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Annual Review of Physical Chemistry

STARK DECELERATION AND TRAPPING OF OH RADICALS

Sebastiaan Y. T. van de Meerakker, Nicolas Vanhaecke, Gerard Meijer

Published Dec 1, 2005• 90 citations
Publisher

Abstract

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.

DOI
10.1146/annurev.physchem.55.091602.094337

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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.
We demonstrate feedback control optimization for the Stark deceleration and trapping of neutral polar molecules using evolutionary strategies. In a Stark-decelerator beamline, pulsed electric fields are used to decelerate OH\mathrm{OH}OH radicals and subsequently store them in an electrostatic trap. The efficiency of the deceleration and trapping process is determined by the exact timings of the applied electric field pulses. Automated optimization of these timings yields an increase of 40% of the number of trapped OH\mathrm{OH}OH radicals.
A pulsed beam of ground state OH radicals is slowed down using a Stark decelerator and is subsequently loaded into an electrostatic trap. Characterization of the molecular beam production, deceleration, and trap loading process is performed via laser induced fluorescence detection inside the quadrupole trap. Depending on the details of the trap loading sequence, typically 10(5) OH (X2Pi(3/2),J=3/2) radicals are trapped at a density of around 10(7) cm(-3) and at temperatures in the 50-500 mK range. The 1/e trap lifetime is around 1.0 s.
Samples of cold and ultracold polar molecules have the potential to revolutionize physical chemistry, precision measurement, and few-body quantum physics. This thesis describes experimental results for the production of cold samples of OH radicals by Stark deceleration of a supersonic beam. Since Stark deceleration cannot increase the phase space density of the sample, the initial production stage of the OH molecule is critical. The first set of experiments describes a general methodology for the production of OH beams with maximal phase space density, as well as the subsequent coupling to a Stark decelerator. Additionally, we describe the redesign of our electrostatic trap, optimized for future collision experiments of OH with co-trapped ultracold Rb atoms. The new design resulted in a 15-fold increase in total number of trapped molecules over the previous design when tested with ND3 molecules. The second set of experiments focuses on laser-based detection of OH molecules at the exit of the decelerator based on laser induced fluorescence (LIF) and resonance enhanced multiphoton ionizaton (REMPI). The latter method uses vacuum-ultraviolet light at 118nm produced by third-harmonic generation in Xe/Ar gas mixtures as the ionizing step. The sensitivity of this latter technique is limited by the attainable photon flux of the ionizing radiation at 118nm. We present detailed measurements of the conversion efficiencies as well as absolute photon fluxes. Strategies to overcome these limitations as well as prospects for detection of OH molecules in a trap are discussed.
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.
Abstract Stark deceleration is a technique that uses time-varying inhomogeneous electric fields to decelerate polar molecules for various molecular beam and trapping experiments. New ring-geometry Stark decelerators with continuously varying voltages offer a method to produce a more intense source of molecules than in the more typically used crossed-pin geometry Stark decelerators. However, this new technique, traveling-wave Stark deceleration, is more experimentally challenging due to the electronic requirements. A third method, pulsed-ring Stark deceleration, uses ring-geometry electrodes with high-voltage pulses to decelerate molecules. The discrete voltages make it easier to implement, and it is more efficient in certain situations due to an increased longitudinal potential gradient. Here, we present an experimental realization of a ring-geometry Stark decelerator using both continuously varying and discrete voltages. Using the pulsed-ring method, we demonstrate a newly accessible low-velocity regime for moderate peak voltages on ring electrodes. This opens up the opportunity to efficiently decelerate various molecular species using a medium length decelerator. A comparison of experimental and simulated results between traveling-wave and pulsed-ring Stark deceleration is presented along with a simple model for determining when each mode is more efficient.