Formation of coherent rotational wavepackets in small molecule-helium clusters using impulsive alignment
Résumé
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, timedelayed
femtosecond laser pulse. By means of a Fourier transform a rich spectrum of
rotational eigenstates was derived. For the smallest cluster, C2H2–He, we were able
to establish essentially all rotational eigenstates up to the dissociation threshold on
the basis of theoretical level predictions. The C2H2–He complex is found to exhibit
distinct features of large amplitude motion and very early onset of free internal rotor
energy level structure.