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Two-dimensional vibronic spectroscopy of coherent wave-packet motion.

We theoretically study two-dimensional (2D) spectroscopic signals obtained from femtosecond pulse interactions with diatomic molecules. The vibrational wave-packet dynamics is monitored in the signals. During the motion in anharmonic potentials the wave packets exhibit vibrational revivals and fractional revivals which are associated with particular quantum phases. The time-dependent phase changes are identified by inspection of the complex-valued 2D spectra. We use the Na(2) molecule as a numerical example and discuss various pulse sequences which yield information about vibrational level structure and phase relationships in different electronic states.