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arXiv:1609.05823 · ChemPhysChem

Principles and Design of a Zeeman–Sisyphus Decelerator for Molecular Beams

Noah J. Fitch, Michael R. Tarbutt

Published Sep 15, 2016• 32 citations
arXivHTMLPDF

Abstract

We explore a technique for decelerating molecules using a static magnetic field and optical pumping. Molecules travel through a spatially varying magnetic field and are repeatedly pumped into a weak-field seeking state as they move towards each strong field region, and into a strong-field seeking state as they move towards weak field. The method is time-independent and so is suitable for decelerating both pulsed and continuous molecular beams. By using guiding magnets at each weak field region, the beam can be simultaneously guided and decelerated. By tapering the magnetic field strength in the strong field regions, and exploiting the Doppler shift, the velocity distribution can be compressed during deceleration. We develop the principles of this deceleration technique, provide a realistic design, use numerical simulations to evaluate its performance for a beam of CaF, and compare this performance to other deceleration methods.

DOI
10.1002/cphc.201600656

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Inside Cover: Principles and Design of a Zeeman–Sisyphus Decelerator for Molecular Beams (ChemPhysChem 22/2016)

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The Inside Cover picture illustrates the essential elements of the deceleration method; molecules propagate through an array of permanent magnets in the presence of a frequency-split optical-pumping laser, resulting in deceleration. More information can be found in the Full Paper by N. J. Fitch and M. R. Tarbutt on page 3609 in Issue 22, 2016 (DOI: 10.1002/cphc.201600656).

ChemPhysChem•Nov 17, 2016•0 citations
We explore a technique for decelerating molecules using a static magnetic field and optical pumping. Molecules travel through a spatially varying magnetic field and are repeatedly pumped into a weak-field seeking state as they move towards each strong field region, and into a strong-field seeking state as they move towards weak field. The method is time-independent and so is suitable for decelerating both pulsed and continuous molecular beams. By using guiding magnets at each weak field region, the beam can be simultaneously guided and decelerated. By tapering the magnetic field strength in the strong field regions, and exploiting the Doppler shift, the velocity distribution can be compressed during deceleration. We develop the principles of this deceleration technique, provide a realistic design, use numerical simulations to evaluate its performance for a beam of CaF, and compare this performance to other deceleration methods.
We present a robust, continuous molecular decelerator that employs high magnetic fields and few optical pumping steps. CaOH molecules are slowed, accumulating at low velocities in a range sufficient for loading both magnetic and magneto-optical traps. During the slowing, the molecules scatter only seven photons, removing around 8 K of energy. Because large energies can be removed with only a few spontaneous radiative decays, this method can in principle be applied to nearly any paramagnetic atomic or molecular species, opening a general path to trapping of complex molecules.
We present a moving-trap Zeeman decelerator (MTZD) for use in molecular beam manipulation and magnetic-trapping experiments of paramagnetic atoms and molecules. The 0.49 m MTZD consists of a combination of a 2D magnetic quadrupole guide and deceleration coils, which together produce an array of 3D magnetic traps. The design is based on that of Trimeche et al. with significant modifications. The 2D quadrupole is driven by fast rising and falling square pulses of current (up to 700 A) of arbitrary lengths of time. The traps can be made to move at velocities from ca. 370 m/s down to zero, which is done by driving through the deceleration coils a sinusoidal current with frequencies ranging from zero to ca. 9 kHz and peak currents up to 1000 A. The trap velocity is proportional to the current frequency. The MTZD manipulates the velocities of molecular beams by traveling initially at the same velocity as the beam. 3D guiding is achieved with a constant current frequency and deceleration is achieved with a downward chirp of the current frequency at a rate corresponding to the desired deceleration. We explain the technical design and operation principles of the MTZD and we detail the custom power electronics that drive the 2D quadrupole guide and the decelerator coils. We present extensive Monte-Carlo trajectory simulations to demonstrate the properties of the MTZD and we conclude that decelerations should be kept below 30000 m/s/s to maintain a good 6D phase-space acceptance. In proof-of-principle experiments, with the deceleration coils operating with a reduced current in the range 100-200 A, we demonstrate the 3D guiding of a beam of metastable argon atoms at 373 m/s and deceleration at 25000 m/s/s from 342 m/s to 304 m/s. The deceleration corresponds to the removal of 21% of the kinetic energy of the beam.
Laser cooling and trapping in a magneto-optical trap (MOT) have been essential to the success of cold atom physics in the last decades. Recently, the application of the same techniques to molecules has begun. The complexity of even a simple diatomic molecule makes laser cooling difficult, but promises new applications in many areas of research. In this thesis I describe the development of the first three-dimensional MOT of calcium fluoride (CaF) molecules. First, a cryogenic buffer gas source was set up, producing a pulsed beam of 9.3*10^10 molecules per steradian per pulse with forward velocities around 170 m/s. A similar source for very large molecules was set up during a 5 month internship at the University of Vienna. Next, the molecular pulse was slowed down to the capture velocity of a MOT using chirped laser slowing, resulting in about 7*10^5 CaF molecules passing through the typical MOT volume of 1 cm^3 at velocities of 15+-5 m/s. A new deceleration method, called Zeeman-Sisyphus deceleration, was also investigated. In this method molecules move through a spatially varying magnetic field and are optically pumped between low- and high-field seeking states in such as a way that they are always losing kinetic energy. The method promises to deliver more slow molecules because the molecules are guided transversely as they are decelerated. A small prototype was built and the optical pumping step was tested successfully. Finally, 7.6*10^3 CaF molecules were trapped in a MOT and cooled to a temperature of 8.5 mK. The radial trap frequency is 2 pi*130 Hz and the damping constant is beta=9.5*10^2 s^-1. The lifetime is about 100 ms and depends strongly on the scattering rate. This MOT is an an ideal starting point for a wide range of new experiments with ultracold molecules.
A novel traveling-wave Zeeman decelerator based on a double-helix coil geometry capable of decelerating paramagnetic molecules with high efficiency is presented. Moving magnetic traps are generated by applying time-dependent currents through the decelerator coils. Paramagnetic molecules in low-field-seeking Zeeman states are confined inside the moving traps which are decelerated to lower forward velocities. As a prototypical example, we demonstrate the deceleration of OH radicals from an initial velocity of 445 m s −1 down to various final velocities. The experimental results are analyzed and numerically reproduced with the help of trajectory simulations confirming the phase-space stability and efficiency of the deceleration of the molecules in the new device.
We demonstrate and characterize Zeeman-Sisyphus (ZS) deceleration of a beam of ytterbium monohydroxide. Our method uses a combination of large magnetic fields ($\ensuremath{\sim}2.5$ T) and optical spin-flip transitions to decelerate molecules while scattering only $\ensuremath{\sim}10$ photons per molecule. We study the challenges associated with the presence of internal molecular perturbations among the excited electronic states and discuss the methods used to overcome these challenges, including a modified ZS decelerator using microwave and optical transitions.