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Issue 42, 2011
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Theoretical description of adiabatic laser alignment and mixed-field orientation: the need for a non-adiabatic model

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Abstract

We present a theoretical study of recent laser-alignment and mixed-field-orientation experiments of asymmetric top molecules. In these experiments, pendular states were created using linearly polarized strong ac electric fields from pulsed lasers in combination with weak electrostatic fields. We compare the outcome of our calculations with experimental results obtained for the prototypical large molecule benzonitrile (C7H5N) [J. L. Hansen et al., Phys. Rev. A, 2011, 83, 023406.] and explore the directional properties of the molecular ensemble for several field configurations, i.e., for various field strengths and angles between ac and dc fields. For perpendicular fields one obtains pure alignment, which is well reproduced by the simulations. For tilted fields, we show that a fully adiabatic description of the process does not reproduce the experimentally observed orientation, and it is mandatory to use a diabatic model for population transfer between rotational states. We develop such a model and compare its outcome to the experimental data confirming the importance of non-adiabatic processes in the field-dressed molecular dynamics.

Graphical abstract: Theoretical description of adiabatic laser alignment and mixed-field orientation: the need for a non-adiabatic model

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Article information


Submitted
15 Apr 2011
Accepted
01 Jun 2011
First published
29 Jun 2011

Phys. Chem. Chem. Phys., 2011,13, 18815-18824
Article type
Paper

Theoretical description of adiabatic laser alignment and mixed-field orientation: the need for a non-adiabatic model

J. J. Omiste, M. Gärttner, P. Schmelcher, R. González-Férez, L. Holmegaard, J. H. Nielsen, H. Stapelfeldt and J. Küpper, Phys. Chem. Chem. Phys., 2011, 13, 18815
DOI: 10.1039/C1CP21195A

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