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Journal of Physics D Applied Physics

Comparative spin-exchange efficiency of Rb– 129 Xe and Cs– 129 Xe in the long-lived van der Waals regime: implications for high-throughput 129 Xe hyperpolarization

Tao shi, Ge Jin, Liu Bowen, Yuxin Chen, Yongjun Zhou, Junjian Tang, Sheng Zou

Published Jun 23, 2026• 0 citations
Publisher

Abstract

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.

DOI
10.1088/1361-6463/ae80db

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Oct 8, 2015•0 citations
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.
Abstract The relative spin-exchange efficiencies of Cs and Rb remain an important question in the field of hyperpolarized 129 Xe; however, direct experimental comparisons are still limited. We present measurements of the spin-exchange efficiency for 129 Xe–Cs/Rb in 129 Xe: N 2 = 1 : 50 mixtures. Under low-magnetic-field and short-lifetimes van der Waals molecular regime, we determine the spin-exchange efficiencies of 129 Xe–Cs/Rb by measuring the spin-exchange rate coefficient for 129 Xe–Cs/Rb and the Xe-induced spin-relaxation rate of Cs/Rb. Under identical gas composition and pressure conditions, the spin-exchange efficiency of Cs is approximately 1.2–1.5 times higher than Rb. We also derive an expression that enables the prediction of the spin-exchange efficiency for 129 Xe–Cs/Rb in arbitrary 129 Xe– N 2 mixtures.
Spin-exchange optical pumping (SEOP) enables hyperpolarization of magnetic noble gas nuclei and allows enormously enhanced signal in nuclear magnetic resonance studies in materials, biosciences, and medicine. We model the dynamics of the SEOP process taking place in a $\mathrm{Rb}\ensuremath{-}^{129}\mathrm{Xe}$ gas mixture and shed light on how the different microscopic processes influence the macroscopic polarization transfer. For each Rb-Xe collision taking place in simulated molecular dynamics trajectory, we sample a time series of quantum-chemically preparametrized Hamiltonians. Combined electron and nuclear spin dynamics of each event is propagated by solving the corresponding Liouville--von Neumann equation. The rarely occurring, long-lived van der Waals molecules are seen to give the most significant contribution to polarization transfer under the simulated conditions (T=300T=300T=300 K, p=2.4p=2.4p=2.4 bar), in agreement with earlier findings. Besides the lifetime of the collision complex, the average and minimum Rb-Xe interatomic distances characterize the efficiency of the polarization transfer events. We obtain insight into magnetization transfer in both individual binary collisions and van der Waals complexes and demonstrate a stepwise buildup of 129Xe^{129}\mathrm{Xe}129Xe spin polarization upon bond-length oscillations in the latter.
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.
We experimentally study the Rb-Xe spin-exchange optical pumping process. The dependence of the spin-exchange rate on the intensity of the pumping light is measured at different temperatures under low magnetic fields. We demonstrate that the spin-exchange rate will decrease as the Rb spin polarization increases, which agrees well with the theoretical prediction. In our measurement, three spin exchange and spin relaxation mechanisms, namely, the spin exchange rates between Rb and Xe atoms caused by van der Waals molecule (${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{vdW}}$) and binary collision (${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{bin}}$) processes, and the spin relaxation rate due to the wall collision of Xe atoms (${\mathrm{\ensuremath{\Gamma}}}_{\mathrm{w}}$), have comparable magnitudes. These rates are extracted separately from the measured data with different Rb spin polarization at various temperatures. Our work provides a comprehensive confirmation of the physical picture of the spin-exchange optical pumping process.
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.
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.