Characterizing and modeling the efficiency limits in large-scale production of hyperpolarized Xe129
Year: 2014
Type: article
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.
Source: Physical Review A
Authors: M. S. Freeman, K. Emami, B. Driehuys
Institutions: Duke University, Duke Medical Center
Language: Latvian
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W2059700219