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Faraday Discuss. 2014;171:195-218. doi: 10.1039/c4fd00099d. Epub 2014 Aug 04.

Formation of coherent rotational wavepackets in small molecule-helium clusters using impulsive alignment.

Faraday discussions

Gediminas Galinis, Luis G Mendoza Luna, Mark J Watkins, Andrew M Ellis, Russell S Minns, Mirjana Mladenović, Marius Lewerenz, Richard T Chapman, I C Edmond Turcu, Cephise Cacho, Emma Springate, Lev Kazak, Sebastian Göde, Robert Irsig, Slawomir Skruszewicz, Josef Tiggesbäumker, Karl-Heinz Meiwes-Broer, Arnaud Rouzée, Jonathan G Underwood, Marco Siano, Klaus von Haeften

Affiliations

  1. University of Leicester, Department of Physics & Astronomy, Leicester, LE1 7RH, UK. [email protected].

PMID: 25415646 DOI: 10.1039/c4fd00099d

Abstract

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.

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