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arXiv:1501.02204 · Physical Review A

Model for the overall phase-space acceptance in a Zeeman decelerator

Katrin Dulitz, Nicolas Vanhaecke, T. P. Softley

Published Jan 22, 2015• 11 citations
arXivHTMLPDF

Abstract

We present a formalism to calculate phase-space acceptance in a Zeeman decelerator. Using parameters closely mimicking previous Zeeman deceleration experiments, this approach reveals a 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 (characterized by the reduced position of the synchronous particle ${\ensuremath{\kappa}}_{0}$) 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-defined characteristics. We also find that the time overlap between fields of adjacent coils has an influence on the phase-space acceptance. Previous theoretical and experimental results [A. W. Wiederkehr et al., Phys. Rev. A 82, 043428 (2010); J. Chem. Phys. 135, 214202 (2011).] suggested unfilled regions in phase space that influence particle transmission through the decelerator. Our model provides a means to directly identify the origin of these effects due to coupling between longitudinal and transverse dynamics. Since optimum phase stability is restricted to a rather small parameter range in terms of the reduced position of the synchronous particle ${\ensuremath{\kappa}}_{0}$, only a limited range of final velocities can be attained using a given number of coils. We evaluate phase stability for different Zeeman deceleration sequences, and by comparison with numerical three-dimensional particle-trajectory simulations, we demonstrate that our model provides a valuable tool to find optimum parameter sets for improved Zeeman deceleration schemes. An acceleration-deceleration scheme is shown to be a useful approach to generating beams with well-defined properties for variable-energy collision experiments. More generally, the model provides significant physical insights that are applicable to other types of particle decelerators with finite rise and fall time fields.

DOI
10.1103/physreva.91.013409

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Phase stability in a multistage Zeeman decelerator

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The phase stability of a multistage Zeeman decelerator is analyzed by numerical particle-trajectory simulations and experimental measurements. A one-dimensional model of the phase stability in multistage Stark deceleration [Bethlem et al., Phys. Rev. Lett. 84, 5744 (2000)] has been adapted to multistage Zeeman deceleration and compared with one- and three-dimensional particle-trajectory simulations, including the analysis of the effect of finite switch-on and -off times of the deceleration pulses. The comparison reveals that transverse effects in the decelerator lead to a considerable reduction of the phase-space acceptance at low values of the phase angle and an enhancement at high values. The optimal combinations of phase angles and currents with which a preset amount of kinetic energy can be removed from atoms and molecules in a pulsed supersonic beam using a multistage decelerator are determined by simulation. Quantitative analysis of the phase-space acceptance within a given volume reveals that for our decelerator (8 $\mathrm{\ensuremath{\mu}}\mathrm{s}$ switch-off time) optimal conditions are achieved for values of the phase angle between ${45}^{\ifmmode^\circ\else\textdegree\fi{}}$ and ${55}^{\ifmmode^\circ\else\textdegree\fi{}}$. This conclusion is examined and confirmed by experimental measurements using deuterium atoms. Alternative approaches to generate optimal deceleration pulse sequences, such as the implementation of evolutionary algorithms or the use of higher-order modes of the decelerator, are discussed.

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Zeeman deceleration is an experimental technique which allows for the manipulation of open-shell atoms and molecules in a supersonic beam thus producing mK-cold, velocity-tunable beams of particles in selected quantum states. The method relies on the Zeeman interaction between paramagnetic particles and time-varying, inhomogeneous magnetic fields generated by pulsing high currents through an array of solenoid coils. This thesis describes the construction and implementation of a supersonic beam setup including a 12-stage Zeeman decelerator. The Zeeman decelerator follows an original design that makes it possible to replace individual deceleration coils. Using ground-state hydrogen atoms as a test system, it is shown that the transverse acceptance in a Zeeman decelerator can be significantly increased by generating a rather low, temporally varying quadrupole field in one of the solenoid coils. An electron-impact source was constructed and optimised enabling, for the first time, the Zeeman deceleration of metastable helium atoms in the 23S1 state, with an up to 40 % decrease in the kinetic energy of the beam. It is shown that the pulse duration for electron-impact excitation needs to be matched to the acceptance of the decelerator in order to attain a good contrast between the decelerated and undecelerated parts of the beam. Experimental results are rigorously analysed and interpreted using three-dimensional numerical particle trajectory simulations. A phase-space model provides, for the first time, a means to estimate the six-dimensional phase-space acceptance in a Zeeman decelerator and to find optimum parameter sets for improved Zeeman deceleration schemes. The approach also reveals a hitherto unconsidered velocity dependence of the phase stability which is ascribed mainly to the rise and fall times of the current pulses that generate the magnetic fields inside the deceleration coils. In the future, it is planned to combine the Zeeman decelerator with a source of cold atomic and molecular ions to study chemical collisions at low temperatures. A hybrid magnetic guide consisting of permanent magnet assemblies (Halbach arrays) in hexapole configuration and a set of current-carrying wires is proposed and simulated as an interface between these setups. The design promises very efficient velocity selection, a high degree of quantum-state selection and a nearly complete removal of residual carrier gas. Prospects for using magnetic hexapole focusing in front of the Zeeman decelerator are discussed. The work represents a major step towards the study and control of chemical reactivity of paramagnetic species in the low-temperature regime and it will help in the testing of fundamental chemical reaction theories.

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We present a formalism to calculate phase-space acceptance in a Zeeman decelerator. Using parameters closely mimicking previous Zeeman deceleration experiments, this approach reveals a 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 (characterized by the reduced position of the synchronous particle \ensuremathκ0{\ensuremath{\kappa}}_{0}\ensuremathκ0​) 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-defined characteristics. We also find that the time overlap between fields of adjacent coils has an influence on the phase-space acceptance. Previous theoretical and experimental results [A. W. Wiederkehr et al., Phys. Rev. A 82, 043428 (2010); J. Chem. Phys. 135, 214202 (2011).] suggested unfilled regions in phase space that influence particle transmission through the decelerator. Our model provides a means to directly identify the origin of these effects due to coupling between longitudinal and transverse dynamics. Since optimum phase stability is restricted to a rather small parameter range in terms of the reduced position of the synchronous particle \ensuremathκ0{\ensuremath{\kappa}}_{0}\ensuremathκ0​, only a limited range of final velocities can be attained using a given number of coils. We evaluate phase stability for different Zeeman deceleration sequences, and by comparison with numerical three-dimensional particle-trajectory simulations, we demonstrate that our model provides a valuable tool to find optimum parameter sets for improved Zeeman deceleration schemes. An acceleration-deceleration scheme is shown to be a useful approach to generating beams with well-defined properties for variable-energy collision experiments. More generally, the model provides significant physical insights that are applicable to other types of particle decelerators with finite rise and fall time fields.
The phase stability of a multistage Zeeman decelerator is analyzed by numerical particle-trajectory simulations and experimental measurements. A one-dimensional model of the phase stability in multistage Stark deceleration [Bethlem et al., Phys. Rev. Lett. 84, 5744 (2000)] has been adapted to multistage Zeeman deceleration and compared with one- and three-dimensional particle-trajectory simulations, including the analysis of the effect of finite switch-on and -off times of the deceleration pulses. The comparison reveals that transverse effects in the decelerator lead to a considerable reduction of the phase-space acceptance at low values of the phase angle and an enhancement at high values. The optimal combinations of phase angles and currents with which a preset amount of kinetic energy can be removed from atoms and molecules in a pulsed supersonic beam using a multistage decelerator are determined by simulation. Quantitative analysis of the phase-space acceptance within a given volume reveals that for our decelerator (8 $\mathrm{\ensuremath{\mu}}\mathrm{s}$ switch-off time) optimal conditions are achieved for values of the phase angle between ${45}^{\ifmmode^\circ\else\textdegree\fi{}}$ and ${55}^{\ifmmode^\circ\else\textdegree\fi{}}$. This conclusion is examined and confirmed by experimental measurements using deuterium atoms. Alternative approaches to generate optimal deceleration pulse sequences, such as the implementation of evolutionary algorithms or the use of higher-order modes of the decelerator, are discussed.
Zeeman deceleration is an experimental technique which allows for the manipulation of open-shell atoms and molecules in a supersonic beam thus producing mK-cold, velocity-tunable beams of particles in selected quantum states. The method relies on the Zeeman interaction between paramagnetic particles and time-varying, inhomogeneous magnetic fields generated by pulsing high currents through an array of solenoid coils. This thesis describes the construction and implementation of a supersonic beam setup including a 12-stage Zeeman decelerator. The Zeeman decelerator follows an original design that makes it possible to replace individual deceleration coils. Using ground-state hydrogen atoms as a test system, it is shown that the transverse acceptance in a Zeeman decelerator can be significantly increased by generating a rather low, temporally varying quadrupole field in one of the solenoid coils. An electron-impact source was constructed and optimised enabling, for the first time, the Zeeman deceleration of metastable helium atoms in the 23S1 state, with an up to 40 % decrease in the kinetic energy of the beam. It is shown that the pulse duration for electron-impact excitation needs to be matched to the acceptance of the decelerator in order to attain a good contrast between the decelerated and undecelerated parts of the beam. Experimental results are rigorously analysed and interpreted using three-dimensional numerical particle trajectory simulations. A phase-space model provides, for the first time, a means to estimate the six-dimensional phase-space acceptance in a Zeeman decelerator and to find optimum parameter sets for improved Zeeman deceleration schemes. The approach also reveals a hitherto unconsidered velocity dependence of the phase stability which is ascribed mainly to the rise and fall times of the current pulses that generate the magnetic fields inside the deceleration coils. In the future, it is planned to combine the Zeeman decelerator with a source of cold atomic and molecular ions to study chemical collisions at low temperatures. A hybrid magnetic guide consisting of permanent magnet assemblies (Halbach arrays) in hexapole configuration and a set of current-carrying wires is proposed and simulated as an interface between these setups. The design promises very efficient velocity selection, a high degree of quantum-state selection and a nearly complete removal of residual carrier gas. Prospects for using magnetic hexapole focusing in front of the Zeeman decelerator are discussed. The work represents a major step towards the study and control of chemical reactivity of paramagnetic species in the low-temperature regime and it will help in the testing of fundamental chemical reaction theories.
A modular multistage Zeeman decelerator consisting of an array of solenoids has been developed to control the velocity of cold, paramagnetic atoms and molecules in supersonic beams. The translational motion these atoms and molecules was manipulated with high precision by exploiting the interaction between their magnetic moments and timedependent inhomogeneous magnetic elds. Deceleration was achieved by pulsing high currents (up to 300 A) through the solenoids of the decelerator with pulse sequences calculated to preserve the phase-space density of the atomic and molecular samples while removing a preset amount of kinetic energy. For the operation of the multistage Zeeman decelerator, solenoids and electronic units were developed to generate strong magneticeld pulses (> 2 T) with rise and fall times of only a few microseconds. An accurate three-dimensional particle-trajectory simulation program has been developed to analyze the deceleration process and optimize its e ciency. This software was thoroughly tested by systematic comparison with experimental results and enabled, in combination with measurements, the complete characterization of the spatial and velocity distributions of the decelerated and trapped atoms for di erent sets of experimental conditions. The program was essential to achieve a complete interpretation of the dynamics of the deceleration process and to devise a strategy to e ciently load the decelerated atoms and molecules into magnetic quadrupole traps. In a rst experiment, hydrogen atoms seeded in a supersonic expansion of Kr have been decelerated from an initial velocity of 435 m/s to nal velocities as low as 107 m/s in a 12-stage Zeeman decelerator. The operation of the decelerator has been analyzed by comparing the results of numerical particle-trajectory simulations with those of independent measurements of the velocity distribution by ion time-ofight mass spectrometry following photoionization of the decelerated atoms. The velocity distribution of the decelerated atom cloud was found to have a half width at half maximum of 25± 12 m/s corresponding to a temperature of ∼ 40 mK. The phase stability of the multistage-Zeeman-deceleration process has been investigated by numerical particle-trajectory simulations and experimental measurements on deuterium atoms in a 24-stage Zeeman decelerator. A one-dimensional analytical model of the phase stability in a multistage Zeeman decelerator was adapted from a one-dimensional model of phase stability in a multistage Stark decelerator and compared with the results of oneand three-dimensional particle-trajectory simulations. The comparison, which included the analysis of the e ects of nite switch-on and switch-o times of the deceleration pulses, revealed that transverse e ects in the decelerator lead to a considerable reduction of the
We present a concept for a multistage 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-dimensional phase-space acceptance. The separated focusing and deceleration elements result in an unequal partitioning of this acceptance between the longitudinal and transverse directions. This is ideal in scattering experiments, which typically benefit from a large longitudinal acceptance combined with narrow transverse distributions. We demonstrate the successful experimental implementation of this concept using a Zeeman decelerator consisting 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^{3}S3S) 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 which cooling liquid is passed. The solenoid design allows for excellent thermal properties and enables the use of readily available and cheap electronics components to pulse high currents through the solenoids. The Zeeman decelerator demonstrated here is mechanically easy to build, can be operated with cost-effective electronics, and can run at repetition rates up to 10 Hz.
In Zeeman deceleration, time-varying spatially inhomogeneous magnetic fields are used to create packets of translationally cold, quantum-state-selected paramagnetic particles with a tuneable forward velocity, which are ideal for cold reaction dynamics studies. Here, the covariance matrix adaptation evolutionary strategy is adopted in order to optimise deceleration switching sequences for the operation of a Zeeman decelerator. Using the optimised sequences, a 40% increase in the number of decelerated particles is observed compared to standard sequences for the same final velocity, imposing the same experimental boundary conditions. Furthermore, we demonstrate that it is possible to remove up to 98% of the initial kinetic energy of particles in the incoming beam, compared to the removal of a maximum of 83% of kinetic energy with standard sequences. Three-dimensional particle trajectory simulations are employed to reproduce the experimental results and to investigate differences in the deceleration mechanism adopted by standard and optimised sequences. It is experimentally verified that the optimal solution uncovered by the evolutionary algorithm is not merely a local optimisation of the experimental parameters—it is a novel mode of operation that goes beyond the standard periodic phase stability approach typically adopted.
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 can be significantly increased with only minor changes to the setup itself. This is achieved by applying a rather low, anti-parallel magnetic field in one of the solenoid coils that forms a temporally varying quadrupole field, and improves particle confinement in the transverse direction. The results are reproduced by three-dimensional numerical particle trajectory simulations thus allowing for a rigorous analysis of the experimental data. The findings suggest the use of a modified coil configuration to improve transverse focusing during the deceleration process.