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Issue 7, 2007
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Ultrafast dynamics of halogens in rare gas solids

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Abstract

We perform time resolved pump–probe spectroscopy on small halogen molecules ClF, Cl2, Br2, and I2 embedded in rare gas solids (RGS). We find that dissociation, angular depolarization, and the decoherence of the molecule is strongly influenced by the cage structure. The well ordered crystalline environment facilitates the modelling of the experimental angular distribution of the molecular axis after the collision with the rare gas cage. The observation of many subsequent vibrational wave packet oscillations allows the construction of anharmonic potentials and indicate a long vibrational coherence time. We control the vibrational wave packet revivals, thereby gaining information about the vibrational decoherence. The coherence times are remarkable larger when compared to the liquid or high pressure gas phase. This fact is attributed to the highly symmetric molecular environment of the RGS. The decoherence and energy relaxation data agree well with a perturbative model for moderate vibrational excitation and follow a classical model in the strong excitation limit. Furthermore, a wave packet interferometry scheme is applied to deduce electronic coherence times. The positions of those cage atoms, excited by the molecular electronic transitions are modulated by long living coherent phonons of the RGS, which we can probe via the molecular charge transfer states.

Graphical abstract: Ultrafast dynamics of halogens in rare gas solids

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Article information


Submitted
26 Jun 2006
Accepted
16 Nov 2006
First published
06 Dec 2006

Phys. Chem. Chem. Phys., 2007,9, 779-801
Article type
Invited Article

Ultrafast dynamics of halogens in rare gas solids

M. Gühr, M. Bargheer, M. Fushitani, T. Kiljunen and N. Schwentner, Phys. Chem. Chem. Phys., 2007, 9, 779
DOI: 10.1039/B609058N

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