique information can be obtained about the dynamics, interactions, and structures of molecular systems. The form and time evolution of the 2D IR spectrum permits examination of processes that cannot be studied with linear infrared absorption experiments. Three examples are given: organic solute-solvent complex chemical exchange, dynamics of the hydrogen-bond network of water, and assigning peaks in an IR spectrum of a mixture of species.
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