Design and characterization of a cryogenic linear Paul ion trap for ion-neutral reaction studies.

Ultra-high vacuum conditions are ideal for the study of trapped ions. They offer an almost perturbation-free environment, where ions confined in traps can be studied for extended periods of time-facilitating precision measurements and allowing infrequent events to be observed. However, if one wishes to study processes involving molecular ions, it is important to consider the effect of blackbody radiation (BBR). The vast majority of molecular ions interact with BBR. At 300 K, state selection in trapped molecular ions can be rapidly lost (in a matter of seconds). To address this issue, and to maintain state selectivity in trapped molecular ions, a cryogenic ion trap chamber has been constructed and characterized. At the center of the apparatus is a linear Paul ion trap, where Coulomb crystals can be formed for ion-neutral reaction studies. Optical access is provided, for lasers and for imaging of the crystals, alongside ion optics and a flight tube for recording time-of-flight mass spectra. The ion trap region, encased within two nested temperature stages, reaches temperatures below 9 K. To avoid vibrations from the cryocooler impeding laser cooling or imaging of the ions, vibration-damping elements are explicitly included. These components successfully inhibit the coupling of vibrations from the cold head to the ion trap-confirmed by accelerometer measurements and by the resolution of images recorded at the trap center (at 9 and 295 K). These results confirm that the cryogenic ion trap apparatus meets all requirements for studying ion-neutral reactions under cold, controlled conditions.

A stand-alone magnetic guide for producing tuneable radical beams.

Radicals are prevalent in gas-phase environments such as the atmosphere, combustion systems, and the interstellar medium. To understand the properties of the processes occurring in these environments, it is helpful to study radical reaction systems in isolation-thereby avoiding competing reactions from impurities. There are very few methods for generating a pure beam of gas-phase radicals, and those that do exist involve complex setups. Here, we provide a straightforward and versatile solution. A magnetic radical filter (MRF), composed of four Halbach arrays and two skimming blades, can generate a beam of velocity-selected low-field-seeking hydrogen atoms. As there is no line-of-sight through the device, all species that are unaffected by the magnetic fields are physically blocked; only the target radicals are successfully guided around the skimming blades. The positions of the arrays and blades can be adjusted, enabling the velocity distribution of the beam (and even the target radical species) to be modified. The MRF is employed as a stand-alone device-filtering radicals directly from the source. Our findings open up the prospect of studying a range of radical reaction systems with a high degree of control over the properties of the radical reactants.

Manipulating hydrogen atoms using permanent magnets: Characterisation of a velocity-filtering guide.

A Halbach array composed of 12 permanent magnets in a hexapole configuration is employed to deflect hydrogen atoms as they exit a Zeeman decelerator. The ability to preferentially manipulate H atoms is very useful, as there are currently very few techniques that are appropriate for purifying a beam of H atoms from precursor molecules (such as molecular hydrogen or ammonia), seed gases, and other contaminant species. The extent to which hydrogen atoms are deflected by a single Halbach array when it is tilted or shifted off the main beam axis is characterised experimentally and interpreted with the aid of a simple mathematical model. A radical beam filter is subsequently introduced, where four Halbach arrays arranged in series serve to deflect H atoms away from the main beam axis and around skimming blades; all other components of the incoming beam are blocked by the blades and are thus not transmitted through the magnetic guide. The properties of the guide, as established by experimental measurements and complemented by detailed simulations, confirm that it is a highly effective beam filter-successfully generating a pure and velocity-selected beam of H atoms.

Towards state selective recombination of H3+ under astrophysically relevant conditions.

We present studies on the thermalisation of H3+ ions in a cold He/Ar/H2 plasma at temperatures 30-70 K. We show that we are able to generate a rotationally thermalised H3+ ensemble with a population of rotational and nuclear spin states corresponding to a particular ion translational temperature. By varying the para-H2 fraction used in the experiment we are able to produce para-H3+ ions with fractional populations higher than those corresponding to thermodynamic values. At 35 K, only the lowest rotational states of para and ortho H3+ are populated. This is the first step towards experimental studies of electron-molecular ion recombination processes with precisely specified quantum states at astrophysically relevant temperatures.

Evolutionary Algorithm Optimization of Zeeman Deceleration: Is It Worthwhile for Longer Decelerators?

In Zeeman deceleration, only a small subset of low-field-seeking particles in the incoming beam possess initial velocities and positions that place them within the phase-space acceptance of the device. In order to maximize the number of particles that are successfully decelerated to a selected final velocity, we seek to optimize the phase-space acceptance of the decelerator. Three-dimensional particle trajectory simulations are employed to investigate the potential benefits of using a covariance matrix adaptation evolutionary strategy (CMA-ES) optimization method for decelerators longer than 12 stages and for decelerating species other than H atoms. In all scenarios considered, the evolutionary algorithm-optimized sequences yield vastly more particles within the target velocity range. This is particularly evident in scenarios where standard sequences are known to perform poorly; simulations show that CMA-ES optimization of a standard sequence decelerating H atoms from an initial velocity of 500 ms-1 down to a final velocity of 200 ms-1 in a 24-stage decelerator produces a considerable 5921% (or 60-fold) increase in the number of successfully decelerated particles. Particle losses that occur with standard pulse sequences-for example, arising from the coupling of longitudinal and transverse motion-are overcome in the CMA-ES optimization process as the passage of all particles through the decelerator is explicitly considered and focusing effects are accounted for in the optimization process.

Off-axis parabolic mirror relay microscope for experiments with ultra-cold matter.

A new optical system is introduced for the imaging of Coulomb crystals held in a cryogenic ion trap where there are space limitations preventing the placement of an objective close to the fluorescing ions. The optical system features an off-axis parabolic (OAP) mirror relay microscope that will serve to acquire images of a lattice of fluorescing ions confined within an ultra-high-vacuum vessel operating at temperatures below 10 K. We report that the OAP mirror relay setup can resolve features smaller than the separation between neighboring ions in Coulomb crystals. The setup presented here consists of two 90-degree OAP mirrors arranged into a relay from which standard microscope optics deliver the image to a camera. This design allows the first element in the imaging setup-an OAP mirror-to be located as close as possible to the ion trap, achieving high resolution without the need for a direct line-of-sight to the trap center or for a view port to be located in close proximity to the ion trap. Such an arrangement would not be possible with a standard microscope objective, which is the approach commonly adopted by the field. OAP mirrors represent a novel solution for delivering polychromatic images with micrometer-scale resolution over extended distances.

Flowing-afterglow study of electron-ion recombination of para-H3(+) and ortho-H3(+) ions at temperatures from 60 K to 300 K.

Detailed measurements employing a combination of a cryogenic flowing afterglow with Langmuir probe (Cryo-FALP II) and a stationary afterglow with near-infrared absorption spectroscopy (SA-CRDS) show that binary electron recombination of para-H3(+) and ortho-H3(+) ions occurs with significantly different rate coefficients, (p)αbin and (o)αbin, especially at very low temperatures. The measurements cover temperatures from 60 K to 300 K. At the lowest temperature of 60 K, recombination of para-H3(+) is at least three times faster than that of ortho-H3(+) ((p)αbin=(1.8±0.4)×10(-7) cm(3) s(-1) vs. (o)αbin=(0-0 (+5))×10(-8) cm(3) s(-1)).

Binary recombination of H3(+) and D3(+) ions with electrons in plasma at 50-230 K.

The results of an experimental study of the H3(+) and D3(+) ions recombination with electrons in afterglow plasmas in the temperature range 50-230 K are presented. A flowing afterglow apparatus equipped with a Langmuir probe was used to measure the evolution of the electron number density in the decaying plasma. The obtained values of the binary recombination rate coefficient are αbinH3(+) = (6.0 ± 1.8) × 10(-8)(300/T)(0.36±0.09) cm(3) s(-1) for H3(+) ions in the temperature range 80-300 K and αbinD3(+) = (3.5 ± 1.1) × 10(-8)(300/T)(0.73±0.09) cm(3) s(-1) for D3(+) ions in the temperature range 50-300 K. This is the first measurement of the binary recombination rate coefficient of H3(+) and D3(+) ions in a plasma experiment down to 50 K.

Binary and ternary recombination of D3+ ions at 80-130 K: application of laser absorption spectroscopy.

Recombination of D(3)(+) ions with electrons at low temperatures (80-130 K) was studied using spectroscopic determination of D(3)(+) ions density in afterglow plasmas. The use of cavity ring-down absorption spectroscopy enabled an in situ determination of the abundances of the ions in plasma and the translational and the rotational temperatures of the recombining ions. Two near infrared transitions at (5792.70 ± 0.01) cm(-1) and at (5793.90 ± 0.01) cm(-1) were used to probe the number densities of the lowest ortho state and of one higher lying rotational state of the vibrational ground state of D(3)(+) ion. The results show that D(3)(+) recombination with electrons consists of the binary and the third-body (helium) assisted process. The obtained binary recombination rate coefficients are in agreement with a recent theoretical prediction for electron-ion plasma in thermodynamic equilibrium with α(bin)(80 K) = (9.2 ± 2.0) × 10(-8) cm(3) s(-1). The measured helium assisted ternary rate coefficients K(He) are in agreement with our previously measured flowing afterglow data giving a value of K(He)(80 K) = (1.2 ± 0.3) × 10(-25) cm(6) s(-1).

Binary and ternary recombination of para-H3(+) and ortho-H3(+) with electrons: state selective study at 77-200 K.

Measurements in H(3)(+) afterglow plasmas with spectroscopically determined relative abundances of H(3)(+) ions in the para-nuclear and ortho-nuclear spin states provide clear evidence that at low temperatures (77-200 K) para-H(3)(+) ions recombine significantly faster with electrons than ions in the ortho state, in agreement with a recent theoretical prediction. The cavity ring-down absorption spectroscopy used here provides an in situ determination of the para/ortho abundance ratio and yields additional information on the translational and rotational temperatures of the recombining ions. The results show that H(3)(+) recombination with electrons occurs by both binary recombination and third-body (helium) assisted recombination, and that both the two-body and three-body rate coefficients depend on the nuclear spin states. Electron-stabilized (collisional-radiative) recombination appears to make only a small contribution.