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Physical Chemistry Chemical Physics

Molecular beams with a tunable velocity

Cynthia E. Heiner, Hendrick L. Bethlem, Gerard Meijer

Published Jan 1, 2006• 44 citations
Publisher

Abstract

The merging of molecular beam methods with those of accelerator physics has yielded new tools to manipulate the motion of molecules. Over the last few years, decelerators, lenses, bunchers, traps, and storage rings for neutral molecules have been demonstrated. Molecular beams with a tunable velocity and with a tunable width of the velocity distribution can now be produced, and are expected to become a valuable tool in a variety of physical chemistry and chemical physics experiments. Here we present a compact molecular beam machine, capable of producing 3D spatially focused packets of state-selected accelerated or decelerated molecules.

DOI
10.1039/b602260j

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The merging of molecular beam methods with those of accelerator physics has yielded new tools to manipulate the motion of molecules. Over the last few years, decelerators, lenses, bunchers, traps, and storage rings for neutral molecules have been demonstrated. Molecular beams with a tunable velocity and with a tunable width of the velocity distribution can now be produced, and are expected to become a valuable tool in a variety of physical chemistry and chemical physics experiments. Here we present a compact molecular beam machine, capable of producing 3D spatially focused packets of state-selected accelerated or decelerated molecules.
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.
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.
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.
Cryogenic buffer-gas beams are a promising method for producing bright sources of cold molecular radicals for cold-collision and chemical-reaction experiments. In order to use these beams in studies of reactions with controlled collision energies or in trapping experiments, one needs a method of controlling the forward velocity of the beam. A Stark decelerator can be an effective tool for controlling the mean speed of molecules produced by supersonic jets, but efficient deceleration of buffer-gas beams presents new challenges due to longer pulse lengths. Traveling-wave decelerators are uniquely suited to meet these challenges because of their ability to confine molecules in three dimensions during deceleration and their versatility afforded by the analog control of the electrodes. We have created ground-state $\mathrm{CH}(X{\phantom{\rule{0.16em}{0ex}}}^{2}\ensuremath{\Pi})$ radicals in a cryogenic buffer-gas cell with the potential to produce a cold molecular beam of 1011{10}^{11}1011 molecules/pulse. We present a general protocol for Stark deceleration of beams with a large position and velocity spread for use with a traveling-wave decelerator. Our method involves confining molecules transversely with a hexapole for an optimized distance before deceleration. This rotates the phase-space distribution of the molecular packet so that the packet is matched to the time-varying phase-space acceptance of the decelerator. We demonstrate with simulations and an analytic one-dimensional model that this method can decelerate a significant fraction of the molecules in successive wells of a traveling-wave decelerator to produce energy-tuned beams for cold and controlled-molecule experiments.
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.
With the Stark deceleration technique, packets of molecules with a tunable velocity, a narrow velocity spread, and a high state purity can be produced. These tamed molecular beams find applications in high resolution spectroscopy, cold molecule trapping, and controlled scattering experiments. The quality and purity of the packets of molecules emerging from the decelerator critically depend on the specifications of the decelerator, but also on the characteristics of the molecular beam pulse with which the decelerator is loaded. We consider three frequently used molecular beam sources, and discuss their suitability for molecular beam deceleration experiments, in particular with the application in crossed beam scattering in mind. The performance of two valves in particular, the Nijmegen Pulsed Valve and the Jordan Valve, is illustrated by decelerating ND 3 molecules in a 2.6 meter-long Stark decelerator. We describe a protocol to characterize the valve, and to optimally load the pulse of molecules into the decelerator. We characterize the valves regarding opening time duration, optimal valve-to-skimmer distance, mean velocity, velocity spread, state purity, and relative intensity.