The spectroscopic characteristics of the polarization of 129Xe nuclei in Xe gas by spin exchange with optically pumped Rb atoms is examined in high magnetic field. The high field Zeeman effect provides the spectral dispersion necessary to separate the effects of different light polarizations and incident wavelengths on the pumping cycle. Indirect detection of the D1 line in Rb using 129Xe nuclear magnetic resonance in combination with direct optical detection indicates that conventional container construction significantly decreases the efficiency of the 129Xe polarization. The decreased pumping efficiency is due to randomly polarized photons that can be eliminated by using containers with good optical quality windows. Study of these effects is facilitated by the large Zeeman shifts obtained with multi-tesla fields which resolve the D1 multiplet structure even in the presence of the significant pressure-broadening incells with typical gas pressures of 0⋅1-1 atm.
We present a constructed setup for polarizing 129 Xe noble gas. Hyperpolarized 129 Xe has been obtained via spin exchange with an optically pumped rubidium vapor. Optical pumping is based on polarizing the valence electron of rubidium by the resonant absorption of a circularly polarized laser light. The magnetic field of 30 G was used for obtaining 129 Xe polarization. The apparatus for detecting polarization is a nuclear magnetic resonance spectrometer. The highest 129 Xe polarization of 54% has been obtained using 60 W circularly polarized laser light with wavelength of 794.7 nm. The measured longitudinal relaxation time of the hyperpolarized 129 Xe was 72.3 minutes.
We present a comprehensive theory of nuclear spin polarization of
3He and
129Xe gases by spin-exchange collisions with optically pumped alkali-metal vapors. The most important physical processes considered are (1) spin-conserving spin-exchange collisions between like or unlike alkali-metal atoms; (2) spin-destroying collisions of the alkali-metal atoms with each other and with buffer-gas atoms; (3) electron-nuclear spin-exchange collisions between alkali-metal atoms and
3He or
129Xe atoms; (4) spin interactions in van der Waals molecules consisting of a Xe atom bound to an alkali-metal atom; (5) optical pumping by laser photons; (6) spatial diffusion. The static magnetic field is assumed to be small enough that the nuclear spin of the alkali-metal atom is well coupled to the electron spin and the total spin is very nearly a good quantum number. Conditions appropriate for the production of large quantities of spin-polarized
3He or
129Xe gas are assumed, namely, atmospheres of gas pressure and nearly complete quenching of the optically excited alkali-metal atoms by collisions with
N2 or
H2 gas. Some of the more important results of this work are as follows: (1) Most of the pumping and relaxation processes are sudden with respect to the nuclear polarization. Consequently, the steady-state population distribution of alkali-metal atoms is well described by a spin temperature, whether the rate of spin-exchange collisions between alkali-metal atoms is large or small compared to the optical pumping rate or the collisional spin-relaxation rates. (2) The population distributions that characterize the response to sudden changes in the intensity of the pumping light are not described by a spin temperature, except in the limit of very rapid spin exchange. (3) Expressions given for the radio-frequency (rf) resonance linewidths and areas can be used to make reliable estimates of the local spin polarization of the alkali-metal atoms. (4) Diffusion effects for these high-pressure conditions are mainly limited to thin layers at the cell surface and at internal resonant surfaces generated by radio-frequency magnetic fields when the static magnetic field has substantial spatial inhomogeneities. The highly localized effects of diffusion at these surfaces are described with closed-form analytic functions instead of the spatial eigenmode expansions that are appropriate for lower-pressure cells.
We have measured the binary spin-exchange rate coefficient for collisions between Rb and
129Xe atoms at a magnetic field
B=9.4T and in the temperature range $160<T<200\ifmmode^\circ\else\textdegree\fi{}\mathrm{C}.$ The longitudinal spin-relaxation rate
1/T1 of
129Xe is dominated by ${}^{129}\mathrm{Xe}\ensuremath{-}\mathrm{Rb}$ binary collisions. We measured
1/T1 using the methods of conventional nuclear magnetic resonance, with no spin enhancement by optical pumping. At the high magnetic field and large gas pressures used in this work, the contribution of ${}^{129}\mathrm{Xe}\ensuremath{-}\mathrm{Rb}$ molecules to the spin-exchange rate was less than 0.1% of the binary-collision rate. The Rb atomic number density [Rb] was measured directly from the large Faraday rotation of the polarization of near-resonant light passing through the sample cells. The rate coefficient is $\ensuremath{\kappa}{=d(1/T}_{1})/d[\mathrm{Rb}]=(1.75\ifmmode\pm\else\textpm\fi{}0.12)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}16}{\mathrm{cm}}^{3}/\mathrm{s}.$
Abstract The polarization of 129 Xe gas by spin exchange with optically pumped Rb vapor is examined in high magnetic field. Measurements of the Rb–Xe velocity averaged spin exchange cross section 〈 σ v 〉 and the 129 Xe relaxation time in the absence of Rb, T 1 Xe , are discussed. Comparison of these high field results to low field literature values for 〈 σ v 〉 show that this parameter is essentially field independent. T 1 Xe is also found to be significantly longer in high field. On the basis of these observations, it is shown that production of large amounts of spin polarized 129 Xe gas can be made more efficient by high field operation.
Spin-exchange optical pumping (SEOP) is a method for producing spin-hyperpolarized noble gas nuclei, such as 129Xe and 131Xe, which are used in various magnetic resonance applications from fundamental physics to quantum sensing and medical imaging. In SEOP, optically polarized alkali-metal atoms transfer their spin polarization to the noble gas nuclei in gas-phase collision events via the hyperfine coupling (HFC) between the alkali valence electron and the noble gas nucleus. While the polarization transfer physics of spin
I=1/2 nuclei, such as 129Xe, is relatively well understood, that of spin
I>1/2 nuclei, such as 131Xe (
I=3/2), has been far less studied, and no rigorous theoretical model has been presented to date. To this end, we derive a simple analytical model for the upper limit, neglecting relaxation, of the SEOP polarization transfer, applicable to noble gases with arbitrary nuclear spin. Analytical evaluation of the Baker-Campbell-Hausdorff expansion for the time evolution of the spin density operator
ρ^(t) reveals that only even-order terms in the HFC contribute to the polarization transfer, with the leading-order quadratic term being the most significant. We obtain a result similar to that derived for the spin-exchange cross section by Herman [Phys. Rev. 137, A 1062 (1965)], but in a more general framework for the time evolution of
ρ^(t) that is also more familiar to magnetic resonance researchers. The model is applied to understand the difference in the polarization transfer efficiency between 129Xe and 131Xe, yielding results in agreement with previous experiments. We also validate the model by comparison to detailed numerical multiscale simulations of the SEOP process, where full quantum-chemically computed spin Hamiltonians sampled from molecular dynamics simulations of the gas-phase collision events are used to propagate the spin dynamics.