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Physical Review Letters

Xe 129 -Rb Spin-Exchange Optical Pumping with High Photon Efficiency

Graham Norquay, Guilhem J. Collier, Madhwesha R. Rao, Neil J. Stewart, Jim M. Wild

Published Oct 8, 2018• 95 citations
Publisher

Abstract

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 $^{129}\mathrm{Xe}$ gas. Through modeling and measurements we maximize the $^{129}\mathrm{Xe}$ nuclear spin polarization output to enable the generation of polarized $^{129}\mathrm{Xe}$ gas imaging volumes ($300\text{ }\text{ }{\mathrm{cm}}^{3}$) every 5 min within a clinical setting. Our model is verified by experiment to correctly predict the optimum Rb vapor density for maximum $^{129}\mathrm{Xe}$ nuclear polarization for a flux $3.4\text{ }\text{ }\mathrm{W}/{\mathrm{cm}}^{2}$ of circularly polarized Rb ${D}_{1}$ photons incident on an 80 cm long cylindrical optical cell. We measure a $^{129}\mathrm{Xe}$ 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 $2.72\ifmmode\times\else\texttimes\fi{}{10}^{22}$ $^{129}\mathrm{Xe}$ spins per hour, corresponding to $1013\text{ }\text{ }{\mathrm{cm}}^{3}$ of 100% polarized $^{129}\mathrm{Xe}$ at STP. This magnetization production rate is threefold higher than the highest previously published $^{129}\mathrm{Xe}$ magnetization production rate and has enabled routine clinical lung magnetic resonance imaging (MRI) with hyperpolarized $^{129}\mathrm{Xe}$ doses available on demand at run time, as well as high-SNR $^{129}\mathrm{Xe}$ MRI of the human brain and kidneys.

DOI
10.1103/physrevlett.121.153201

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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.
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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.
The ability to produce liter volumes of highly-spin-polarized 129Xe^{129}\mathrm{Xe}129Xe 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 129Xe^{129}\mathrm{Xe}129Xe 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 129Xe^{129}\mathrm{Xe}129Xe polarizer using three different SEOP cells with internal volumes of 100, 200, and 300cm3300\phantom{\rule{0.16em}{0ex}}{\mathrm{cm}}^{3}300cm3 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 129Xe^{129}\mathrm{Xe}129Xe 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 129Xe^{129}\mathrm{Xe}129Xe 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 129Xe^{129}\mathrm{Xe}129Xe 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.
A method is described for producing several liters of nuclear spin polarized 129Xe gas via spin exchange with an optically pumped Rb vapor. We use a 140 W AlGaAs laser diode array whose broad spectral output is efficiently absorbed by employing ∼10 atm of 4He to pressure broaden the Rb D1 absorption profile. 129Xe is polarized in a continuous gas flow and is then cryogenically accumulated and stored. Extensions of this technique should enable the production of tens of liters of 129Xe with a nuclear spin polarization of order 50%. Production of laser-polarized 129Xe in liter quantities is important for the continued development of magnetic resonance imaging using spin-polarized 129Xe.
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.