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Physical Review A

Characterizing and modeling the efficiency limits in large-scale production of hyperpolarized Xe129

Matthew S. Freeman, Kiarash Emami, Bastiaan Driehuys

Published Aug 6, 2014• 55 citations
Publisher

Abstract

The ability to produce liter volumes of highly-spin-polarized $^{129}\mathrm{Xe}$ enables a wide range of investigations, most notably in the fields of materials science and biomedical magnetic resonance imaging. However, for nearly all polarizers built to date, both peak $^{129}\mathrm{Xe}$ polarization and the rate at which it is produced fall far below those predicted by the standard model of Rb metal vapor, spin-exchange optical pumping (SEOP). In this work we comprehensively characterized a high-volume flow-through $^{129}\mathrm{Xe}$ polarizer using three different SEOP cells with internal volumes of 100, 200, and $300\phantom{\rule{0.16em}{0ex}}{\mathrm{cm}}^{3}$ and two types of optical sources: a broad-spectrum 111-W laser [full width at half maximum (FWHM) equal to 1.92 nm] and a line-narrowed 71-W laser (FWHM equal to 0.39 nm). By measuring $^{129}\mathrm{Xe}$ polarization as a function of gas flow rate, we extracted the peak polarization and polarization production rate across a wide range of laser absorption levels. Peak polarization for all cells consistently remained a factor of 2--3 times lower than predicted at all absorption levels. Moreover, although production rates increased with laser absorption, they did so much more slowly than predicted by the standard theoretical model and basic spin-exchange efficiency arguments. Underperformance was most notable in the smallest optical cells. We propose that all these systematic deviations from theory can be explained by invoking the presence of paramagnetic Rb clusters within the vapor. Cluster formation within saturated alkali-metal vapors is well established and their interaction with resonant laser light was recently shown to create plasmalike conditions. Such cluster systems cause both Rb and $^{129}\mathrm{Xe}$ depolarization, as well as excess photon scattering. These effects were incorporated into the SEOP model by assuming that clusters are activated in proportion to excited-state Rb number density and by further estimating physically reasonable values for the nanocluster-induced velocity-averaged spin-destruction cross section for Rb $(\ensuremath{\langle}{\ensuremath{\sigma}}_{\text{cluster-Rb}}v\ensuremath{\rangle}\phantom{\rule{0.16em}{0ex}}\ensuremath{\approx}\phantom{\rule{0.16em}{0ex}}4\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}7}\phantom{\rule{0.16em}{0ex}}{\mathrm{cm}}^{3}\phantom{\rule{0.16em}{0ex}}{\mathrm{s}}^{\ensuremath{-}1})$, the $^{129}\mathrm{Xe}$ relaxation cross section $(\ensuremath{\langle}{\ensuremath{\sigma}}_{\text{cluster-Xe}}v\ensuremath{\rangle}\phantom{\rule{0.16em}{0ex}}\ensuremath{\approx}\phantom{\rule{0.16em}{0ex}}4\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}13}\phantom{\rule{0.16em}{0ex}}{\mathrm{cm}}^{3}\phantom{\rule{0.16em}{0ex}}{\mathrm{s}}^{\ensuremath{-}1})$, and a non-wavelength-specific photon-scattering cross section $({\ensuremath{\sigma}}_{\mathrm{cluster}}\phantom{\rule{0.16em}{0ex}}\ensuremath{\approx}\phantom{\rule{0.16em}{0ex}}1\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}12}\phantom{\rule{0.16em}{0ex}}{\mathrm{cm}}^{2})$. The resulting modified SEOP model now closely matches experimental observations.

DOI
10.1103/physreva.90.023406

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Here we present a $\mathrm{Rb}\text{\ensuremath{-}}^{129}\mathrm{Xe}$ spin-exchange optical pumping polarizer capable of rapid generation of large volumes of highly polarized 129Xe^{129}\mathrm{Xe}129Xe gas. Through modeling and measurements we maximize the 129Xe^{129}\mathrm{Xe}129Xe nuclear spin polarization output to enable the generation of polarized 129Xe^{129}\mathrm{Xe}129Xe gas imaging volumes (300  cm3300\text{ }\text{ }{\mathrm{cm}}^{3}300  cm3) every 5 min within a clinical setting. Our model is verified by experiment to correctly predict the optimum Rb vapor density for maximum 129Xe^{129}\mathrm{Xe}129Xe nuclear polarization for a flux 3.4  W/cm23.4\text{ }\text{ }\mathrm{W}/{\mathrm{cm}}^{2}3.4  W/cm2 of circularly polarized Rb D1{D}_{1}D1​ photons incident on an 80 cm long cylindrical optical cell. We measure a 129Xe^{129}\mathrm{Xe}129Xe magnetization production efficiency of ${\ensuremath{\eta}}_{\mathrm{pr}}=1.8%$, which approaches the photon efficiency limit ${\ensuremath{\eta}}_{\ensuremath{\gamma}}=3.3%$ of this system and enables the polarization of $2.72\ifmmode\times\else\texttimes\fi{}{10}^{22}$ 129Xe^{129}\mathrm{Xe}129Xe spins per hour, corresponding to 1013  cm31013\text{ }\text{ }{\mathrm{cm}}^{3}1013  cm3 of 100% polarized 129Xe^{129}\mathrm{Xe}129Xe at STP. This magnetization production rate is threefold higher than the highest previously published 129Xe^{129}\mathrm{Xe}129Xe magnetization production rate and has enabled routine clinical lung magnetic resonance imaging (MRI) with hyperpolarized 129Xe^{129}\mathrm{Xe}129Xe doses available on demand at run time, as well as high-SNR 129Xe^{129}\mathrm{Xe}129Xe MRI of the human brain and kidneys.
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 design for a spin-exchange optical pumping system to produce large quantities of highly polarized 129Xe. Low xenon concentrations in the flowing gas mixture allow the laser to maintain high Rb polarization. The large spin-exchange rate between Rb and 129Xe through the long-lived van der Waals molecules at low pressure, combined with a high flow rate, results in large production rates of hyperpolarized xenon. We report a maximum polarization of 64% achieved for a 0.3 l/h Xe flow rate, and maximum magnetization output of 6 l/h at 22% polarization. Our findings regarding the polarization dependence on temperature, nitrogen partial pressure, and gas mixture flow velocity are also reported.
Abstract Efficient production of hyperpolarized 129 Xe at clinically relevant output levels remains an important challenge for spin-exchange optical pumping (SEOP). In this work, we report a comparative experimental study of Cs– 129 Xe and Rb– 129 Xe SEOP. The spin-exchange and spin-relaxation rates are measured and separated into binary-collision and van der Waals (vdW) molecular contributions. The resulting parameter set shows that long-lived vdW interactions enhance the intrinsic spin-exchange efficiency within a narrow pressure window, with Cs exhibiting a modest advantage over Rb under comparable conditions. Using these experimentally constrained quantities in a device-level model, we predict that clinically relevant 129 Xe polarization levels and throughput could be achievable at pump powers near 5 W.
We present a comprehensive theory of nuclear spin polarization of 3He{}^{3}\mathrm{He}3He and 129Xe{}^{129}\mathrm{Xe}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{}^{3}\mathrm{He}3He or 129Xe{}^{129}\mathrm{Xe}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{}^{3}\mathrm{He}3He or 129Xe{}^{129}\mathrm{Xe}129Xe gas are assumed, namely, atmospheres of gas pressure and nearly complete quenching of the optically excited alkali-metal atoms by collisions with N2{\mathrm{N}}_{2}N2​ or H2{\mathrm{H}}_{2}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.
Analytical model for polarization transfer during gas-phase collision events in spin-exchange optical pumping: Spin-12\frac{1}{2}21​ 129^{129}129Xe versus spin-32\frac{3}{2}23​ 131^{131}131Xe
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=1/2I = 1/2I=1/2 nuclei, such as 129Xe, is relatively well understood, that of spin I>1/2I > 1/2I>1/2 nuclei, such as 131Xe (I=3/2I = 3/2I=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)\hatρ(t)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)\hatρ(t)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.