27 research outputs found
Probing the structure and dynamics of molecular clusters using rotational wavepackets
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.Comment: 5 pages, 6 figure
Formation of coherent rotational wavepackets in small molecule-helium clusters using impulsive alignment.
We show that rotational line spectra of molecular clusters with near zero permanent dipole moments can be observed using impulsive alignment. Aligned rotational wavepackets were generated by non-resonant interaction with intense femtosecond laser pump pulses and then probed using Coulomb explosion by a second, time-delayed femtosecond laser pulse. By means of a Fourier transform a rich spectrum of rotational eigenstates was derived. For the smallest cluster, C(2)H(2)-He, we were able to establish essentially all rotational eigenstates up to the dissociation threshold on the basis of theoretical level predictions. The C(2)H(2)-He complex is found to exhibit distinct features of large amplitude motion and very early onset of free internal rotor energy level structure