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Physical Review A

Slowing molecules by optical microlinear deceleration

P. F. Barker, Mikhail N. Shneider

Published Dec 12, 2002• 55 citations
Publisher

Abstract

We study the creation of stationary cold molecules by rapid deceleration of supersonically cooled molecules in a high-intensity pulsed optical lattice. Using the heavy molecule ${\mathrm{I}}_{2}$ as an example we predict the evolution of the velocity distribution function of the ensemble during the deceleration period, and show that stationary cold molecules with temperatures below 1 K and densities of approximately ${10}^{12}{\mathrm{cm}}^{\ensuremath{-}3}$ can be produced over length scales of hundreds of micrometers on submicrosecond time scales.

DOI
10.1103/physreva.66.065402

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•Jun 1, 2014•1 citation
We study the creation of stationary cold molecules by rapid deceleration of supersonically cooled molecules in a high-intensity pulsed optical lattice. Using the heavy molecule I2{\mathrm{I}}_{2}I2​ as an example we predict the evolution of the velocity distribution function of the ensemble during the deceleration period, and show that stationary cold molecules with temperatures below 1 K and densities of approximately 1012cm\ensuremath−3{10}^{12}{\mathrm{cm}}^{\ensuremath{-}3}1012cm\ensuremath−3 can be produced over length scales of hundreds of micrometers on submicrosecond time scales.
This work presents the proposed schemes for decelerating cold molecules created in pulsed supersonic expansions using pulsed optical lattices. The first scheme relies on the application of a decelerating optical lattice with a dipole-potential well depth of approximately 1 K, created by rapidly chirping medium-intensity fields in the 10 W/cm/sup 2/ range. This scheme is an optical analog of the Start decelerator that has been successfully used to slow a range of polar molecules. A significant fraction (about 10%) of the very heavy I/sub 2 /molecules in an Ar buffer gas is shown to be slowed by using this method over sub-microsecond time scales. In the second technique, an optical lattice with larger well depth in the 100 K range travelling at half the supersonic beam velocity is used to trap a significant fraction of the cold, high-velocity molecules. This technique is developed based on the property of periodic motion of the trapped molecules in the optical lattice; the molecules reverse their initial (relative) velocities in the lattice reference frame after half a period. Using this method the cold molecules can be transferred from high speed to zero velocity on nanosecond time scales. As an example, 33% of a CO molecule beam (1 K) with a velocity of 230 m/s is slowed utilising optical intensities of less than 10/sup 12/ W/cm/sup 2/.
The deceleration of molecules from cold molecular beams using electric and magnetic fields has become an important means for producing stationary, cold dipolar or paramagnetic molecular gases that can be trapped and potentially cooled to ultra-cold temperatures in the μK range. We report on a general scheme for the creation of cold molecules of essentially any type by deceleration of a cold molecular beam using intense optical fields. Deceleration of benzene molecules to zero velocity is achieved by utilizing a single half oscillation of the center-of-mass motion of the molecules within a moving optical lattice. The lattice traveling at half the speed of the molecular beam is created by the interference of two near-counter-propagating fields at different frequencies. We show that by rapidly switching on the optical lattice for approximately the time required for a half oscillation, a bunch of approximately 10 5 benzene molecules can be rapidly decelerated and brought to rest in the laboratory frame.
We investigate the deceleration and bunching of cold molecules in a pulsed supersonic jet using a far-off-resonant optical lattice traveling with a constant velocity. Using an analytical treatment, we show that by choosing the lattice velocity equal to half the supersonic beam velocity and by optimizing the pulse duration, a significant fraction $(\ensuremath{\sim}33%)$ of translationally cold (1 K) CO molecules from a supersonic molecular beam can be decelerated to zero velocity, and simultaneously bunched in velocity space. Due to the large difference of polarizability to mass ratio between the buffer gas and the CO molecules in the pulsed jet, the buffer gas can be precluded from the fraction of stationary molecules by choosing a suitable pulse duration. Furthermore, we find that spatial bunching within the optical lattice is induced and the position of the bunch within the lattice can be chosen by varying the lattice velocity.
We propose a promising scheme to realize the deceleration of a pulsed subsonic molecular beam by using a multistage optical Stark decelerator (i.e., a 1D quasi-cw traveling optical lattice), which is composed of two nearly counter-propagating, time-varying, red-detuned light fields with an intensity of ~10⁷Wcm⁻² and a fixed frequency difference between them. We also study the influence of the velocity reduced amount of the traveling lattice, the lattice power, the synchronous phase angle, the deceleration-stage number and the temporal profile of laser pulses on the molecular slowing results by using 3D Monte-Carlo method. Our study shows that the proposed decelerator cannot only be used to slow a pulsed subsonic beam from 240m/s to standstill, but also to obtain a cold molecular packet with a temperature of a few µK, and the corresponding fraction of cold molecules is 10⁻⁶-10⁻⁷, which strongly depends on the synchronous phase angle. And we also find that a pair of appropriate rising and falling times of laser pulses will lead to a better slowing effect than that produced by the top-hat temporal ones.
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.
Cold and ultracold molecules are highly desirable for a diverse range of applications in physics and chemistry such as precision measurements, tests of fundamental physics, quantum simulation and information processing, quantum chemistry, and the physics of strongly correlated quantum matter. Laser cooling is usually infeasible in molecules because their rotational and vibrational transitions make is difficult to come up with a closed scattering cycle. Recently, a narrow range of diatomic molecules, one of which is CaF, has been shown to possess a convenient electronic structure and a highly-diagonal Franck-Condon matrix and thus be amenable to laser cooling. This thesis describes experiments on laser cooling of CaF radicals produced in a supersonic source. We first investigate the increased fluorescence when multi-frequency resonant light excites the molecules from the four hyperfine levels of the ground X²∑+(N = 1, v = 0) state to the first excited A²π½ (J’ = 1=2; v’ = 0) state. The number of photons scattered per molecule increases significantly from one or two in the single frequency case to more than 50 before the molecules get pumped into the X²∑+(N = 1; v = 1) state. We demonstrate laser cooling and slowing of CaF using counter-propagating laser light which causes the molecules to scatter more than a thousand photons on the X (N = 1, v = 0, 1) <->A (J’ = 1=2; v’ = 0) transition. The effect of the laser cooling is to slow a group of molecules from 600 ms-1 to about 580 ms-1 and to narrow their velocity distribution from an initial temperature of 3 K down to 300 mK. In addition, chirping the frequency of the cooling light to keep it on resonance with the decelerating molecules doubles the deceleration and further compresses the velocity distribution. The effect of the laser cooling is limited by the optical pumping of molecules in the X (N = 1, v = 2) state.