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Chemical Physics Letters

Optical pumping magnetic resonance in high magnetic fields: Measurement of high field spin exchange cross sections

Matthew P. Augustine, Kurt W. Zilm

Published Nov 1, 1997• 18 citations
Publisher

Abstract

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.

DOI
10.1016/s0009-2614(97)01076-2

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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.

Physical Review Letters•Feb 9, 2006•203 citations
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.
The production of hyperpolarized Xe via spin exchange with optically pumped Rb atoms was studied at 47 000 G under high-pressure conditions. From variable pressure and temperature studies, the spin exchange efficiency was found to be pressure dependent and lower than comparable low-field measurements. Spin exchange due to short binary collisions is expected to be pressure independent, and the cross section was measured to be 〈σν〉SE=6.0 (±0.1)×10−17 cm3 s−1. The pressure dependent component was attributed to the formation of Rb–Xe van der Waals (vdW) complexes. The rate constant for spin exchange in Rb–Xe vdW complexes was measured to be κ=1400 (±100) s−1 in He buffer gas. This value is comparable, though somewhat smaller than vdW rates measured previously for other buffer gases. While it is well known that spin exchange occurs readily in vdW complexes when B0<200 G, vdW spin exchange at fields >10 000 G is not accounted for in current theories. Modulation of the hyperfine interaction during the vdW complex lifetime is proposed to account for these observations. Finally, relaxation by the walls of the pumping cell was found to increase with buffer gas pressure. These factors impact the equilibrium Xe polarization obtainable with high-field optical pumping.
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.
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.
We present a design for a spin-exchange optical pumping system to produce large quantities of highly polarized 129Xe and 131Xe. Low xenon concentrations in the flowing gas mixture which allow the laser to maintain high Cs polarization. The large spin-exchange rate between Cs and Xe 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. The fast rates make it possible to obtain large nuclear polarizations after several minutes of optical pumping with a laser.At high Xe pressures. According to the theory, the longitudinal spin-elaxation rate 1T1 of Xe in a high-pressure sample containing only Xe and Cs vapor has the simple form is the velocity averaged binary spin-exchange cross section, It is the relaxation rate due to wall collisions and perhaps magnetic field inhomogeneities. Our results complement earlier studies performed at 129Xe pressures of about 20 Torr and 131Xe pressures of about 20 Torr and N2 pressures of 600 Torr . This work is useful for predicting spin-exchange rates between polarized Cs atoms and Xe nuclei.
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.