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arXiv:0903.5413 · The Journal of Chemical Physics

Quantum-state selection, alignment, and orientation of large molecules using static electric and laser fields

Frank Filsinger, Jochen Küpper, Gerard Meijer, Lotte Holmegaard, Jens Hedegaard Nielsen, Iftach Nevo, Jonas L. Hansen, Henrik Stapelfeldt

Published Aug 14, 2009• 154 citations
arXivHTMLPDF

Abstract

Supersonic beams of polar molecules are deflected using inhomogeneous electric fields. The quantum-state selectivity of the deflection is used to spatially separate molecules according to their quantum state. A detailed analysis of the deflection and the obtained quantum-state selection is presented. The rotational temperatures of the molecular beams are determined from the spatial beam profiles and are all approximately 1 K. Unprecedented degrees of laser-induced alignment (<cos2 theta2D>=0.972) and orientation of iodobenzene molecules are demonstrated when the state-selected samples are used. Such state-selected and oriented molecules provide unique possibilities for many novel experiments in chemistry and physics.

DOI
10.1063/1.3194287

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Supersonic beams of polar molecules are deflected using inhomogeneous electric fields. The quantum-state selectivity of the deflection is used to spatially separate molecules according to their quantum state. A detailed analysis of the deflection and the obtained quantum-state selection is presented. The rotational temperatures of the molecular beams are determined from the spatial beam profiles and are all approximately 1 K. Unprecedented degrees of laser-induced alignment (<cos2 theta2D>=0.972) and orientation of iodobenzene molecules are demonstrated when the state-selected samples are used. Such state-selected and oriented molecules provide unique possibilities for many novel experiments in chemistry and physics.
Supersonic beams of polar molecules are deflected using inhomogeneous electric fields. The quantum-state selectivity of the deflection is used to spatially separate molecules according to their quantum state. A detailed analysis of the deflection and the obtained quantum-state selection is presented. The rotational temperatures of the molecular beams are determined from the spatial beam profiles and are all approximately 1 K. Unprecedented degrees of laser-induced alignment (<cos2 theta2D>=0.972) and orientation of iodobenzene molecules are demonstrated when the state-selected samples are used. Such state-selected and oriented molecules provide unique possibilities for many novel experiments in chemistry and physics.
A strong inhomogeneous static electric field is used to spatially disperse a supersonic beam of polar molecules, according to their quantum state. We show that the molecules residing in the lowest-lying rotational states can be selected and used as targets for further experiments. As an illustration, we demonstrate an unprecedented degree of laser-induced one-dimensional alignment (cos;(2)theta_(2D)=0.97) and strong orientation of state-selected iodobenzene molecules. This method should enable experiments on pure samples of polar molecules in their rotational ground state, offering new opportunities in molecular science.
The ability to deflect neutral polar molecules present in supersonic molecular beams using inhomogeneous electric fields is a consequence of these molecules possessing a dipole moment. As a dipole moment is inherently a quantum state-dependent feature, it can thus be exploited to allow spatial separation of neutral molecules in different quantum states. In this report, the Stark interaction was exploited to provide deflection of a gaseous sample of indole (C8H7N). Spatial profiles of the molecular beam at various electric field strengths were measured, showing an observed deviation in the beam path attributed to the indole molecules residing in different quantum states. These state-selected samples produced act as ideal samples for laser alignment techniques, in preparation for further experiments such as diffraction on gaseous molecular samples.
We consider deflection of polarizable molecules by inhomogeneous optical fields, and analyze the role of molecular orientation and rotation in the scattering process. We show that by preshaping molecular angular distribution with the help of short and strong femtosecond laser pulses, one may efficiently control the scattering process, manipulate the average deflection angle and its distribution, and reduce substantially the angular dispersion of the deflected molecules. This opens new ways for many applications involving molecular focusing, guiding, and trapping by optical and static fields.
In a typical experiment aiming to control quantum dynamics phenomena, each molecule experiences the same temporal laser field, but with an amplitude that depends on the spatial location and orientation of the molecule in the laser beam. It is proved under commonly arising conditions that at least one optimal laser field exists which will control all molecules in the sample, regardless of their orientation or spatial location. The optimal laser field may consist of a multipolarization control containing up to three orthogonal, independently shaped components. The analysis also includes the prospect of multipartite control where the field couples distinct groupings of states (e.g., multiple vibronic states), but without direct coupling within a group of states. This conclusion shows that achieving quantum control is not a matter of striking a compromise over the sample diversity, but rather a task subject to optimization to reach the highest possible level of control for all molecules in the sample.
The properties of molecule-optical elements such as lenses or prisms based on the interaction of molecules with optical fields depend in a crucial way on the molecular quantum state and its alignment created by the optical field. Herein, we consider the effects of state-dependent alignment in estimating the optical dipole force acting on the molecules and, to this end, introduce an effective polarizability which takes proper account of molecular alignment and is directly related to the alignment-dependent optical dipole force. We illustrate the significance of including molecular alignment in the optical dipole force by a trajectory study that compares previously used approximations with the present approach. The trajectory simulations were carried out for an ensemble of linear molecules subject to either propagating or standing-wave optical fields for a range of temperatures and laser intensities. The results demonstrate that the alignment-dependent effective polarizability can serve to provide correct estimates of the optical dipole force, on which a state-selection method applicable to nonpolar molecules could be based. We note that an analogous analysis of the forces acting on polar molecules subject to an inhomogeneous static electric field reveals a similarly strong dependence on molecular orientation.