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Spin-exchange optical pumping with alkali-metal vapors

Earl Babcock

Published Jan 1, 2005• 21 citations
OpenAlex

Abstract

While the method of Spin-exchange optical pumping, SEOP, of noble gases has existed since 1960 [Bouchiat60], many fundamental aspects of spin exchange optical pumping have gone largely unexplained. These questions included the values of the rate coefficients for spin-exchange, many aspects of the alkali-metal polarization and density inside the SEOP cells, the mechanisms of He wall relaxation, non-ideal values of the observed He polarization, and efficiency to produce it. This thesis describes the results of our efforts to quantity all parameters in SEOP and to begin to determine some of these unknowns. This thesis presents measurements of spin-exchange rate coefficients and efficiencies. A method to extend SEOP to multiple alkali species is presented. In addition, limits to the efficiency of optical pumping, the efficiency of spin-exchange, and the observed He polarization are explored.

Related papers

Analytical model for polarization transfer during gas-phase collision events in spin-exchange optical pumping: Spin-$\frac{1}{2}$ $^{129}$Xe versus spin-$\frac{3}{2}$ $^{131}$Xe

Perttu Hilla, Rajgowrav Cheenikundil, Juha Vaara

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 $I = 1/2$ nuclei, such as 129Xe, is relatively well understood, that of spin $I > 1/2$ nuclei, such as 131Xe ($I = 3/2$), 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 $\hatρ(t)$ 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 $\hatρ(t)$ 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.

physics.atom-phCross-listedarXiv:2609.04743•Sep 7, 2026•0 citations

Spin-exchange optical pumping of He3 with Rb-K mixtures and pure K

Wangchun Chen, T. Gentile, Thad G Walker +1 more

We have studied the efficiency of spin-exchange optical pumping (SEOP) in cells that contain either pure rubidium, mixtures of rubidium and potassium, or pure potassium. Optical pumping was performed with spectrally narrowed diode array lasers operating at either the wavelength of the Rb $5{s}_{1∕2}\ensuremath{-}5{p}_{1∕2}$ transition $(795\phantom{\rule{0.3em}{0ex}}\mathrm{nm})$ or the K $4{s}_{1∕2}\ensuremath{-}4{p}_{1∕2}$ transition $(770\phantom{\rule{0.3em}{0ex}}\mathrm{nm})$. Calculations of the expected efficiency are shown for practical conditions and compared to measurements. We have measured the vapor density ratio in Rb-K mixture cells using absorption of white light. Our focus is on the conditions that are relevant for neutron spin filters, but the results are relevant to all applications of SEOP. We find that both Rb-K and pure K cells yield improvements in the spin-exchange efficiency, and each approach has its own advantages. Overall, the best results for high polarizing rate with high polarization were obtained with mixture cells with K-Rb vapor density ratios between 2 and 6.

Physical Review A•Jan 23, 2007•107 citations

Spin-exchange optical pumping of noble-gas nuclei

Thad G Walker, W. Happer

Spin-exchange optical pumping of mixtures of alkali-metal vapors and noble gases can be used to efficiently polarize the nuclei of the noble-gas atoms. Liters of noble gases at standard temperature and pressure and with nuclear spin polarizations of several tens of percent are now used in many applications. The authors describe the basic phenomena that govern the spin-exchange process and review the physics of angular momentum transfer and loss in optical pumping and spin-exchange collisions.

Reviews of Modern Physics•Apr 1, 1997•1,447 citations

Polarization of the nuclear spins of noble-gas atoms by spin exchange with optically pumped alkali-metal atoms

W. Happer, E. Miron, S. Schaefer +3 more

The theory of spin exchange between optically pumped alkali-metal atoms and noble-gas nuclei is presented. Spin exchange with heavy noble gases is dominated by interactions in long-lived van der Waals molecules. The main spin interactions are assumed to be the spin-rotation interactions $\ensuremath{\gamma}\stackrel{\ensuremath{\rightarrow}}{\mathrm{N}}\ifmmode\cdot\else\textperiodcentered\fi{}\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$ between the rotational angular momentum $\stackrel{\ensuremath{\rightarrow}}{\mathrm{N}}$ of the alkali-metal---noble-gas pair and the electron spin $\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$ of the alkali-metal atom, and the contact hyperfine interaction $\ensuremath{\alpha}\stackrel{\ensuremath{\rightarrow}}{\mathrm{K}}\ifmmode\cdot\else\textperiodcentered\fi{}\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$ between the nuclear spin $\stackrel{\ensuremath{\rightarrow}}{\mathrm{K}}$ of the noble-gas atom and the electron spin $\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$. Arbitrary values for $K$ and for the nuclear spin $I$ of the alkali-metal atom are assumed. Precise formal expressions for spin transfer coefficients are given along with convenient approximations based on a perturbation expansion in powers of ${(\frac{\ensuremath{\alpha}}{\ensuremath{\gamma}N})}^{2}$, a quantity which has been shown to be small by experiment.

Physical Review A•Jun 1, 1984•468 citations

Theory of spin-exchange optical pumping of 3 He and 129 Xe

Stephan Appelt, Andrei Ben-Amar Baranga, Christopher Erickson +3 more

We present a comprehensive theory of nuclear spin polarization of ${}^{3}\mathrm{He}$ and ${}^{129}\mathrm{Xe}$ 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 ${}^{3}\mathrm{He}$ or ${}^{129}\mathrm{Xe}$ 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 ${}^{3}\mathrm{He}$ or ${}^{129}\mathrm{Xe}$ gas are assumed, namely, atmospheres of gas pressure and nearly complete quenching of the optically excited alkali-metal atoms by collisions with ${\mathrm{N}}_{2}$ or ${\mathrm{H}}_{2}$ 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.

Physical Review A•Aug 1, 1998•443 citations

Fundamentals of Spin-Exchange Optical Pumping

Thad G Walker

The standard model of Spin-Exchange Optical Pumping of 3 He has come under close scrutiny as researchers try to maximize the quantity and polarization of 3 He. This paper will review four important effects that have come to light: 1) pumping with frequency narrowed diode lasers significantly improves the polarization and production rate as compared to off-the-shelf broadband sources 2) Rb-K mixtures again improve the production rate due to reduced collisional loss in K-He collisions, 3) a unexplained 3 He wall relaxation mechanism that scales closely with alkali vapor pressure limits the attainable 3 He polarization to about 80%, 4) a small collisionally-induced breakdown in the selection rules for optical pumping explains why narrowband lasers are so advantageous, and may explain some observed limitations for Rb-K pumping as well.

Journal of Physics Conference Series•Jun 1, 2011•67 citations
While the method of Spin-exchange optical pumping, SEOP, of noble gases has existed since 1960 [Bouchiat60], many fundamental aspects of spin exchange optical pumping have gone largely unexplained. These questions included the values of the rate coefficients for spin-exchange, many aspects of the alkali-metal polarization and density inside the SEOP cells, the mechanisms of He wall relaxation, non-ideal values of the observed He polarization, and efficiency to produce it. This thesis describes the results of our efforts to quantity all parameters in SEOP and to begin to determine some of these unknowns. This thesis presents measurements of spin-exchange rate coefficients and efficiencies. A method to extend SEOP to multiple alkali species is presented. In addition, limits to the efficiency of optical pumping, the efficiency of spin-exchange, and the observed He polarization are explored.
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.
We have studied the efficiency of spin-exchange optical pumping (SEOP) in cells that contain either pure rubidium, mixtures of rubidium and potassium, or pure potassium. Optical pumping was performed with spectrally narrowed diode array lasers operating at either the wavelength of the Rb $5{s}_{1∕2}\ensuremath{-}5{p}_{1∕2}$ transition (795nm)(795\phantom{\rule{0.3em}{0ex}}\mathrm{nm})(795nm) or the K $4{s}_{1∕2}\ensuremath{-}4{p}_{1∕2}$ transition (770nm)(770\phantom{\rule{0.3em}{0ex}}\mathrm{nm})(770nm). Calculations of the expected efficiency are shown for practical conditions and compared to measurements. We have measured the vapor density ratio in Rb-K mixture cells using absorption of white light. Our focus is on the conditions that are relevant for neutron spin filters, but the results are relevant to all applications of SEOP. We find that both Rb-K and pure K cells yield improvements in the spin-exchange efficiency, and each approach has its own advantages. Overall, the best results for high polarizing rate with high polarization were obtained with mixture cells with K-Rb vapor density ratios between 2 and 6.
The theory of spin exchange between optically pumped alkali-metal atoms and noble-gas nuclei is presented. Spin exchange with heavy noble gases is dominated by interactions in long-lived van der Waals molecules. The main spin interactions are assumed to be the spin-rotation interactions $\ensuremath{\gamma}\stackrel{\ensuremath{\rightarrow}}{\mathrm{N}}\ifmmode\cdot\else\textperiodcentered\fi{}\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$ between the rotational angular momentum $\stackrel{\ensuremath{\rightarrow}}{\mathrm{N}}$ of the alkali-metal---noble-gas pair and the electron spin $\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$ of the alkali-metal atom, and the contact hyperfine interaction $\ensuremath{\alpha}\stackrel{\ensuremath{\rightarrow}}{\mathrm{K}}\ifmmode\cdot\else\textperiodcentered\fi{}\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$ between the nuclear spin $\stackrel{\ensuremath{\rightarrow}}{\mathrm{K}}$ of the noble-gas atom and the electron spin $\stackrel{\ensuremath{\rightarrow}}{\mathrm{S}}$. Arbitrary values for KKK and for the nuclear spin III of the alkali-metal atom are assumed. Precise formal expressions for spin transfer coefficients are given along with convenient approximations based on a perturbation expansion in powers of ${(\frac{\ensuremath{\alpha}}{\ensuremath{\gamma}N})}^{2}$, a quantity which has been shown to be small by experiment.
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.
The standard model of Spin-Exchange Optical Pumping of 3 He has come under close scrutiny as researchers try to maximize the quantity and polarization of 3 He. This paper will review four important effects that have come to light: 1) pumping with frequency narrowed diode lasers significantly improves the polarization and production rate as compared to off-the-shelf broadband sources 2) Rb-K mixtures again improve the production rate due to reduced collisional loss in K-He collisions, 3) a unexplained 3 He wall relaxation mechanism that scales closely with alkali vapor pressure limits the attainable 3 He polarization to about 80%, 4) a small collisionally-induced breakdown in the selection rules for optical pumping explains why narrowband lasers are so advantageous, and may explain some observed limitations for Rb-K pumping as well.