A new model is presented for spin-exchange optical pumping using an open-source code, ElmerFEM-CSC. The model builds on previous models by adding the effects of alkali-vapor heterogeneity in optical pumping cells and by modeling the effects of hyperpolarized-gas wall-relaxation using a diffusion model. The code supports full, three-dimensional solutions to optical-pumping models, and solves for (1) laser absorption, (2) alkali vapor concentration, (3) fluid flow parameters, (4) thermal affects due to the pumping laser, and (5) noble gas polarization. The source code for the model is available for researchers to utilize and modify.
We present a finite-element analysis of the fluid dynamics, thermal dynamics, and alkali diffusion in a common cell geometry used for spin-exchange optical pumping of
129Xe using a flow-through polarizer design. The analysis is the first to simulate aspects of the laser run-away effect observed in some optical pumping cells. The analysis further suggests that high-temperature gas in the outlet tube may give rise to rapid depolarization due to high concentrations of alkali vapor. Finally, the analysis indicates that the alkali number density distribution and the specifics of the dynamics are highly dependent upon the the distribution of the alkali metal in the optical pumping portion and outlet tube of the cell.
While the method of Spin-exchange optical pumping, SEOP, of noble gases has existed since 1960 [Bouchiat60], many fundamental aspects of spin exchange optical pumping have gone largely unexplained. These questions included the values of the rate coefficients for spin-exchange, many aspects of the alkali-metal polarization and density inside the SEOP cells, the mechanisms of He wall relaxation, non-ideal values of the observed He polarization, and efficiency to produce it. This thesis describes the results of our efforts to quantity all parameters in SEOP and to begin to determine some of these unknowns. This thesis presents measurements of spin-exchange rate coefficients and efficiencies. A method to extend SEOP to multiple alkali species is presented. In addition, limits to the efficiency of optical pumping, the efficiency of spin-exchange, and the observed He polarization are explored.
The applicability of commonly used 129Xe nuclear polarization (PXe) buildup models to large optical cell polarizers, which operate at lower gas pressures when compared to small cell polarizers for which spin-exchange optical pumping (SEOP) models were originally developed, has yet to be systematically evaluated. In addition, spatial heterogeneity of Rb vapor density ([Rb]) and its impact on SEOP in low pressure, large optical cell polarizers remains poorly understood. In this theoretical study, it was shown that 1D analytical and numerical PXe buildup models yield diverging PXe and critical flow rate values at low flow rates and high laser absorption, contributing to the discrepancy between theoretical and experimentally measured production rates. Additionally, it was found that [Rb] heterogeneity leads to lower PXe buildup and an undesirable increase in optimal cell temperature, while the optimal laser absorption remains relatively unchanged. The updated simulation framework presented here can be utilized to model other SEOP systems.
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 experimentally and theoretically investigate the effect of optical pump beam size on narrowband spin polarized optical pumping of alkali atom vapor. We developed a six-level model describing narrowband spin polarized optical pumping of alkali atoms and applied this model to an atomic vapor cell, accounting for atomic transit time through the optical beam and wall collision effects. Our expression for the wall collision effects is derived from the diffusion model. Overall, we obtained good agreement between theory and experimentally measured relaxation time constants.
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.