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Journal of the Vacuum Society of Japan

Selection of a Single Spin-rotational State of Molecular Oxygen by a Hexapole Magnet

Mitsunori Kurahashi, Yasushi Yamauchi

Published Jan 1, 2010• 0 citations
Publisher

Abstract

O2 is one of the most important chemical species in every field of natural science. In the present study, a state-selected triplet molecular oxygen beam, in which nearly 100% of the molecules are in the spin-rotational state of (J, M)=(2, 2), has been produced by combining a supersonic seeded O2 beam with a hexapole magnet. The (2, −2) beam with >90% purity has also been obtained by a controlled non-adiabatic transition. The (2, ±2) beam, for which we can determine the spin and rotational angular momenta of O2 almost independently, is the most promising probe for studying the spin effects as well as the steric effects in O2 molecular scattering.

DOI
10.3131/jvsj2.53.681

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O2 is one of the most important chemical species in every field of natural science. In the present study, a state-selected triplet molecular oxygen beam, in which nearly 100% of the molecules are in the spin-rotational state of (J, M)=(2, 2), has been produced by combining a supersonic seeded O2 beam with a hexapole magnet. The (2, −2) beam with >90% purity has also been obtained by a controlled non-adiabatic transition. The (2, ±2) beam, for which we can determine the spin and rotational angular momenta of O2 almost independently, is the most promising probe for studying the spin effects as well as the steric effects in O2 molecular scattering.
A state-selected O(2)((3)Sigma(g)(-)) molecular beam, in which nearly 100% of the molecules are in the spin-rotational state of (J,M) = (2,2), has been produced by combining a supersonic seeded O(2) beam with a hexapole magnet. The (2,-2) beam has also been obtained by the state inversion of the (2,2) beam through the nonadiabatic passage in a reversing longitudinal magnetic field along the beam axis. The intensities of the other (2,M) states, which appear when applying additional transverse magnetic fields to the reversing field region, were well reproduced by the Majorana's formula for J = 2. The (2,+/-2) beam, for which we can determine the spin and rotational angular momenta of O(2) almost independently, is the most promising probe for studying the spin effects as well as the steric effects in O(2) molecular scattering.
Cold samples of oxygen molecules in supersonic beams have been decelerated from initial velocities of 390 and 450 m s−1 to final velocities in the range between 150 and 280 m s−1 using a 90-stage Zeeman decelerator. (2 + 1) resonance-enhanced-multiphoton-ionization (REMPI) spectra of the 3sσ g 3Π g (C) two-photon transition of O2 have been recorded to characterize the state selectivity of the deceleration process. The decelerated molecular sample was found to consist exclusively of molecules in the J ′′ = 2 spin–rotational component of the X ground state of O2. Measurements of the REMPI spectra using linearly polarized laser radiation with polarization vector parallel to the decelerator axis, and thus to the magnetic-field vector of the deceleration solenoids, further showed that only the magnetic sublevel of the N′′ = 1, J ′′ = 2 spin–rotational level is populated in the decelerated sample, which therefore is characterized by a fully oriented total-angular-momentum vector. By maintaining a weak quantization magnetic field beyond the decelerator, the polarization of the sample could be maintained over the 5 cm distance separating the last deceleration solenoid and the detection region.
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.
In the past, the Stern–Gerlach experiment has been used as a standard method for analyzing the population of magnetic substates contained in spin-polarized and/or state-selected atomic/molecular beams. However, this experiment is quite demanding due to its low signal intensity and difficulty in beam alignment. The present study shows that the use of a hexapole magnet and a spin flipper, together with the time-of-flight analysis, allows us to conduct an almost equivalent analysis while greatly improving the signal intensity. Applications to the analysis of spin-polarized triplet excited helium and state-selected O2( 3 Σg−) beams are presented.
We have demonstrated that supersonic beams of oxygen molecules (O2)({\text{O}}_{2})(O2​) in the ground rotational state were slowed to a near standstill by a linear Zeeman decelerator and successfully confined spatially in an anti-Helmholtz magnetic trap. The translational temperature of the decelerated O2{\text{O}}_{2}O2​ molecules was about 800 mK. The demonstrated trapping capability of paramagnetic species opens up various possibilities for the investigation of cold collisions and reactions of various radicals in the sub-kelvin regime by spatially confining them in a magnetic trap.
Collision cross sections and rate constants between two ground-state oxygen molecules are investigated theoretically at translational energies below $\ensuremath{\sim}1$ K and in zero magnetic field. We present calculations for elastic and spin-changing inelastic collision rates for different isotopic combinations of oxygen atoms as a prelude to understanding their collisional stability in ultracold magnetic traps. A numerical analysis has been made in the framework of a rigid-rotor model that accounts fully for the singlet, triplet, and quintet potential-energy surfaces in this system. The results offer insights into the effectiveness of evaporative cooling and the properties of molecular Bose-Einstein condensates, as well as estimates of collisional lifetimes in magnetic traps. Specifically, 17O2{}^{17}{\mathrm{O}}_{2}17O2​ looks like a good candidate for ultracold studies, while 16O2{}^{16}{\mathrm{O}}_{2}16O2​ is unlikely to survive evaporative cooling. Since 17O2{}^{17}{\mathrm{O}}_{2}17O2​ is representative of a wide class of molecules that are paramagnetic in their ground state we conclude that many molecules can be successfully magnetically trapped at ultralow temperatures.