Abstract

The dynamics of vibrational wave packets in triplet states of rubidium dimers $({\text{Rb}}_{2})$ formed on helium nanodroplets are studied using femtosecond pump-probe photoionization spectroscopy. Due to fast desorption of the excited ${\text{Rb}}_{2}$ molecules off the droplets and due to their low internal temperature, wave-packet oscillations can be followed up to very long pump-probe delay times $\ensuremath{\gtrsim}1.5\text{ }\text{ns}$. In the first-excited triplet state $(1){^{3}\ensuremath{\Sigma}}_{g}^{+}$, full and fractional revivals are observed with high contrast. Fourier analysis provides high-resolution vibrational spectra which are in excellent agreement with ab initio calculations.

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