  The chemical and physical properties of molecular clusters can heavily depend
on their size, which makes them very attractive for the design of new materials
with tailored properties. Deriving the structure and dynamics of clusters is
therefore of major interest in science. Weakly bound clusters can be studied
using conventional spectroscopic techniques, but the number of lines observed
is often too small for a comprehensive structural analysis. Impulsive alignment
generates rotational wavepackets, which provides simultaneous information on
structure and dynamics, as has been demonstrated successfully for isolated
molecules. Here, we apply this technique for the firsttime to clusters
comprising of a molecule and a single helium atom. By forcing the population of
high rotational levels in intense laser fields we demonstrate the generation of
rich rotational line spectra for this system, establishing the highly
delocalised structure and the coherence of rotational wavepacket propagation.
Our findings enable studies of clusters of different sizes and complexity as
well as incipient superfluidity effects using wavepacket methods.
