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Low-field NMR has emerged as a new analytical technique for the investigation of molecular structure and dynamics. Here, we introduce a highly integrated ultralow-frequency NMR spectrometer designed for the purpose of ultralow-field NMR polarimetry of hyperpolarized contrast media. The device measures 10 cm × 10 cm × 2.0 cm and weighs only 370 g. The spectrometer's aluminum enclosure contains all components, including an RF amplifier. The device has four ports for connecting to a high-impedance RF transmit-receive coil, a trigger input, a USB port for connectivity to a PC computer, and an auxiliary RS-485/24VDC port for system integration with other devices. The NMR spectrometer is configured for a pulse-wait-acquire-recover pulse sequence, and key sequence parameters are readily controlled by a graphical user interface (GUI) of a Windows-based PC computer. The GUI also displays the time-domain and Fourier-transformed NMR signal and allows autosaving of NMR data as a CSV file. Alternatively, the RS485 communication line allows for operating the device with sequence parameter control and data processing directly on the spectrometer board in a fully automated and integrated manner. The NMR spectrometer, equipped with a 250 ksamples/s 17-bit analog-to-digital signal converter, can perform acquisition in the 1-125 kHz frequency range. The utility of the device is demonstrated for NMR polarimetry of hyperpolarized 129Xe gas and [1-13C]pyruvate contrast media (which was compared to the 13C polarimetry using a more established technology of benchtop 13C NMR spectroscopy, and yielded similar results), allowing reproducible quantification of polarization values and relaxation dynamics. The cost of the device components is only â¼$200, offering a low-cost integrated NMR spectrometer that can be deployed as a plug-and-play device for a wide range of applications in hyperpolarized contrast media productionâand beyond.
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We present a pilot quality assurance (QA) study of a clinical-scale, automated, third-generation (GEN-3) 129Xe hyperpolarizer employing batch-mode spin-exchange optical pumping (SEOP) with high-Xe densities (50% natural abundance Xe and 50% N2 in ~2.6 atm total pressure sourced from Nova Gas Technologies) and rapid temperature ramping enabled by an aluminum heating jacket surrounding the 0.5 L SEOP cell. 129Xe hyperpolarization was performed over the course of 700 gas loading cycles of the SEOP cell, simulating long-term hyperpolarized contrast agent production in a clinical lung imaging setting. High levels of 129Xe polarization (avg. %PXe = 51.0% with standard deviation σPXe = 3.0%) were recorded with fast 129Xe polarization build-up time constants (avg. Tb = 25.1 min with standard deviation σTb = 3.1 min) across the first 500 SEOP cell refills, using moderate temperatures of 75 °C. These results demonstrate a more than 2-fold increase in build-up rate relative to previously demonstrated results in a comparable QA study on a second-generation (GEN-2) 129Xe hyperpolarizer device, with only a minor reduction in maximum achievable %PXe and with greater consistency over a larger number of SEOP cell refill processes at a similar polarization lifetime duration (avg. T1 = 82.4 min, standard deviation σT1 = 10.8 min). Additionally, the effects of varying SEOP jacket temperatures, distribution of Rb metal, and preparation and operation of the fluid path are quantified in the context of device installation, performance optimization and maintenance to consistently produce high 129Xe polarization values, build-up rates (Tb as low as 6 min) and lifetimes over the course of a typical high-throughput 129Xe polarization SEOP cell life cycle. The results presented further demonstrate the significant potential for hyperpolarized 129Xe contrast agent in imaging and bio-sensing applications on a clinical scale.
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We present on the utility of in situ nuclear magnetic resonance (NMR) and near-infrared (NIR) spectroscopic techniques for automated advanced analysis of the 129Xe hyperpolarization process during spin-exchange optical pumping (SEOP). The developed software protocol, written in the MATLAB programming language, facilitates detailed characterization of hyperpolarized contrast agent production efficiency based on determination of key performance indicators, including the maximum achievable 129Xe polarization, steady-state Rb-129Xe spin-exchange and 129Xe polarization build-up rates, 129Xe spin-relaxation rates, and estimates of steady-state Rb electron polarization. Mapping the dynamics of 129Xe polarization and relaxation as a function of SEOP temperature enables systematic optimization of the batch-mode SEOP process. The automated analysis of a typical experimental data set, encompassing â¼300 raw NMR and NIR spectra combined across six different SEOP temperatures, can be performed in under 5 min on a laptop computer. The protocol is designed to be robust in operation on any batch-mode SEOP hyperpolarizer device. In particular, we demonstrate the implementation of a combination of low-cost NIR and low-frequency NMR spectrometers (â¼$1,100 and â¼$300 respectively, ca. 2020) for use in the described protocols. The demonstrated methodology will aid in the characterization of NMR hyperpolarization hardware in the context of SEOP and other hyperpolarization techniques for more robust and less expensive clinical production of HP 129Xe and other contrast agents.
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Hyperpolarization is a technique that can increase nuclear spin polarization with the corresponding gains in nuclear magnetic resonance (NMR) signals by 4-8 orders of magnitude. When this process is applied to biologically relevant samples, the hyperpolarized molecules can be used as exogenous magnetic resonance imaging (MRI) contrast agents. A technique called spin-exchange optical pumping (SEOP) can be applied to hyperpolarize noble gases such as 129 Xe. Techniques based on hyperpolarized 129 Xe are poised to revolutionize clinical lung imaging, offering a non-ionizing, high-contrast alternative to computed tomography (CT) imaging and conventional proton MRI. Moreover, CT and conventional proton MRI report on lung tissue structure but provide little functional information. On the other hand, when a subject breathes hyperpolarized 129 Xe gas, functional lung images reporting on lung ventilation, perfusion and diffusion with 3D readout can be obtained in seconds. In this Review, the physics of SEOP is discussed and the different production modalities are explained in the context of their clinical application. We also briefly compare SEOP to other hyperpolarization methods and conclude this paper with the outlook for biomedical applications of hyperpolarized 129 Xe to lung imaging and beyond.
Assuntos
Xenônio/química , Humanos , Imageamento por Ressonância Magnética , Espectroscopia de Ressonância MagnéticaRESUMO
We present spin-exchange optical pumping (SEOP) using a third-generation (GEN-3) automated batch-mode clinical-scale 129Xe hyperpolarizer utilizing continuous high-power (â¼170 W) pump laser irradiation and a novel aluminum jacket design for rapid temperature ramping of xenon-rich gas mixtures (up to 2 atm partial pressure). The aluminum jacket design is capable of heating SEOP cells from ambient temperature (typically 25 °C) to 70 °C (temperature of the SEOP process) in 4 min, and perform cooling of the cell to the temperature at which the hyperpolarized gas mixture can be released from the hyperpolarizer (with negligible amounts of Rb metal leaving the cell) in approximately 4 min, substantially faster (by a factor of 6) than previous hyperpolarizer designs relying on air heat exchange. These reductions in temperature cycling time will likely be highly advantageous for the overall increase of production rates of batch-mode (i.e., stopped-flow) 129Xe hyperpolarizers, which is particularly beneficial for clinical applications. The additional advantage of the presented design is significantly improved thermal management of the SEOP cell. Accompanying the heating jacket design and performance, we also evaluate the repeatability of SEOP experiments conducted using this new architecture, and present typically achievable hyperpolarization levels exceeding 40% at exponential build-up rates on the order of 0.1 min-1.
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Nuclear spin polarization can be significantly increased through the process of hyperpolarization, leading to an increase in the sensitivity of nuclear magnetic resonance (NMR) experiments by 4-8 orders of magnitude. Hyperpolarized gases, unlike liquids and solids, can often be readily separated and purified from the compounds used to mediate the hyperpolarization processes. These pure hyperpolarized gases enabled many novel MRI applications including the visualization of void spaces, imaging of lung function, and remote detection. Additionally, hyperpolarized gases can be dissolved in liquids and can be used as sensitive molecular probes and reporters. This Minireview covers the fundamentals of the preparation of hyperpolarized gases and focuses on selected applications of interest to biomedicine and materials science.
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The exquisite NMR spectral sensitivity and negligible reactivity of hyperpolarized xenon-129 (HP(129)Xe) make it attractive for a number of magnetic resonance applications; moreover, HP(129)Xe embodies an alternative to rare and nonrenewable (3)He. However, the ability to reliably and inexpensively produce large quantities of HP(129)Xe with sufficiently high (129)Xe nuclear spin polarization (P(Xe)) remains a significant challenge--particularly at high Xe densities. We present results from our "open-source" large-scale (â¼1 L/h) (129)Xe polarizer for clinical, preclinical, and materials NMR and MRI research. Automated and composed mostly of off-the-shelf components, this "hyperpolarizer" is designed to be readily implementable in other laboratories. The device runs with high resonant photon flux (up to 200 W at the Rb D1 line) in the xenon-rich regime (up to 1,800 torr Xe in 500 cc) in either single-batch or stopped-flow mode, negating in part the usual requirement of Xe cryocollection. Excellent agreement is observed among four independent methods used to measure spin polarization. In-cell P(Xe) values of â¼90%, â¼57%, â¼50%, and â¼30% have been measured for Xe loadings of â¼300, â¼500, â¼760, and â¼1,570 torr, respectively. P(Xe) values of â¼41% and â¼28% (with â¼760 and â¼1,545 torr Xe loadings) have been measured after transfer to Tedlar bags and transport to a clinical 3 T scanner for MR imaging, including demonstration of lung MRI with a healthy human subject. Long "in-bag" (129)Xe polarization decay times have been measured (T1 â¼38 min and â¼5.9 h at â¼1.5 mT and 3 T, respectively)--more than sufficient for a variety of applications.
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Imageamento por Ressonância Magnética/métodos , Espectroscopia de Ressonância Magnética/métodos , Isótopos de Xenônio/química , Humanos , Pulmão/patologiaRESUMO
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 â¼74 ± 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 â¼ 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.
Assuntos
Imageamento Tridimensional/instrumentação , Espectroscopia de Ressonância Magnética/instrumentação , Desenho de Equipamento , Temperatura , Isótopos de XenônioRESUMO
We describe temperature-ramped spin-exchange optical pumping (TR-SEOP) in an automated high-throughput batch-mode (129)Xe hyperpolarizer utilizing three key temperature regimes: (i) "hot"-where the (129)Xe hyperpolarization rate is maximal, (ii) "warm"-where the (129)Xe hyperpolarization approaches unity, and (iii) "cool"-where hyperpolarized (129)Xe gas is transferred into a Tedlar bag with low Rb content (<5 ng per â¼1 L dose) suitable for human imaging applications. Unlike with the conventional approach of batch-mode SEOP, here all three temperature regimes may be operated under continuous high-power (170 W) laser irradiation, and hyperpolarized (129)Xe gas is delivered without the need for a cryocollection step. The variable-temperature approach increased the SEOP rate by more than 2-fold compared to the constant-temperature polarization rate (e.g., giving effective values for the exponential buildup constant γSEOP of 62.5 ± 3.7 × 10(-3) min(-1) vs 29.9 ± 1.2 × 10(-3) min(-1)) while achieving nearly the same maximum %PXe value (88.0 ± 0.8% vs 90.1% ± 0.8%, for a 500 Torr (67 kPa) Xe cell loading-corresponding to nuclear magnetic resonance/magnetic resonance imaging (NMR/MRI) enhancements of â¼3.1 × 10(5) and â¼2.32 × 10(8) at the relevant fields for clinical imaging and HP (129)Xe production of 3 T and 4 mT, respectively); moreover, the intercycle "dead" time was also significantly decreased. The higher-throughput TR-SEOP approach can be implemented without sacrificing the level of (129)Xe hyperpolarization or the experimental stability for automation-making this approach beneficial for improving the overall (129)Xe production rate in clinical settings.
Assuntos
Imageamento por Ressonância Magnética/instrumentação , Espectroscopia de Ressonância Magnética/instrumentação , Xenônio/química , Desenho de Equipamento , TemperaturaRESUMO
We report on hyperpolarization of quadrupolar (I=3/2) 131Xe via spin-exchange optical pumping. Observations of the 131Xe polarization dynamics via in situ low-field NMR show that the estimated alkali-metal/131Xe spin-exchange rates can be large enough to compete with 131Xe spin relaxation. 131Xe polarization up to 7.6±1.5% was achieved in â¼8.5×1020 spins-a â¼100-fold improvement in the total spin angular momentum-potentially enabling various applications, including: measurement of spin-dependent neutron-131Xe s-wave scattering; sensitive searches for time-reversal violation in neutron-131Xe interactions beyond the Standard Model; and surface-sensitive pulmonary MRI.
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Spin-exchange optical pumping (SEOP) can enhance the NMR sensitivity of noble gases by up to five orders of magnitude at Tesla-strength magnetic fields. SEOP-generated hyperpolarised (HP) 129Xe is a promising contrast agent for lung imaging but an ongoing barrier to widespread clinical usage has been economical production of sufficient quantities with high 129Xe polarisation. Here, the 'standard model' of SEOP, which was previously used in the optimisation of continuous-flow 129Xe polarisers, is modified for validation against two Xe-rich stopped-flow SEOP datasets. We use this model to examine ways to increase HP Xe production efficiency in stopped-flow 129Xe polarisers and provide further insight into the underlying physics of Xe-rich stopped-flow SEOP at high laser fluxes.
Assuntos
Meios de Contraste/química , Pulmão/diagnóstico por imagem , Espectroscopia de Ressonância Magnética/métodos , Rubídio/química , Isótopos de Xenônio/química , Simulação por Computador , Conjuntos de Dados como Assunto , Lasers , Fótons , Sensibilidade e EspecificidadeRESUMO
We present a pilot quality assurance (QA) study of spin-exchange optical pumping (SEOP) performed on two nearly identical second-generation (GEN-2) automated batch-mode clinical-scale 129Xe hyperpolarizers, each utilizing a convective forced air oven, high-power (~170 W) continuous pump laser irradiation, and xenon-rich gas mixtures (~1.30 atm partial pressure). In one study, the repeatability of SEOP in a 1000 Torr Xe/900 Torr N2/100 Torr 4He (2000 Torr total pressure) gas mixture is evaluated over the course of ~700 gas loading cycles, with negligible decrease in performance during the first ~200 cycles, and with high 129Xe polarization levels (avg. %PXe = 71.7% with standard deviation σPXe = 1.5%), build-up rates (avg. γSEOP = 0.019 min-1 with standard deviation σγ = 0.003 min-1) and polarization lifetimes (avg. T1 = 90.5 min with standard deviation σT = 10.3 min) reported at moderate oven temperature of ~70 °C. Although the SEOP cell in this study exhibited a detectable performance decrease after 400 cycles, the cell continued to produce potentially useable HP 129Xe with %PXe = 42.3 ± 0.6% even after nearly 700 refill cycles. The possibility of "regenerating" "dormant" (i.e., not used for an extended period of time) SEOP cells using repeated temperature cycling methods to recover %PXe is also demonstrated. The quality and consistency of results show significant promise for translation to clinical-scale production of hyperpolarized 129Xe contrast agents for imaging and bio-sensing applications.
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We present studies of spin-exchange optical pumping (SEOP) using ternary xenon-nitrogen-helium gas mixtures at high xenon partial pressures (up to 1330 Torr partial pressure at loading, out of 2660 Torr total pressure) in a 500-mL volume SEOP cell, using two automated batch-mode clinical-scale 129Xe hyperpolarizers operating under continuous high-power (~170 W) pump laser irradiation. In this pilot study, we explore SEOP in gas mixtures with up to 45% 4He content under a wide range of experimental conditions. When an aluminum jacket cooling/heating design was employed (GEN-3 hyperpolarizer), 129Xe polarization (%PXe) of 55.9 ± 0.9% was observed with mono-exponential build-up rate γSEOP of 0.049 ± 0.001 min-1 for the 4He-rich mixture (1000 Torr Xe/900 Torr He, 100 Torr N2), compared to %PXe of 49.3 ± 3.3% at γSEOP of 0.035 ± 0.004 min-1 for the N2-rich gas mixture (1000 Torr Xe/100 Torr He, 900 Torr N2). When forced-air cooling/heating was used (GEN-2 hyperpolarizer), %PXe of 83.9 ± 2.7% was observed at γSEOP of 0.045 ± 0.005 min-1 for the 4He-rich mixture (1000 Torr Xe/900 Torr He, 100 Torr N2), compared to %PXe of 73.5 ± 1.3% at γSEOP of 0.028 ± 0.001 min-1 for the N2-rich gas mixture (1000 Torr Xe and 1000 Torr N2). Additionally, %PXe of 72.6 ± 1.4% was observed at a build-up rate γSEOP of 0.041 ± 0.003 min-1 for a super-high-density 4He-rich mixture (1330 Torr Xe/1200 Torr 4He/130 Torr N2), compared to %PXe = 56.6 ± 1.3% at a build-up rate of γSEOP of 0.034 ± 0.002 min-1 for an N2-rich mixture (1330 Torr Xe/1330 Torr N2) using forced air cooling/heating. The observed SEOP hyperpolarization performance under these conditions corresponds to %PXe improvement by a factor of 1.14 ± 0.04 at 1000 Torr Xe density and by up to a factor of 1.28 ± 0.04 at 1330 Torr Xe density at improved SEOP build-up rates by factors of 1.61 ± 0.18 and 1.21 ± 0.11 respectively. Record %PXe levels have been obtained here: 83.9 ± 2.7% at 1000 Torr Xe partial pressure and 72.6 ± 1.4% at 1330 Torr Xe partial pressure. In addition to improved thermal stability for SEOP, the use of 4He-rich gas mixtures also reduces the overall density of produced inhalable HP contrast agents; this property may be desirable for HP 129Xe inhalation by human subjects in clinical settings-especially in populations with heavily impaired lung function. The described approach should enjoy ready application in the production of inhalable 129Xe contrast agent with near-unity 129Xe nuclear spin polarization.
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We present a second-generation open-source automated batch-mode 129Xe hyperpolarizer (XeUS GEN-2), designed for clinical-scale hyperpolarized (HP) 129Xe production via spin-exchange optical pumping (SEOP) in the regimes of high Xe density (0.66-2.5 atm partial pressure) and resonant photon flux (~170 W, Δλ = 0.154 nm FWHM), without the need for cryo-collection typically employed by continuous-flow hyperpolarizers. An Arduino micro-controller was used for hyperpolarizer operation. Processing open-source software was employed to program a custom graphical user interface (GUI), capable of remote automation. The Arduino Integrated Development Environment (IDE) was used to design a variety of customized automation sequences such as temperature ramping, NMR signal acquisition, and SEOP cell refilling for increased reliability. A polycarbonate 3D-printed oven equipped with a thermo-electric cooler/heater provides thermal stability for SEOP for both binary (Xe/N2) and ternary (4He-containing) SEOP cell gas mixtures. Quantitative studies of the 129Xe hyperpolarization process demonstrate that near-unity polarization can be achieved in a 0.5 L SEOP cell. For example, %PXe of 93.2 ± 2.9% is achieved at 0.66 atm Xe pressure with polarization build-up rate constant γSEOP = 0.040 ± 0.005 min-1, giving a max dose equivalent ≈ 0.11 L/h 100% hyperpolarized, 100% enriched 129Xe; %PXe of 72.6 ± 1.4% is achieved at 1.75 atm Xe pressure with γSEOP of 0.041 ± 0.001 min-1, yielding a corresponding max dose equivalent of 0.27 L/h. Quality assurance studies on this device have demonstrated the potential to refill SEOP cells hundreds of times without significant losses in performance, with average %PXe = 71.7%, (standard deviation σP = 1.52%) and mean polarization lifetime T1 = 90.5 min, (standard deviation σT = 10.3 min) over the first ~200 gas mixture refills, with sufficient performance maintained across a further ~700 refills. These findings highlight numerous technological developments and have significant translational relevance for efficient production of gaseous HP 129Xe contrast agents for use in clinical imaging and bio-sensing techniques.
Assuntos
Espectroscopia de Ressonância Magnética , Compostos Radiofarmacêuticos/síntese química , Isótopos de Xenônio/síntese química , Automação , Reprodutibilidade dos Testes , SoftwareRESUMO
We present a systematic, multiparameter study of Rb/(129)Xe 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 (129)Xe polarization as a function of SEOP-cell operating temperature, photon flux, and xenon partial pressure to maximize (129)Xe 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 (129)Xe 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 (129)Xe production efficiency.
Assuntos
Óptica e Fotônica/instrumentação , Isótopos de Xenônio/análise , Desenho de Equipamento , Imageamento por Ressonância Magnética , Espectroscopia de Ressonância Magnética , Fótons , Pressão , Espectrofotometria InfravermelhoRESUMO
Here we provide a full report on the construction, components, and capabilities of our consortium's "open-source" large-scale (~1L/h) (129)Xe 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 (129)Xe nuclear spin polarization values of ~30%-90% have been measured for Xe loadings of ~300-1600Torr. Typical (129)Xe 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 (129)Xe 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.
Assuntos
Análise de Injeção de Fluxo/instrumentação , Calefação/instrumentação , Marcação por Isótopo/instrumentação , Robótica/instrumentação , Análise Espectral/instrumentação , Isótopos de Xenônio/síntese química , Isótopos de Xenônio/isolamento & purificação , Desenho de Equipamento , Falha de Equipamento , Compostos Radiofarmacêuticos/síntese química , Compostos Radiofarmacêuticos/isolamento & purificaçãoRESUMO
The (129)Xe nuclear spin polarization (P(Xe)) that can be achieved via spin-exchange optical pumping (SEOP) is typically limited at high in-cell xenon densities ([Xe](cell)), due primarily to corresponding reductions in the alkali metal electron spin polarization (e.g. P(Rb)) caused by increased non-spin-conserving Rb-Xe collisions. While demonstrating the utility of volume holographic grating (VHG)-narrowed lasers for Rb/(129)Xe SEOP, we recently reported [P. Nikolaou et al., JMR 197 (2009) 249] an anomalous dependence of the observed P(Xe) on the in-cell xenon partial pressure (p(Xe)), wherein P(Xe) values were abnormally low at decreased p(Xe), peaked at moderate p(Xe) (~300 torr), and remained surprisingly elevated at relatively high p(Xe) values (>1000 torr). Using in situ low-field (129)Xe NMR, it is shown that the above effects result from an unexpected, inverse relationship between the xenon partial pressure and the optimal cell temperature (T(OPT)) for Rb/(129)Xe SEOP. This interdependence appears to result directly from changes in the efficiency of one or more components of the Rb/(129)Xe SEOP process, and can be exploited to achieve improved P(Xe) with relatively high xenon densities measured at high field (including averaged P(Xe) values of ~52%, ~31%, ~22%, and ~11% at 50, 300, 500, and 2000 torr, respectively).
Assuntos
Espectroscopia de Ressonância Magnética/instrumentação , Rubídio/química , Xenônio/química , Algoritmos , Campos Eletromagnéticos , Lasers , Espectroscopia de Ressonância Magnética/métodos , Temperatura , Isótopos de XenônioRESUMO
Volume holographic gratings (VHGs) can be exploited to narrow the spectral output of high-power laser-diode arrays (LDAs) by nearly an order of magnitude, permitting more efficient generation of laser-polarized noble gases for various applications. A approximately 3-fold improvement in (129)Xe nuclear spin polarization, P(Xe), (compared to a conventional LDA) was achieved with the VHG-LDA's center wavelength tuned to a wing of the Rb D(1) line. Additionally, an anomalous dependence of P(Xe) on the xenon density within the OP cell is reported-including high P(Xe) values (>10%) at high xenon partial pressures (approximately 1000 torr).