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Physical Review A

Molecular-beam resonance method with Zeeman-decelerated samples: Application to metastable helium molecules

Luca Semeria, Paul Jansen, Gloria Clausen, Josef A. Agner, Hansjürg Schmutz, Frédéric Merkt

Published Dec 26, 2018• 17 citations
Publisher

Abstract

We use a multistage Zeeman decelerator to generate slow beams ($v\ensuremath{\simeq}100\phantom{\rule{0.16em}{0ex}}\mathrm{m}/\mathrm{s}$) of translationally cold, spin-polarized metastable $a\phantom{\rule{0.16em}{0ex}}^{3}\mathrm{\ensuremath{\Sigma}}_{u}^{+}\phantom{\rule{4pt}{0ex}}{\mathrm{He}}_{2}$ molecules and perform a precision measurement of their spin-rotation fine structure. The spin polarization results from the elimination of the high-field-seeking $J=N$ spin-rotational component of each rotational level (rotational quantum number $N$) by the Zeeman deceleration process. By repopulating the $J=N$ component from the $J=N\ifmmode\pm\else\textpm\fi{}1$ low-field-seeking components using radio-frequency radiation, we measured the spin-rotation fine structure of 13 rovibrational levels with $v=0$, 1 and $N=1\text{--}21$. The low beam velocity and the resulting long interaction times with the radio-frequency radiation were exploited to determine the transition frequencies with a precision of 300 Hz.

DOI
10.1103/physreva.98.062518

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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 the moving frame of the decelerated sample. In combination with particle-trajectory simulations, these measurements allowed the phase-space acceptance of the decelerator to be quantified. The degree of isotope separation that can be achieved by multistage Zeeman deceleration was also studied by performing experiments with pulse sequences generated for ²⁰Ne and ²²Ne. © 2011 American Institute of Physics.

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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. We use this decelerator to demonstrate the state-selective deceleration of atomic oxygen to final mean velocities in the range 500--125 m/s. We further characterize our decelerator with molecular oxygen, which, despite its heavier mass, is velocity tuned in the range 350--150 m/s. This corresponds to a maximum kinetic-energy reduction of 95% and 80% for atomic and molecular oxygen, respectively. The long multistage Zeeman decelerator presented here demonstrates that the concept of using alternating hexapoles and solenoids is truly phase stable. This Zeeman decelerator is ideally suited for applications in crossed-beam scattering experiments; the state-selected and velocity-controlled samples of O atoms and ${\mathrm{O}}_{2}$ molecules are particularly relevant for studies of inelastic and reactive processes.

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We use a multistage Zeeman decelerator to generate slow beams (v\ensuremath≃100m/sv\ensuremath{\simeq}100\phantom{\rule{0.16em}{0ex}}\mathrm{m}/\mathrm{s}v\ensuremath≃100m/s) of translationally cold, spin-polarized metastable a3\ensuremathΣu+He2a\phantom{\rule{0.16em}{0ex}}^{3}\mathrm{\ensuremath{\Sigma}}_{u}^{+}\phantom{\rule{4pt}{0ex}}{\mathrm{He}}_{2}a3\ensuremathΣu+​He2​ molecules and perform a precision measurement of their spin-rotation fine structure. The spin polarization results from the elimination of the high-field-seeking J=NJ=NJ=N spin-rotational component of each rotational level (rotational quantum number NNN) by the Zeeman deceleration process. By repopulating the J=NJ=NJ=N component from the J=N\ifmmode±\else\textpm\fi1J=N\ifmmode\pm\else\textpm\fi{}1J=N\ifmmode±\else\textpm\fi1 low-field-seeking components using radio-frequency radiation, we measured the spin-rotation fine structure of 13 rovibrational levels with v=0v=0v=0, 1 and N=1–21N=1\text{--}21N=1–21. The low beam velocity and the resulting long interaction times with the radio-frequency radiation were exploited to determine the transition frequencies with a precision of 300 Hz.
We report on the use of multistage Zeeman deceleration to generate beams of He2{\mathrm{He}}_{2}He2​ molecules in the metastable $a\phantom{\rule{0.16em}{0ex}}{}^{3}{\ensuremath{\Sigma}}_{u}^{+}$ state with velocities tunable down to 100 m/s. The metastable molecules are generated by striking a discharge in a supersonic expansion of pure helium gas from a pulsed valve held at cryogenic temperature. The velocity and internal-state distributions of the metastable He2{\mathrm{He}}_{2}He2​ molecules are measured for nozzle temperatures of 300, 77, and 10 K by high-resolution photoelectron and photoionization spectroscopy. The deceleration process does not exhibit any rotational state selectivity with rotational levels up to ${N}^{\ensuremath{'}\ensuremath{'}}=21$ being populated, but eliminates molecules in spin-rotational sublevels with ${J}^{\ensuremath{'}\ensuremath{'}}={N}^{\ensuremath{'}\ensuremath{'}}$ from the beam, where ${J}^{\ensuremath{'}\ensuremath{'}}$ and ${N}^{\ensuremath{'}\ensuremath{'}}$ are the total and the rotational angular momentum quantum number, respectively. The lack of rotational state selectivity is attributed to the fact that the Paschen-Back regime of the Zeeman effect in the rotational levels of He2{\mathrm{He}}_{2}He2​ is already reached at fields of only 0.1 T.
"Having three and four electrons, respectively, He2+_2^+2+​ and He2_22​ represent systems for which highly accurate \textit{ab-initio} calculations might become feasible in the near future\footnote{W.-C. Tung, M. Pavanello, L. Adamowicz, \textit{J. Chem. Phys.} \textbf{136}, 104309 (2012).}. With the goal of performing accurate measurements of the rovibrational energy-level structure of He2+_2^+2+​ by Rydberg spectroscopy of He2_22​ and multichannel quantum-defect theory extrapolation techniques\footnote{D. Sprecher, J. Liu, T. Kr\""ahenmann, M. Sch\""afer, and F. Merkt, \textit{J. Chem. Phys.} \textbf{140}, 064304 (2014).}, we have produced samples of helium molecules in the a3Σu+a ^3\Sigma_\mathrm{u}^+a3Σu+​ state in supersonic beams with velocities tunable down to 100\,m/s by combining a cryogenic supersonic-beam source with a multistage Zeeman decelerator\footnote{M. Motsch, P. Jansen, J. A. Agner, H. Schmutz, and F. Merkt, \textit{arXiv:1401.7774}.}. The molecules are formed at an initial velocity of 500 m/s by striking a discharge in the pulsed expansion of helium gas from a reservoir kept at a cryogenic temperature of 10 K. Using rotationally-resolved PFI-ZEKE (pulsed-field-ionization zero-kinetic-energy) photoelectron spectroscopy, we have probed the rotational-state distribution of the molecules produced in the discharge and found vibrational levels up to ν′′=2\nu'' = 2ν′′=2 and rotational levels up to N′′=21N''=21N′′=21 to be populated. The molecular beam is coupled to a multistage Zeeman decelerator\footnote{N. Vanhaecke, U. Meier, M. Andrist, B. H. Meier, and F. Merkt, \textit{Phys. Rev. A} \textbf{75}, 031402(R) (2007).} that employs pulsed inhomogeneous magnetic fields to further reduce the beam velocity. By measuring the quantum-state distribution of the decelerated sample using photoelectron and photoionization spectroscopy we observed no rotational or vibrational state-selectivity of the deceleration process, but found that one of the three spin-rotation components of the He2_22​ a3Σu+a ^3\Sigma_\mathrm{u}^+a3Σu+​ rotational levels is eliminated."
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
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 the moving frame of the decelerated sample. In combination with particle-trajectory simulations, these measurements allowed the phase-space acceptance of the decelerator to be quantified. The degree of isotope separation that can be achieved by multistage Zeeman deceleration was also studied by performing experiments with pulse sequences generated for ²⁰Ne and ²²Ne. © 2011 American Institute of Physics.
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 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 decelerator features a modular design that is mechanically easy to extend to arbitrary length and allows for solenoid and hexapole elements that are convenient to replace. The solenoids and associated electronics are efficiently water cooled and allow the Zeeman decelerator to operate at repetition rates exceeding 10 Hz. We characterize the performance of the decelerator using various beams of metastable rare gas atoms. Imaging of the atoms that exit the Zeeman decelerator reveals the transverse focusing properties of the hexapole array in the Zeeman decelerator.
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. We use this decelerator to demonstrate the state-selective deceleration of atomic oxygen to final mean velocities in the range 500--125 m/s. We further characterize our decelerator with molecular oxygen, which, despite its heavier mass, is velocity tuned in the range 350--150 m/s. This corresponds to a maximum kinetic-energy reduction of 95% and 80% for atomic and molecular oxygen, respectively. The long multistage Zeeman decelerator presented here demonstrates that the concept of using alternating hexapoles and solenoids is truly phase stable. This Zeeman decelerator is ideally suited for applications in crossed-beam scattering experiments; the state-selected and velocity-controlled samples of O atoms and O2{\mathrm{O}}_{2}O2​ molecules are particularly relevant for studies of inelastic and reactive processes.