Hendrick L. Bethlem

Production and application of translationally cold molecules

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.

Manipulation and Control of Molecular Beams

A study was conducted to demonstrate the manipulation of molecular beams with electric and magnetic fields. Seeded pulsed supersonic expansions were employed to conduct the investigations. The conservative forces exerted further downstream by the electric and magnetic fields enabled the researchers to manipulate and control the shape and the position of the distribution in the six-dimensional phase-space. All of the original experimental geometries were devised to create strong magnetic or electric field gradients to efficiently deflect particles from the beam axis. It was demonstrated that a detailed understanding of the influence of the external field on the energy level structure of the molecules was required for the manipulation of molecules with electric or magnetic fields.

Slowing heavy, ground-state molecules using an alternating gradient decelerator

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.

A prototype storage ring for neutral molecules

The ability to cool and manipulate atoms with light has yielded atom interferometry, precision spectroscopy, Bose–Einstein condensates and atom lasers. The extension of controlled manipulation to molecules is expected to be similarly rewarding, but molecules are not as amenable to manipulation by light owing to a far more complex energy-level spectrum. However, time-varying electric and magnetic fields have been successfully used to control the position and velocity of ions, suggesting that these schemes can also be used to manipulate neutral particles having an electric or magnetic dipole moment. Although the forces exerted on neutral species are many orders of magnitude smaller than those exerted on ions, beams of neutral dipolar molecules have been successfully slowed down in a series of pulsed electric fields and subsequently loaded into an electrostatic trap. Here we extend the scheme to include a prototype electrostatic storage ring made of a hexapole torus with a circumference of 80 cm. After injection, decelerated bunches of deuterated ammonia molecules, each containing about 106 molecules in a single quantum state and with a translational temperature of 10 mK, travel up to six times around the ring. Stochastic cooling might provide a means to increase the phase-space density of the stored molecules in the storage ring, and we expect this to open up new opportunities for molecular spectroscopy and studies of cold molecular collisions.

A Stringent Limit on a Drifting Proton-to-Electron Mass Ratio from Alcohol in the Early Universe

Varying Constant? Searches for time-varying fundamental constants provide a means to look beyond the standard model of particle physics. Bagdonaite et al. (p. 46, published online 13 December) set an improved limit on the possible timevariation of the proton-to-electron mass ratio by comparing the frequencies of methanol transitions observed in a galaxy at a look-back time of 7 billion years with those measured in the laboratory. The values agree within 10−7, consistent with no variation over cosmic time. The proton-to-electron mass ratio inferred from methanol lines in a distant galaxy is in accord with the laboratory value. The standard model of physics is built on the fundamental constants of nature, but it does not provide an explanation for their values, nor require their constancy over space and time. Here we set a limit on a possible cosmological variation of the proton-to-electron mass ratio μ by comparing transitions in methanol observed in the early universe with those measured in the laboratory. From radio-astronomical observations of PKS1830-211, we deduced a constraint of ∆μ/μ = (0.0 ± 1.0) × 10−7 at redshift z = 0.89, corresponding to a look-back time of 7 billion years. This is consistent with a null result.

ac Electric Trap for Ground-State Molecules

We here report on the realization of an electrodynamic trap, capable of trapping neutral atoms and molecules in both low-field and high-field seeking states. Confinement in three dimensions is achieved by switching between two electric field configurations that have a saddle point at the center of the trap, i.e., by alternating a focusing and a defocusing force in each direction. The ac trapping of 15ND(3) molecules is experimentally demonstrated, and the stability of the trap is studied as a function of the switching frequency. A 1 mK sample of 15ND(3) molecules in the high-field seeking component of the |J,K=|1,1 level, the ground state of para-ammonia, is trapped in a volume of about 1 mm(3).

Alternating gradient focusing and deceleration of polar molecules.

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.

Perspective: Tipping the scales: Search for drifting constants from molecular spectra

Transitions in atoms and molecules provide an ideal test ground for constraining or detecting a possible variation of the fundamental constants of nature. In this perspective, we review molecular species that are of specific interest in the search for a drifting proton-to-electron mass ratio μ. In particular, we outline the procedures that are used to calculate the sensitivity coefficients for transitions in these molecules and discuss current searches. These methods have led to a rate of change in μ bounded to 6 × 10(-14)/yr from a laboratory experiment performed in the present epoch. On a cosmological time scale, the variation is limited to ∣Δμ∕μ∣ < 10(-5) for look-back times of 10-12× 10(9) years and to ∣Δμ∕μ∣ < 10(-7) for look-back times of 7× 10(9) years. The last result, obtained from high-redshift observation of methanol, translates into μ̇/μ=(1.4±1.4)×10(-17)/yr if a linear rate of change is assumed.

Trapping molecules on a chip in traveling potential wells.

A microstructured array of over 1200 electrodes on a substrate has been configured to generate an array of local minima of electric field strength with a periodicity of 120 microm about 25 microm above the substrate. By applying sinusoidally varying potentials to the electrodes, these minima can be made to move smoothly along the array. Polar molecules in low field seeking quantum states can be trapped in these traveling potential wells. This is experimentally demonstrated by transporting metastable CO molecules in 30 mK deep wells that move at constant velocities above the substrate.

Robust Constraint on a Drifting Proton-to-Electron Mass Ratio at z=0.89 from Methanol Observation at Three Radio Telescopes

A limit on a possible cosmological variation of the proton-to-electron mass ratio μ is derived from methanol (CH3OH) absorption lines in the benchmark PKS1830-211 lensing galaxy at redshift z=0.89 observed with the Effelsberg 100-m radio telescope, the Institute de Radio Astronomie Millimétrique 30-m telescope, and the Atacama Large Millimeter/submillimeter Array. Ten different absorption lines of CH3OH covering a wide range of sensitivity coefficients K(μ) are used to derive a purely statistical 1σ constraint of Δμ/μ=(1.5±1.5)×10(-7) for a lookback time of 7.5 billion years. Systematic effects of chemical segregation, excitation temperature, frequency dependence, and time variability of the background source are quantified. A multidimensional linear regression analysis leads to a robust constraint of Δμ/μ=(-1.0±0.8(stat)±1.0(sys))×10(-7).