Femtosecond pump—probe study of the spreading and recurrence of a vibrational wave packet in Na2

The motion of a vibrational wave packet in the bound A (1Σu+) electronic state of the sodium dimer is detected in a femtosecond pump/probe molecular beam experiment. For short times harmonic motion is seen in the total ion yield of Na2+ as a function of delay time between the two laser pulses. The spreading of the wave packet results in the loss of the periodic variation of the ion signal. For longer delay times (47 ps) the wave packet regains its initial form which is reflected in the revival structure of the Na2+ signal. Time-dependent quantum calculations reproduce the measured effects.