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Published Online: 20 December 2013
Accepted: December 2013

Mixed-field orientation of molecules without rotational symmetry

J. Chem. Phys. 139, 234313 (2013); https://doi.org/10.1063/1.4848735
Jonas L. Hansen1, Juan J. Omiste2, Jens H. Nielsen3, a), Dominik Pentlehner4, Jochen Küpper5,6,7, Rosario González-Férez2,7, and Henrik Stapelfeldt1,4
more...View Affiliations
  • 1Interdisciplinary Nanoscience Center (iNANO), Aarhus University, 8000 Aarhus C, Denmark
  • 2Instituto Carlos I de Física Teórica y Computacional and Departamento de Física Atómica, Molecular y Nuclear, Universidad de Granada, 18071 Granada, Spain
  • 3Department of Physics and Astronomy, Aarhus University, 8000 Aarhus C, Denmark
  • 4Department of Chemistry, Aarhus University, 8000 Aarhus C, Denmark
  • 5Center for Free-Electron Laser Science, DESY, 22607 Hamburg, Germany
  • 6Department of Physics, University of Hamburg, 22761 Hamburg, Germany
  • 7The Hamburg Center for Ultrafast Imaging, University of Hamburg, 22761 Hamburg, Germany

  • a)Current address: Research Software Development Team, Research Computing and Facilitating Services, University College London, Gower Street, London, WC1E 6BT, United Kingdom.

Abstract
The mixed-field orientation of an asymmetric-rotor molecule with its permanent dipole moment nonparallel to the principal axes of polarizability is investigated experimentally and theoretically. We find that for the typical case of a strong, nonresonant laser field and a weak static electric field complete 3D orientation is induced if the laser field is elliptically polarized and if its major and minor polarization axes are not parallel to the static field. For a linearly polarized laser field solely the dipole moment component along the most polarizable axis of the molecule is relevant resulting in 1D orientation even when the laser polarization and the static field are nonparallel. Simulations show that the dipole moment component perpendicular to the most-polarizable axis becomes relevant in a strong dc electric field combined with the laser field. This offers an alternative approach to 3D orientation by combining a linearly polarized laser field and a strong dc electric field arranged at an angle equal to the angle between the most polarizable axis of the molecule and its permanent dipole moment.

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