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

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posted on 13.11.2015, 16:32 by Gediminas Galinis, Luis G. Mendoza Luna, Mark J. Watkins, Andrew M. Ellis, R. S. Minns, M. Mladenović, M. Lewerenz, R. T. Chapman, I. C. Turcu, C. Cacho, E. Springate, L. Kazak, S. Göde, R. Irsig, S. Skruszewicz, J. Tiggesbäumker, K. H. Meiwes-Broer, A. Rouzée, J. G. Underwood, M. Siano, Klaus von Haeften
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.


The authors wish to thank STFC for access to the Artemis facility at the Rutherford Appleton Laboratory and the University of Leicester for funding to support the studentship for GG associated with this project. We would like to thank S. Hook, P. Rice, N. Rodrigues and S. Thornton for technical support during the experiment. KVH kindly acknowledges funding by STFC (seed corn fund for experiments using 4th generation light sources) and the Leverhulme Trust (F/00212/ AH). LGML acknowledges Financial support from the Mexican Consejo Nacional de Ciencia y Tecnologıa (CONACYT) Scholarship number 310668, ID 215334. RSM would like to thank the Royal Society for a University Research Fellowship (UF100047), ML and MM acknowledge computational resources funded through ANR grant ANR-08-BLAN-0146-01. KHMB and JT acknowledge Financial support by the Deutsche Forschungsgemeinschft through SFB 652.



Faraday Discussions, 2014, 171, pp. 195-218

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/Organisation/COLLEGE OF SCIENCE AND ENGINEERING/Department of Physics and Astronomy


AM (Accepted Manuscript)

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Faraday Discussions


Royal Society of Chemistry





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Electronic supplementary information (ESI) available. See DOI: 10.1039/c4fd00099d



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