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Physical Review Letters

Alternate Gradient Focusing and Deceleration of a Molecular Beam

Hendrick L. Bethlem, André J. A. van Roij, Rienk T. Jongma, Gerard Meijer

Published Mar 18, 2002• 121 citations
Publisher

Abstract

Neutral dipolar molecules can be decelerated and trapped using time-varying inhomogeneous electric fields. This has been demonstrated only for molecules in low-field seeking states, but can, in principle, be performed on molecules in high-field seeking states as well. Transverse stability is then much more difficult to obtain, however, since molecules in high-field seeking states always experience a force towards the electrodes. Here we demonstrate that an array of dipole lenses in alternate gradient configuration can be used to maintain transverse stability. A pulsed beam of metastable CO in high-field seeking states is accelerated from 275 to 289 m/s as well as decelerated from 275 to 260 m/s.

DOI
10.1103/physrevlett.88.133003

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Neutral dipolar molecules can be decelerated and trapped using time-varying inhomogeneous electric fields. This has been demonstrated only for molecules in low-field seeking states, but can, in principle, be performed on molecules in high-field seeking states as well. Transverse stability is then much more difficult to obtain, however, since molecules in high-field seeking states always experience a force towards the electrodes. Here we demonstrate that an array of dipole lenses in alternate gradient configuration can be used to maintain transverse stability. A pulsed beam of metastable CO in high-field seeking states is accelerated from 275 to 289 m/s as well as decelerated from 275 to 260 m/s.
Beams of polar molecules can be focused using an array of electrostatic lenses in alternating gradient (AG) configuration. They can also be accelerated or decelerated by applying an appropriate high-voltage switching sequence to the lenses. AG focusing is applicable to molecules in both low-field- and high-field-seeking states and is particularly well suited to the problem of decelerating heavy molecules and those in their ground rotational state. We describe the principles of AG deceleration and set out criteria to be followed in decelerator design, construction and operation. We calculate the longitudinal and transverse focusing properties of a decelerator, and exemplify this by 2D-imaging studies of a decelerated beam of metastable CO molecules.
We have focused and decelerated benzonitrile (C7H5N)({\mathrm{C}}_{7}{\mathrm{H}}_{5}\mathrm{N})(C7​H5​N) molecules from a molecular beam, using an array of time-varying inhomogeneous electric fields in alternating-gradient configuration. Benzonitrile is prototypical for large asymmetric top molecules that exhibit rich rotational structure and a high density of states. At the rotational temperature of 3.5K3.5\phantom{\rule{0.3em}{0ex}}\mathrm{K}3.5K in the pulsed molecular beam, many rotational states are populated. Benzonitrile molecules in their absolute ground state are decelerated from 320to289m∕s320\phantom{\rule{0.3em}{0ex}}\text{to}\phantom{\rule{0.3em}{0ex}}289\phantom{\rule{0.3em}{0ex}}\mathrm{m}∕\mathrm{s}320to289m∕s, and similar changes in velocity are obtained for excited rotational states. All measurements agree well with the outcome of trajectory calculations. These experiments demonstrate that such large polyatomic molecules are amenable to the powerful method of Stark deceleration.
It is experimentally demonstrated that a beam of neutral dipolar molecules can be efficiently decelerated with a time-varying electric field. A pulsed beam of neutral metastable CO molecules is slowed down from 225 m/s ( ${E}_{\mathrm{kin}}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}59{\mathrm{cm}}^{\ensuremath{-}1}$) to 98 m/s ( ${E}_{\mathrm{kin}}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}11{\mathrm{cm}}^{\ensuremath{-}1}$) upon passage through an array of 63 synchronously pulsed electric field stages.
A polar molecule experiences a force in an inhomogeneous electric field. Using this force, neutral molecules can be decelerated and trapped. It is shown here that this can in principle be done without loss in phase-space density. Using a series of 64 pulsed inhomogeneous electric fields a supersonic beam of ammonia molecules (14NH3,{(}^{14}{\mathrm{NH}}_{3},(14NH3​, 14ND3,{}^{14}{\mathrm{ND}}_{3},14ND3​, 15ND3){}^{15}{\mathrm{ND}}_{3})15ND3​) is decelerated. Subsequently, the decelerated molecules are loaded into an electrostatic quadrupole trap. Densities on the order of 107molecules/cm3{10}^{7} {\mathrm{m}\mathrm{o}\mathrm{l}\mathrm{e}\mathrm{c}\mathrm{u}\mathrm{l}\mathrm{e}\mathrm{s}/\mathrm{c}\mathrm{m}}^{3}107molecules/cm3 at a temperature of 25 mK are obtained for 14ND3{}^{14}{\mathrm{ND}}_{3}14ND3​ and 15ND3{}^{15}{\mathrm{ND}}_{3}15ND3​ separately and simultaneously. This corresponds to a phase-space density in the trap of $2\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}13},$ 50 times less than the initial phase-space density in the beam.
Inspired by the spectacular successes in the field of cold atoms, there is currently great interest in cold molecules. Cooling molecules is useful for various fundamental physics studies and gives access to an exotic regime in chemistry where the wave property of the molecules becomes important. Although cooling molecules has turned out to be considerably more difficult than cooling atoms, a number of methods to produce samples of cold molecules have been demonstrated over the last few years. This paper aims to review the application of cold molecules and the methods to produce them. Emphasis is put on the deceleration of polar molecules using time-varying electric fields. The operation principle of the array of electrodes that is used to decelerate polar molecules is described in analogy with, and using terminology from, charged-particle accelerators. It is shown that, by applying an appropriately timed high voltage burst, molecules can be decelerated while the phase-space density, i.e. the number of molecules per position-velocity interval, remains constant. In this way the high density and low temperature in the moving frame of a pulsed molecular beam can be transferred to the laboratory frame. Experiments on metastable CO in states that are either repelled by or attracted to high electric fields are presented. Loading of slow molecules into traps and storage rings is discussed.
We have decelerated a supersonic beam of 174YbF molecules using a switched sequence of electrostatic field gradients. These molecules are 7 times heavier than any previously decelerated. An alternating gradient structure allows us to decelerate and focus the molecules in their ground state. We show that the decelerator exhibits the axial and transverse stability required to bring the molecules to rest. Our work significantly extends the range of molecules amenable to this powerful method of cooling and trapping.