We have recently demonstrated static trapping of ammonia isotopologues in a decelerator that consists of a series of ring-shaped electrodes to which oscillating high voltages are applied [Quintero-Pérez et al., Phys. Rev. Lett. 110, 133003 (2013)]. In this paper we provide further details on this traveling wave decelerator and present new experimental data that illustrate the control over molecules that it offers. We analyze the performance of our setup under different deceleration conditions and demonstrate phase-space manipulation of the trapped molecular sample.
We present an analysis of the deceleration and trapping of heavy diatomic molecules in low-field seeking states by a moving electric potential. This moving potential is created by a 'ring-decelerator', which consists of a series of ring-shaped electrodes to which oscillating high voltages are applied. Particle trajectory simulations have been used to analyze the deceleration and trapping efficiency for a group of molecules that is of special interest for precision measurements of fundamental discrete symmetries. For the typical case of the SrF molecule in the (N,M) = (2, 0) state, the ring-dec…
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 unique…
We present a new formalism to calculate phase-space acceptance in a Zeeman decelerator. Using parameters closely mimicking previous Zeeman deceleration experiments, this approach reveals a hitherto unconsidered velocity dependence of the phase stability which we ascribe to the finite rise and fall times of the current pulses that generate the magnetic fields inside the deceleration coils. It is shown that changing the current switch-off times as the sequence progresses, so as to maintain a constant mean acceleration per pulse, can lead to a constant phase stability and hence a beam with well-d…
Zeeman deceleration is an experimental technique in which inhomogeneous, time-dependent magnetic fields generated inside an array of solenoid coils are used to manipulate the velocity of a supersonic beam. A 12-stage Zeeman decelerator has been built and characterized using hydrogen atoms as a test system. The instrument has several original features including the possibility to replace each deceleration coil individually. In this article, we give a detailed description of the experimental setup, and illustrate its performance. We demonstrate that the overall acceptance in a Zeeman decelerator…
We present experiments on decelerating and trapping ammonia molecules using a combination of a Stark decelerator and a traveling wave decelerator. In the traveling wave decelerator a moving potential is created by a series of ring-shaped electrodes to which oscillating high voltages are applied. By lowering the frequency of the applied voltages, the molecules confined in the moving trap are decelerated and brought to a standstill. As the molecules are confined in a true 3D well, this new kind of deceleration has practically no losses, resulting in a great improvement on the usual Stark deceler…
Controlling rovibrational state populations of polar molecules in inhomogeneous electric fields of the Stark deceleration: molecular dynamics and quantum chemistry simulations
We present an experimental realization of a moving magnetic trap decelerator, where paramagnetic particles entrained in a cold supersonic beam are decelerated in a co-moving magnetic trap. Our method allows for an efficient slowing of both paramagnetic atoms and molecules to near stopping velocities. We show that under realistic conditions we will be able to trap and decelerate a large fraction of the initial supersonic beam. We present our first results on deceleration in a moving magnetic trap by bringing metastable neon atoms to near rest. Our estimated phase space volume occupied by decele…
We report the Stark deceleration of CaF molecules in the strong-field seeking ground state and in a weak-field seeking component of a rotationally-excited state. We use two types of decelerator, a conventional Stark decelerator for the weak-field seekers, and an alternating gradient decelerator for the strong-field seekers, and we compare their relative merits. We also consider the application of laser cooling to increase the phase-space density of decelerated molecules.
A new type of decelerator is presented where polar neutral molecules are guided and decelerated using the principle of traveling electric potential wells, such that molecules are confined in stable three-dimensional traps throughout. This new decelerator is superior to the best currently operational decelerator (Scharfenberg et al., Phys.Rev.A 79, 023410(2009)), providing a substantially larger acceptance even at higher accelerations. The mode of operation is described and experimentally demonstrated by guiding and decelerating CO molecules.
We produce SO_2 molecules with a centre of mass velocity near zero using a Stark decelerator. Since the initial kinetic energy of the supersonic SO_2 molecular beam is high, and the removed kinetic energy per stage is small, 326 deceleration stages are necessary to bring SO_2 to a complete standstill, significantly more than in other experiments. We show that in such a decelerator possible loss due to coupling between the motional degrees of freedom must be considered. Experimental results are compared with 3D Monte-Carlo simulations and the quantum state selectivity of the Stark decelerator i…
We report on the deceleration of a beam of SrF molecules from 290 to 120~m/s. Following supersonic expansion, the molecules in the $X^2Σ$ ($v=0$, $N=1$) low-field seeking states are trapped by the moving potential wells of a traveling-wave Stark decelerator. With a deceleration strength of 9.6 km/s$^2$ we have demonstrated the removal of 85 % of the initial kinetic energy in a 4 meter long modular decelerator. The absolute amount of kinetic energy removed is a factor 1.5 higher compared to previous Stark deceleration experiments. The demonstrated decelerator provides a novel tool for the creat…
We present a new concept for a multi-stage Zeeman decelerator that is optimized particularly for applications in molecular beam scattering experiments. The decelerator consists of a series of alternating hexapoles and solenoids, that effectively decouple the transverse focusing and longitudinal deceleration properties of the decelerator. It can be operated in a deceleration and acceleration mode, as well as in a hybrid mode that makes it possible to guide a particle beam through the decelerator at constant speed. The deceleration features phase stability, with a relatively large six-dimensiona…
Multistage Zeeman deceleration is a technique used to reduce the velocity of neutral molecules with a magnetic dipole moment. Here we present a Zeeman decelerator that consists of 100 solenoids and 100 magnetic hexapoles, that is based on a short prototype design presented recently [Phys. Rev. A 95, 043415 (2017)]. The decelerator features a modular design with excellent thermal and vacuum properties, and is robustly operated at a 10 Hz repetition rate. This multistage Zeeman decelerator is particularly optimized to produce molecular beams for applications in crossed beam molecular scattering …
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 i…
A supersonic beam of metastable neon atoms has been decelerated by exploiting the interaction between the magnetic moment of the atoms and time-dependent inhomogeneous magnetic fields in a multistage Zeeman decelerator. Using 91 deceleration solenoids, the atoms were decelerated from an initial velocity of 580m/s to final velocities as low as 105m/s, corresponding to a removal of more than 95% of their initial kinetic energy. The phase-space distribution of the cold, decelerated atoms was characterized by time-of-flight and imaging measurements, from which a temperature of 10mK was obtained in…
Stark deceleration has been utilized for slowing and trapping several species of neutral, ground-state polar molecules generated in a supersonic beam expansion. Due to the finite physical dimension of the electrode array and practical limitations of the applicable electric fields, only molecules within a specific range of velocities and positions can be efficiently slowed and trapped. These constraints result in a restricted phase space acceptance of the decelerator in directions both transverse and parallel to the molecular beam axis; hence, careful modeling is required for understanding and …
We demonstrate the deceleration of heavy polar molecules in low-field seeking states by combining a cryogenic source and a travelling-wave Stark decelerator. The cryogenic source provides a high intensity beam with low speed and temperature, and the travelling-wave decelerator provides large deceleration forces and high phase-space acceptance. We prove these techniques using YbF molecules and find the experimental data to be in excellent agreement with numerical simulations. These methods extend the scope of Stark deceleration to a very wide range of molecules.
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 th…
We propose a promising scheme to decelerate a cw filtering out molecular beam using a red-detuned quasi-cw semi-Gaussian laser beam. By using Monte-Carlo simulation method, we demonstrate this optical Stark deceleration scheme, and study its decelerated dynamic process for a cw ND3 molecular beam as well as the dependence of the deceleration effect on the border width of the semi-Gaussian beam. Our study shows that the proposed scheme can be used to efficiently slow a cw ND3 molecular beam, and obtain a relative average kinetic-energy loss of 9.33% by using a single semi-Gaussian beam with a w…
The transverse motion inside a Stark decelerator plays a large role in the total efficiency of deceleration. We differentiate between two separate regimes of molecule loss during the slowing process. The first mechanism involves distributed loss due to coupling of transverse and longitudinal motion, while the second is a result of the rapid decrease of the molecular velocity within the final few stages. In this work, we describe these effects and present means for overcoming them. Solutions based on modified switching time sequences with the existing decelerator geometry lead to a large gain o…
We have designed and implemented a new Stark decelerator based on wire electrodes, which is suitable for ultrahigh vacuum applications. The 100 deceleration stages are fashioned out of 0.6 mm diameter tantalum and the array's total length is 110 mm, approximately 10 times smaller than a conventional Stark decelerator with the same number of electrode pairs. Using the wire decelerator, we have removed more than 90% of the kinetic energy from metastable CO molecules in a beam.
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 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 radicals.
We report on the production, deceleration and detection of a SrF molecular beam. The molecules are captured from a supersonic expansion and are decelerated in the X$^2Σ^+ (v=0, N=1)$ state. We demonstrate the removal of up to 40% of the kinetic energy with a 2 meter long modular traveling-wave decelerator. Our results demonstrate a crucial step towards the preparation of ultracold gases of heavy diatomic molecules for precision spectroscopy.
We report on the Zeeman deceleration of ground-state NH radicals, using a decelerator that consists of 100 pulsed solenoids and 100 permanent hexapoles. Packets of state-selected NH ($X\,^3Σ^-$, N=0, J=1) radicals are produced with final velocities ranging between 510 m/s and 150 m/s. The velocity distributions of the packets of NH exiting the Zeeman decelerator are probed using velocity map imaging detection. We present a new 1+2' resonance-enhanced multiphoton ionization scheme for NH, that allows for velocity map imaging detection under ion recoil-free conditions. The packets of Zeeman-dece…
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…
Recently, a decelerator for neutral polar molecules has been presented that operates on the basis of macroscopic, three-dimensional, traveling electrostatic traps (Osterwalder et al., Phys. Rev. A 81, 051401 (2010)). In the present paper, a complete description of this decelerator is given, with emphasis on the electronics and the mechanical design. Experimental results showing the transverse velocity distributions of guided molecules are shown and compared to trajectory simulations. An assessment of non-adiabatic losses is made by comparing the deceleration signals from 13-CO with those from …
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 details of the trap loading sequence, typically $10^5$ OH ($X^2Π_{3/2}, J=3/2$) 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 second.
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 7 photons, removing around 8 K of energy. Because large energies can be removed with only a few spontaneous radiative decays, this method can be applied to nearly any paramagnetic atomic or molecular species, opening a general path to trapping of complex molecules.
Zeeman deceleration is a relatively new technique used to obtain full control over the velocity of paramagnetic atoms or molecules in a molecular beam. We present a detailed description of a multistage Zeeman decelerator that has recently become operational in our laboratory [Cremers \emph{et al.}, Phys. Rev. A 98, 033406 (2018)], and that is specifically optimized for crossed molecular beams scattering experiments. The decelerator consists of an alternating array of 100 solenoids and 100 permanent hexapoles to guide or decelerate beams of paramagnetic atoms or molecules. The Zeeman decelerato…
Cold supersonic beams of molecules can be slowed down using a switched sequence of electrostatic field gradients. The energy to be removed is proportional to the mass of the molecules. Here we report deceleration of YbF, which is 7 times heavier than any molecule previously decelerated. We use an alternating gradient structure to decelerate and focus the molecules in their ground state. We show that the decelerator exhibits the axial and transverse stability required to bring these molecules to rest. Our work significantly extends the range of molecules amenable to this powerful method of cool…
Metastable helium molecules (He$_2^*$) have been generated by striking a discharge in a supersonic expansion of helium gas from a pulsed valve. When operating the pulsed valve at room temperature, 77K, and 10K, the mean velocity of the supersonic beam was measured to be 1900m/s, 980m/s, and 530m/s, respectively. A 55-stage Zeeman decelerator operated in a phase-stable manner was then used to further reduce the beam velocity and tune it in the range between 100 and 150m/s. The internal-state distribution of the decelerated sample was established by photoionization spectroscopy.
We here report on the experimental realization of a microwave decelerator for neutral polar molecules, suitable for decelerating and focusing molecules in high-field-seeking states. The multi-stage decelerator consists of a cylindrical microwave cavity oscillating on the TE 11n mode, with n=12 electric field maxima along the symmetry axis. By switching the microwave field on and off at the appropriate times, a beam of state-selected ammonia molecules with an incident mean velocity of 25 m/s is guided while being spatially focussed in the transverse direction and bunched in the forward directio…
We demonstrate the successful experimental implementation of a multi-stage Zeeman decelerator utilizing the new concept described in the accompanying paper. The decelerator consists of an array of 25 hexapoles and 24 solenoids. The performance of the decelerator in acceleration, deceleration and guiding modes is characterized using beams of metastable Helium ($^3S$) atoms. Up to 60% of the kinetic energy was removed for He atoms that have an initial velocity of 520 m/s. The hexapoles consist of permanent magnets, whereas the solenoids are produced from a single hollow copper capillary through …
Beams of helium atoms in Rydberg states with principal quantum number $n=52$, and traveling with an initial speed of 1950 m/s, have been accelerated, decelerated and guided while confined in moving electric traps generated above a curved, surface-based electrical transmission line with a segmented center conductor. Experiments have been performed with atoms guided at constant speed, and with accelerations exceeding $10^7$ m/s$^2$. In each case the manipulated atoms were detected by spatially resolved, pulsed electric field ionization. The effects of tangential and centripetal accelerations on …
We demonstrate and characterize Zeeman-Sisyphus (ZS) deceleration of a beam of ytterbium monohydroxide (YbOH). Our method uses a combination of large magnetic fields ($\sim$ 2.5 T) and optical spin-flip transitions to decelerate molecules while scattering only $\sim$ 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.
A microstructured array of 1254 electrodes on a substrate has been configured to generate an array of local minima of electric field strength with a periodicity of 120 $μ$m about 25 $μ$m 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. Recently, we experimentally demonstrated this by transporting metastable CO molecules at constant velocities above the substrate [Phys. Rev. Lett. 100 (2008) 153003]. …
In a Stark decelerator, polar molecules are slowed down and focussed by an inhomogeneous electric field which switches between two configurations. For the decelerator to work, it is essential that the molecules follow the changing electric field adiabatically. When the decelerator switches from one configuration to the other, the electric field changes in magnitude and direction, and this can cause molecules to change state. In places where the field is weak, the rotation of the electric field vector during the switch may be too rapid for the molecules to maintain their orientation relative to…
We report on the electrostatic trapping of neutral SrF molecules. The molecules are captured from a cryogenic buffer-gas beam source into the moving traps of a 4.5 m long traveling-wave Stark decelerator. The SrF molecules in $X^2Σ^+(v=0, N=1)$ state are brought to rest as the velocity of the moving traps is gradually reduced from 190 m/s to zero. The molecules are held for up to 50 ms in multiple electric traps of the decelerator. The trapped packets have a volume (FWHM) of 1 mm$^{3}$ and a velocity spread of 5(1) m/s which corresponds to a temperature of $60(20)$ mK. Our result demonstrates …
We describe the production of cold, slow-moving LiH molecules. The molecules are produced in the ground state using laser ablation and supersonic expansion, and 68% of the population is transferred to the rotationally excited state using narrowband radiation at the rotational frequency of 444GHz. The molecules are then decelerated from 420m/s to 53m/s using a 100 stage Stark decelerator. We demonstrate and compare two different deceleration modes, one where every stage is used for deceleration, and another where every third stage decelerates and the intervening stages are used to focus the mol…
Metastable (1s)(2s) $^3{\rm S}_1$ helium atoms produced in a supersonic beam were excited to Rydberg-Stark states (with $n$ in the $27-30$ range) in a cryogenic environment and subsequently decelerated by, and trapped above, a surface-electrode decelerator. In the trapping experiments, the Rydberg atoms were brought to rest in 75~$μ$s and over a distance of 33~mm and kept stationary for times $t_{\mathrm{trap}}$ in the $0-525$~$μ$s range, before being re-accelerated for detection by pulsed field ionization. The use of a home-built valve producing short gas pulses with a duration of about 20~$μ…
Beams of helium atoms in Rydberg-Stark states with principal quantum number $n=48$ and electric dipole moments of 4600~D have been decelerated from a mean initial longitudinal speed of 2000~m/s to zero velocity in the laboratory-fixed frame-of-reference in the continuously moving electric traps of a transmission-line decelerator. In this process accelerations up to $-1.3\times10^{7}$~m/s$^2$ were applied, and changes in kinetic energy of $ΔE_{\mathrm{kin}}=1.3\times10^{-20}$~J ($ΔE_{\mathrm{kin}}/e = 83$~meV) per atom were achieved. Guided and decelerated atoms, and those confined in stationar…
