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Manipulation and Control of Molecular Beams: The Development of the Stark-Decelerator

Gerard Meijer

Published Jan 1, 2021• 3 citations
Publisher

Abstract

Abstract State-selective manipulation of beams of atoms and molecules with electric and magnetic fields has been crucial for the success of the field of molecular beams. Originally, this manipulation only involved the transverse motion. In this Chapter, the development of the Stark-decelerator, that allows to also manipulate and control the longitudinal motion of molecules in a beam, is presented.

DOI
10.1007/978-3-030-63963-1_20

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Abstract State-selective manipulation of beams of atoms and molecules with electric and magnetic fields has been crucial for the success of the field of molecular beams. Originally, this manipulation only involved the transverse motion. In this Chapter, the development of the Stark-decelerator, that allows to also manipulate and control the longitudinal motion of molecules in a beam, is presented.
The motion of molecules that possess a permanent electric or magnetic dipole moment can be manipulated using electric or magnetic fields. Various devices have been developed over the last few decades to deflect or focus molecules, to orient them in space, and to decelerate or accelerate them. These precisely controlled molecules are ideal starting points for scattering experiments that reveal the quantum mechanical nature of molecular interactions. In this Tutorial Review, we present an overview of the various manipulation tools, discuss how they can be used to advantage in molecular beam scattering experiments, and review recent progress in this field. We describe a selection of benchmark experiments that illustrate the unique possibilities that are available nowadays to study molecular collisions under controlled conditions.
In the last two decades, enormous progress has been made in the manipulation of molecular beams. In particular, molecular decelerators have been developed with which advanced control over neutral molecules in a beam can be achieved. By using arrays of inhomogeneous and time-varying electric (or magnetic) fields, bunches of molecules can be produced with a tunable velocity, narrow velocity spreads, and almost perfect quantum-state purity. These monochromatic or "tamed" molecular beams are ideally suited to be used in crossed-molecular-beam scattering experiments. Here, we review the first generation of these "cold and controlled" scattering experiments that have been conducted in the last decade and discuss the prospects for this emerging field of research in the years to come.
The motion of polar molecules can be controlled by time-varying inhomogeneous electric fields. In a Stark decelerator, this is exploited to accelerate, transport, or decelerate a fraction of a molecular beam. When combined with a trap, the decelerator provides a means to store the molecules for times up to seconds. Here, we review our efforts to produce cold molecules via this technique. In particular, we present a new generation Stark decelerator and electrostatic trap that selects a significant part of a molecular beam pulse that can be loaded into the trap. Deceleration and trapping experiments using a beam of OH radicals are discussed.
The motion of polar molecules can be controlled by time-varying inhomogeneous electric fields. In a Stark decelerator, this is exploited to select a fraction of a molecular beam that is accelerated, transported, or decelerated. Phase stability ensures that the selected bunch of molecules is kept together throughout the deceleration process. In this paper an extended description of phase stability in a Stark decelerator is given, including higher-order effects. This analysis predicts a wide variety of resonances that originate from the spatial and temporal periodicity of the electric fields. These resonances are experimentally observed using a beam of OH $(^{2}\ensuremath{\Pi}_{3∕2},v=0,J=3∕2)$ radicals passing through a Stark decelerator.
The large electric dipole moments associated with highly excited Rydberg states of atoms and molecules make gas-phase samples in these states very well suited to deceleration and trapping using inhomogeneous electric fields. The methods of Rydberg-Stark deceleration with which this can be achieved are reviewed here. Using these techniques, the longitudinal motion of beams of atoms and molecules moving at speeds as high as 2500 m/s have been manipulated, with changes in kinetic energy of up to |Δ E kin|=1.3×10−20 J (|Δ E kin|/e=80 meV or |Δ E kin|/h c=650 cm −1) achieved, while decelerated and trapped samples with number densities of 106– 107 cm −3 and translational temperatures of ∼150 mK have been prepared. Applications of these samples in areas of research at the interface between physics and physical chemistry are discussed.
With a Stark decelerator, beams of neutral polar molecules can be accelerated, guided at a constant velocity, or decelerated. The effectiveness of this process is determined by the six-dimensional (6D) volume in phase space from which molecules are accepted by the Stark decelerator. Couplings between the longitudinal and transverse motion of the molecules in the decelerator can reduce this acceptance. These couplings are nearly absent when the decelerator operates such that only every third electric-field stage is used for deceleration, while extra transverse focusing is provided by the intermediate stages. For many applications, the acceptance of a Stark decelerator in this so-called s=3s=3s=3 mode significantly exceeds that of a decelerator in the conventionally used (s=1)(s=1)(s=1) mode. This has been experimentally verified by passing a beam of OH radicals through a $2.6\text{\ensuremath{-}}\mathrm{m}$-long Stark decelerator. The experiments are in quantitative agreement with the results of trajectory calculations, and can qualitatively be explained with a simple model for the 6D acceptance. These results imply that the 6D acceptance of a Stark decelerator in the s=3s=3s=3 mode of operation approaches the optimum value, i.e., the value that is obtained when any couplings are neglected.