Spin-exchange Optical Pumping Research Articles

Development of a compact in situ polarized ³He neutron spin filter at Oak Ridge National Laboratory.

We constructed a compact in situ polarized (3)He neutron spin filter based on spin-exchange optical pumping which is capable of continuous pumping of the (3)He gas while the system is in place in the neutron beam on an instrument. The compact size and light weight of the system simplifies its utilization on various neutron instruments. The system has been successfully tested as a neutron polarizer on the triple-axis spectrometer (HB3) and the hybrid spectrometer (HYSPEC) at Oak Ridge National Laboratory. Over 70% (3)He polarization was achieved and maintained during the test experiments. Over 90% neutron polarization and an average of 25% transmission for neutrons of 14.7 meV and 15 meV was also obtained.

Multidimensional mapping of spin-exchange optical pumping in clinical-scale batch-mode 129Xe hyperpolarizers.

We present a systematic, multiparameter study of Rb/129Xe spin-exchange optical pumping (SEOP) in the regimes of high xenon pressure and photon flux using a 3D-printed, clinical-scale stopped-flow hyperpolarizer. In situ NMR detection was used to study the dynamics of 129Xe polarization as a function of SEOP-cell operating temperature, photon flux, and xenon partial pressure to maximize 129Xe polarization (PXe). PXe values of 95 ± 9%, 73 ± 4%, 60 ± 2%, 41 ± 1%, and 31 ± 1% at 275, 515, 1000, 1500, and 2000 Torr Xe partial pressure were achieved. These PXe polarization values were separately validated by ejecting the hyperpolarized 129Xe gas and performing low-field MRI at 47.5 mT. It is shown that PXe in this high-pressure regime can be increased beyond already record levels with higher photon flux and better SEOP thermal management, as well as optimization of the polarization dynamics, pointing the way to further improvements in hyperpolarized 129Xe production efficiency.

Observing and preventing rubidium runaway in a direct-infusion xenon-spin hyperpolarizer optimized for high-resolution hyper-CEST (chemical exchange saturation transfer using hyperpolarized nuclei) NMR

Xenon is well known to undergo host-guest interactions with proteins and synthetic molecules. As xenon can also be hyperpolarized by spin exchange optical pumping, allowing the investigation of highly dilute systems, it makes an ideal nuclear magnetic resonance probe for such host molecules. The utility of xenon as a probe can be further improved using Chemical Exchange Saturation Transfer using hyperpolarized nuclei (Hyper-CEST), but for highly accurate experiments requires a polarizer and xenon infusion system optimized for such measurements. We present the design of a hyperpolarizer and xenon infusion system specifically designed to meet the requirements of Hyper-CEST measurements. One key element of this design is preventing rubidium runaway, a chain reaction induced by laser heating that prevents efficient utilization of high photon densities. Using thermocouples positioned along the pumping cell we identify the sources of heating and conditions for rubidium runaway to occur. We then demonstrate the effectiveness of actively cooling the optical cell to prevent rubidium runaway in a compact setup. This results in a 2-3-fold higher polarization than without cooling, allowing us to achieve a polarization of 25% at continuous flow rates of 9 ml/min of (129)Xe. The simplicity of this design also allows it to be retrofitted to many existing polarizers. Combined with a direction infusion system that reduces shot-to-shot noise down to 0.56% we have captured Hyper-CEST spectra in unprecedented detail, allowing us to completely resolve peaks separated by just 1.62 ppm. Due to its high polarization and excellent stability, our design allows the comparison of underlying theories of host-guest systems with experiment at low concentrations, something extremely difficult with previous polarizers.

Spin-dependent cross sections from the three-body photodisintegration ofHe3at incident energies of 12.8 and 14.7 MeV

The first measurement of the three-body photodisintegration of polarized $^{3}\mathrm{He}$ using a circularly polarized photon beam has been performed at incident energies of 12.8 and 14.7 MeV. This measurement was carried out at the high-intensity $\ensuremath{\gamma}$-ray source located at Triangle Universities Nuclear Laboratory. A high-pressure $^{3}\mathrm{He}$ target, polarized via spin exchange optical pumping with alkali metals, was used in the experiment. The spin-dependent double- and single-differential cross sections from $\stackrel{P\vec}{{}^{3}\text{He}}(\stackrel{P\vec}{\ensuremath{\gamma}},n)pp$ for laboratory angles varying from ${30}^{\ensuremath{\circ}}$ to ${165}^{\ensuremath{\circ}}$ are presented and compared with state-of-the-art three-body calculations. The data reveal the importance of including the Coulomb interaction between protons in the three-body calculations.

XeNA: An automated ‘open-source’ 129Xe hyperpolarizer for clinical use

Here we provide a full report on the construction, components, and capabilities of our consortium’s “open-source” large-scale (~1L/h) 129Xe hyperpolarizer for clinical, pre-clinical, and materials NMR/MRI (Nikolaou et al., Proc. Natl. Acad. Sci. USA, 110, 14150 (2013)). The ‘hyperpolarizer’ is automated and built mostly of off-the-shelf components; moreover, it is designed to be cost-effective and installed in both research laboratories and clinical settings with materials costing less than $125,000. The device runs in the xenon-rich regime (up to 1800Torr Xe in 0.5L) in either stopped-flow or single-batch mode—making cryo-collection of the hyperpolarized gas unnecessary for many applications. In-cell 129Xe nuclear spin polarization values of ~30%–90% have been measured for Xe loadings of ~300–1600Torr. Typical 129Xe polarization build-up and T1 relaxation time constants were ~8.5min and ~1.9h respectively under our spin-exchange optical pumping conditions; such ratios, combined with near-unity Rb electron spin polarizations enabled by the high resonant laser power (up to ~200W), permit such high PXe values to be achieved despite the high in-cell Xe densities. Importantly, most of the polarization is maintained during efficient HP gas transfer to other containers, and ultra-long 129Xe relaxation times (up to nearly 6h) were observed in Tedlar bags following transport to a clinical 3T scanner for MR spectroscopy and imaging as a prelude to in vivo experiments. The device has received FDA IND approval for a clinical study of chronic obstructive pulmonary disease subjects. The primary focus of this paper is on the technical/engineering development of the polarizer, with the explicit goals of facilitating the adaptation of design features and operative modes into other laboratories, and of spurring the further advancement of HP-gas MR applications in biomedicine.

A 3D-Printed High Power Nuclear Spin Polarizer

Three-dimensional printing with high-temperature plastic is used to enable spin exchange optical pumping (SEOP) and hyperpolarization of xenon-129 gas. The use of 3D printed structures increases the simplicity of integration of the following key components with a variable temperature SEOP probe: (i) in situ NMR circuit operating at 84 kHz (Larmor frequencies of (129)Xe and (1)H nuclear spins), (ii) <0.3 nm narrowed 200 W laser source, (iii) in situ high-resolution near-IR spectroscopy, (iv) thermoelectric temperature control, (v) retroreflection optics, and (vi) optomechanical alignment system. The rapid prototyping endowed by 3D printing dramatically reduces production time and expenses while allowing reproducibility and integration of "off-the-shelf" components and enables the concept of printing on demand. The utility of this SEOP setup is demonstrated here to obtain near-unity (129)Xe polarization values in a 0.5 L optical pumping cell, including ∼74 ± 7% at 1000 Torr xenon partial pressure, a record value at such high Xe density. Values for the (129)Xe polarization exponential build-up rate [(3.63 ± 0.15) × 10(-2) min(-1)] and in-cell (129)Xe spin-lattice relaxation time (T1 = 2.19 ± 0.06 h) for 1000 Torr Xe were in excellent agreement with the ratio of the gas-phase polarizations for (129)Xe and Rb (PRb ∼ 96%). Hyperpolarization-enhanced (129)Xe gas imaging was demonstrated with a spherical phantom following automated gas transfer from the polarizer. Taken together, these results support the development of a wide range of chemical, biochemical, material science, and biomedical applications.

Pulmonary MRI contrast using Surface Quadrupolar Relaxation (SQUARE) of hyperpolarized 83Kr

Hyperpolarized 83Kr has previously been demonstrated to enable MRI contrast that is sensitive to the chemical composition of the surface in a porous model system. Methodological advances have lead to a substantial increase in the 83Kr hyperpolarization and the resulting signal intensity. Using the improved methodology for spin exchange optical pumping of isotopically enriched 83Kr, internal anatomical details of ex vivo rodent lung were resolved with hyperpolarized 83Kr MRI after krypton inhalation. Different 83Kr relaxation times were found between the main bronchi and the parenchymal regions in ex vivo rat lungs. The T1 weighted hyperpolarized 83Kr MRI provided a first demonstration of surface quadrupolar relaxation (SQUARE) pulmonary MRI contrast.

Cryogenics free production of hyperpolarized 129Xe and 83Kr for biomedical MRI applications

As an alternative to cryogenic gas handling, hyperpolarized (hp) gas mixtures were extracted directly from the spin exchange optical pumping (SEOP) process through expansion followed by compression to ambient pressure for biomedical MRI applications. The omission of cryogenic gas separation generally requires the usage of high xenon or krypton concentrations at low SEOP gas pressures to generate hp 129Xe or hp 83Kr with sufficient MR signal intensity for imaging applications. Two different extraction schemes for the hp gasses were explored with focus on the preservation of the nuclear spin polarization. It was found that an extraction scheme based on an inflatable, pressure controlled balloon is sufficient for hp 129Xe handling, while 83Kr can efficiently be extracted through a single cycle piston pump. The extraction methods were tested for ex vivo MRI applications with excised rat lungs. Precise mixing of the hp gases with oxygen, which may be of interest for potential in vivo applications, was accomplished during the extraction process using a piston pump. The 83Kr bulk gas phase T1 relaxation in the mixtures containing more than approximately 1% O2 was found to be slower than that of 129Xe in corresponding mixtures. The experimental setup also facilitated 129Xe T1 relaxation measurements as a function of O2 concentration within excised lungs.

Comparative study of in situ N2 rotational Raman spectroscopy methods for probing energy thermalisation processes during spin-exchange optical pumping

Spin-exchange optical pumping (SEOP) has been widely used to produce enhancements in nuclear spin polarisation for hyperpolarised noble gases. However, some key fundamental physical processes underlying SEOP remain poorly understood, particularly in regards to how pump laser energy absorbed during SEOP is thermalised, distributed and dissipated. This study uses in situ ultra-low frequency Raman spectroscopy to probe rotational temperatures of nitrogen buffer gas during optical pumping under conditions of high resonant laser flux and binary Xe/N2 gas mixtures. We compare two methods of collecting the Raman scattering signal from the SEOP cell: a conventional orthogonal arrangement combining intrinsic spatial filtering with the utilisation of the internal baffles of the Raman spectrometer, eliminating probe laser light and Rayleigh scattering, versus a new in-line modular design that uses ultra-narrowband notch filters to remove such unwanted contributions. We report a ~23-fold improvement in detection sensitivity using the in-line module, which leads to faster data acquisition and more accurate real-time monitoring of energy transport processes during optical pumping. The utility of this approach is demonstrated via measurements of the local internal gas temperature (which can greatly exceed the externally measured temperature) as a function of incident laser power and position within the cell.

Comment on “Enhanced polarization and mechanisms in optically pumped hyperpolarized3Hein the presence of4He”

Chen et al. [Phys. Rev. A 81, 033422 (2010)] claim that adding ${}^{4}\mathrm{He}$ to spin-exchange optical pumping (SEOP) cells confines ${}^{3}\mathrm{He}$ atoms to a diffusion-limited region, which effectively reduces the wall relaxation factor $X$. Here $X$ is a phenomenological parameter used to characterize typical SEOP cells; it quantifies the observation that the measured linear slope of the relaxation rate with alkali-metal-atom density exceeds the spin-exchange rate. In addition they claim to demonstrate that magnetic-field gradients cause a diffusive motion of ${}^{3}\mathrm{He}$. We argue that these claims and other central conclusions drawn by Chen et al. [Phys. Rev. A 81, 033422 (2010)] are inconsistent with the physics of diffusion or should not be made from the data as presented. We also draw attention to several additional issues associated with the results, analysis, and presentation of data in Chen et al. [Phys. Rev. A 81, 033422 (2010)] that confound clear interpretation.

Spin exchange optical pumping based polarized 3He filling station for the Hybrid Spectrometer at the Spallation Neutron Source

The Hybrid Spectrometer (HYSPEC) is a new direct geometry spectrometer at the Spallation Neutron Source at the Oak Ridge National Laboratory. This instrument is equipped with polarization analysis capability with 60° horizontal and 15° vertical detector coverages. In order to provide wide angle polarization analysis for this instrument, we have designed and built a novel polarized (3)He filling station based on the spin exchange optical pumping method. It is designed to supply polarized (3)He gas to HYSPEC as a neutron polarization analyzer. In addition, the station can optimize the (3)He pressure with respect to the scattered neutron energies. The depolarized (3)He gas in the analyzer can be transferred back to the station to be repolarized. We have constructed the prototype filling station. Preliminary tests have been carried out demonstrating the feasibility of the filling station. Here, we report on the design, construction, and the preliminary results of the prototype filling station.

Polarized 129Xe Production by Using the Spin Exchange Optical Pumping Method

Polarized 129Xe Production by Using the Spin Exchange Optical Pumping Method

A compact spin-exchange optical pumping system for 3He polarization based on a solenoid coil, a VBG laser diode, and a cosine theta RF coil

For use as a neutron spin polarizer or analyzer in the neutron beam lines of the HANARO (High-flux Advanced Neutron Application ReactOr) nuclear research reactor, a 3He polarizer was designed based on both a compact solenoid coil and a VBG (volume Bragg grating) diode laser with a narrow spectral linewidth of 25 GHz. The nuclear magnetic resonance (NMR) signal was measured and analyzed using both a built-in cosine radio-frequency (RF) coil and a pick-up coil. Using a neutron transmission measurement, we estimated the polarization ratio of the 3He cell as 18% for an optical pumping time of 8 hours.

Optimized production of hyperpolarized 129Xe at 2 bars for in vivo lung magnetic resonance imaging

In this work, the production rate of a spin-exchange optical pumping 129Xe gas polarizer was optimized for routine generation of hyperpolarized 129Xe for in vivo lung MRI. This system uses a narrow (∼ 0.1 nm linewidth), tuneable external cavity laser (operating at ∼25 W) for SEOP of 3% gas mixtures of Xe inside a mid-pressure (2 bars) cell of 491 cm3 volume. Under this regime, theoretical and experimentally measured 129Xe polarizations were calculated to be 24% and 12%, respectively, for a gas flow rate of 300 sccm and a cell temperature of 373 K. The photon efficiency was evaluated, yielding theoretical and experimental values of 0.039 and 0.046, respectively. The theoretical efficiency was calculated from spin-exchange and spin-destruction cross sections and the experimental photon efficiency was measured under flow for a gas-cell residency time equal to an empirically determined spin-exchange time of 45 s. In addition, details of the Xe freeze-out process were analyzed with a model of polarization decay during Xe accumulation in the frozen phase, where a T1 of 87 ± 2 min was observed. To demonstrate the system's application, in vivo lung magnetic resonance images (signal-to-noise ratio ∼ 50 from a voxel of 15 mm× 4 mm× 4 mm) were acquired using modest volumes (&amp;lt;400 ml) of isotopically enriched (86% 129Xe) Xe gas polarized to &amp;gt;10%. Despite the experimental polarization being a factor of 2 lower than the predicted polarization for typical operating parameters, the system is close to the theoretical photon efficiency and the system has so far produced polarized gas for more than 100 in vivo 129Xe lung imaging studies.

Polarized 3He Neutron Spin Filters at Oak Ridge National Laboratory

Abstract The unique advantages of using polarized 3 He as neutron spin filters, such as broadband and wide angular acceptance of neutron beams, have made it widely used in most neutron facilities. Over the last several years, we have developed a polarized 3 He program to meet the increasing needs of 3 He based neutron spin filters at the Oak Ridge National Laboratory's (ORNL) High Flux Isotope Reactor (HFIR) and Spallation Neutron Source (SNS). At ORNL, polarized 3 He is produced using Spin Exchange Optical Pumping (SEOP). We have constructed a 3He cell fabrication station to produce 3 He cells of different pressures and dimensions. Two optical pumping stations have been built in the lab to perform ex situ pumping of 3 He. A compact in situ 3 He analyzer has been constructed and installed for the Magnetism Reflectometer (MAGICS) at SNS. A novel polarized 3 He filling station for the Hybrid Spectrometer (HYSPEC) at SNS is under development.

High-volume 100 Liter-per-day SEOP Polarization of 3He

Abstract We describe a novel apparatus for large-scale production of polarized 3He using Spin-Exchange Optical Pumping (SEOP). The large optical pumping cell is enclosed inside a pressure containment vessel to equalize the differential pressure across the glass cell walls. Numerical simulations of laser absorption and spin-transfer guided our choice of pressure, temperature, and laser power. Computational fluid dynamics simulations of the two-zone thermal bath environment revealed buoyancy-induced flow which favored operation inclined at an angle. We prepared and tested three separate 8.5 liter cells at internal pressures up to six amagat (50 bar-liters) with hybrid alkali ratios of K:Rb of 10:1 by mass (4.4:1 by number ratio) and at temperatures up to 250°C. An early prototype used a 1.4 kW broadband laser, while our most recent prototype incorporated a new 2.2kW spectrally narrowed external cavity laser. Using small surface coil NMR to measure polarization, we obtained spin-up rates greater than 20% per hour consistent with our numerical simulations. Unfortunately, each cell installation to date has been compromised, limiting T1 relaxation times to 12 hours and asymptotic polarizations to values below 50%. If a cell could be installed with 50 hour lifetime and X-factor of 0.2, this polarizer will deliver 50 liters of over 70% polarized 3He twice each day.

Combustion resistance of the129Xe hyperpolarized nuclear spin state

Using a methane-xenon mixture for spin exchange optical pumping, MRI of combustion was enabled. The (129)Xe hyperpolarized nuclear spin state was found to sufficiently survive the complete passage through the harsh environment of the reaction zone. A velocity profile (V(z)(z)) of a flame was recorded to demonstrate the feasibility of MRI velocimetry of transport processes in combustors.

Basic Concepts of Polarisation Analysis for Neutron Chopper Spectrometer POLANO at J-PARC

The basic concept underlying the use of neutron polarisers and analysers in a polarised neutron spectrometer which will be constructed in J-PARC/MLF is discussed. The spectrometer, named POLANO, is a compact chopper spectrometer for polarisation analysis in the energy region up to Ei ~200 meV. In the first stage of this project, a 3He spin filter polarised by the spin exchange optical pumping method will be used as the polariser. Based on the optimisations of the filter parameters, we confirm that the designed optimised 3He spin filters will be feasible for use up to 80 meV.

Pathway to Cryogen Free Production of Hyperpolarized Krypton-83 and Xenon-129

Hyperpolarized (hp) 129Xe and hp 83Kr for magnetic resonance imaging (MRI) are typically obtained through spin-exchange optical pumping (SEOP) in gas mixtures with dilute concentrations of the respective noble gas. The usage of dilute noble gases mixtures requires cryogenic gas separation after SEOP, a step that makes clinical and preclinical applications of hp 129Xe MRI cumbersome. For hp 83Kr MRI, cryogenic concentration is not practical due to depolarization that is caused by quadrupolar relaxation in the condensed phase. In this work, the concept of stopped flow SEOP with concentrated noble gas mixtures at low pressures was explored using a laser with 23.3 W of output power and 0.25 nm linewidth. For 129Xe SEOP without cryogenic separation, the highest obtained MR signal intensity from the hp xenon-nitrogen gas mixture was equivalent to that arising from 15.5±1.9% spin polarized 129Xe in pure xenon gas. The production rate of the hp gas mixture, measured at 298 K, was 1.8 cm3/min. For hp 83Kr, the equivalent of 4.4±0.5% spin polarization in pure krypton at a production rate of 2 cm3/min was produced. The general dependency of spin polarization upon gas pressure obtained in stopped flow SEOP is reported for various noble gas concentrations. Aspects of SEOP specific to the two noble gas isotopes are discussed and compared with current theoretical opinions. A non-linear pressure broadening of the Rb D1 transition was observed and taken into account for the qualitative description of the SEOP process.

Configuration and Performance of a Mobile 129Xe Polarizer

A stand-alone, self-contained and transportable system for the polarization of 129Xe by spin exchange optical pumping with Rb is described. This mobile polarizer may be operated in batch or continuous flow modes with medium amounts of hyperpolarized 129Xe for spectroscopic or small animal applications. A key element is an online nuclear magnetic resonance module which facilitates continuous monitoring of polarization generation in the pumping cell as well as the calculation of the absolute 129Xe polarization. The performance of the polarizer with respect to the crucial parameters temperature, xenon and nitrogen partial pressures, and the total gas flow is discussed. In batch mode the highest 129Xe polarization of PXe = 40 % was achieved using 0.1 mbar xenon partial pressure. For a xenon flow of 6.5 and 26 mln/min, P Xe = 25 % and P Xe = 13 % were reached, respectively. The mobile polarizer may be a practical and efficient means to make the applicability of hyperpolarized 129Xe more widespread.