NMR Study of Laser polarized ~(129) Xe in Low Pressure Natural Xenon Gas

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MEASUREMENTS OF RELAXATION OF SPIN POLARIZED 129Xe NUCLEI IN HIGH MAGNETIC FIELDS

We observed the NMR signal of low-pressure gas ¹²⁹Xe by laser enhanced method on an MSL-400 NMR spectrometer and measured nuclear spin relaxations of ¹²⁹Xe gas at various temperatures. The relaxation rate constant of ¹²⁹Xe-¹³³Cs spin exchange was obtained as (6.8±0.5)×10^-16cm^-3s^-1.     

激光极化129Xe的生物磁共振成像研究进展

激光光抽运自旋交换方法能够极大地增强＾１２９Ｘｅ核自旋极化,其获得的非平衡极化度远远高于在相同磁场里玻尔兹曼平衡值。     

MEASUREMENTS OF RELAXATION OF SPIN POLARIZED 129Xe NUCLEI IN HIGH MAGNETIC FIELDS

We observed the NMR signal of low-pressure gas ¹²⁹Xe by laser enhanced method on an MSL-400 NMR spectrometer and measured nuclear spin relaxations of ¹²⁹Xe gas at various temperatures. The relaxation rate constant of ¹²⁹Xe-¹³³Cs spin exchange was obtained as (6.8±0.5)×10^-16cm^-3s^-1.     

Gas flow MRI using circulating laser-polarized 129Xe.

We describe an experimental approach that combines multidimensional NMR experiments with a steadily renewed source of laser-polarized 129Xe. Using a continuous flow system to circulate the gas mixture, gas phase NMR signals of laser-polarized 129Xe can be observed with an enhancement of three to four orders of magnitude compared to the equilibrium 129Xe NMR signal. Due to the fact that the gas flow recovers the nonequilibrium 129Xe nuclear spin polarization in 0.2 to 4 s, signal accumulation on the time scale of seconds is feasible, allowing previously inaccessible phase cycling and signal manipulation. Several possible applications of MRI of laser-polarized 129Xe under continuous flow conditions are presented here. The spin density images of capillary tubes demonstrate the feasibility of imaging under continuous flow. Dynamic displacement profiles, measured by a pulsed gradient spin echo experiment, show entry flow properties of the gas passing through a constriction under laminar flow conditions. Further, dynamic displacement profiles of 129Xe, flowing through polyurethane foams with different densities and pore sizes, are presented.     

激光极化129Xe核自旋弛豫率的测量

由弱磁场下光泵自旋交换、强磁场中核磁共振测量方法,获得激光极化低压同位素¹²⁹Xe气体的核自旋弛豫率1/T₁及其与N₂气压力、环境温度的关系.结果表明:在291K的室温下,对于0~11 333.05Pa的N₂气压力范围,1/T₁随着N₂气压力的增加而增大;N₂气压力为1 466.63Pa时,1/T₁随着样品温度从234K到292K增高而减小     

Relaxation behavior of laser-polarized (129)Xe gas: size dependency and wall effect of the T(1) relaxation time in glass and gelatin bulbs

Size dependency of the relaxation time T(1) was measured for laser-polarized (129)Xe gas encapsulated in different sized cavities made by glass bulbs or gelatin capsules. The use of laser-polarized gas enhances the sensitivity a great deal, making it possible to measure the longer (129)Xe relaxation time in quite a short time. The size dependency is analyzed on the basis of the kinetic theory of gases and a relationship is derived in which the relaxation rate is connected with the square inverse of the diameter of the cavity. Such an analysis provides a novel parameter which denotes the wall effect on the relaxation rate when a gas molecule collides with the surface once in a second. The relaxation time of (129)Xe gas is also dependent on the material which forms the cavity. This dependency is large and the relaxation study using polarized (129)Xe gas is expected to offer important information about the state of the matter of the cavity wall.     

129Xe核自旋极化转移增强分子的核磁共振信号

激光极化的129Xe核具有极高的非平衡极化度和长的弛豫时间,这一特点使得它能够极化转移增强液体、固体或者固体表面分子中原子核自旋极化。因而,提高了它们的核磁共振探测灵敏度和扩展了在材料和表面科学研究中的应用。综述激光极化129Xe核与其它分子中原子核之间的极化转移研究与进展,介绍相关物理机制和参数的测量。     

Enhanced NMR signal from the laser-polarized129Xe produced by spin exchange at a high magnetic field

Nuclear-magnetic-resonance (NMR) measurement of laser-polarized gaseous¹²⁹Xe produced by spin-exchange optical pumping with a narrow-linewidth laser at a high magnetic field of 4.7 T is reported. The samples are contained in the glass tubes. The nuclear spin polarization of the laserpolarized¹²⁹Xe is 3.9%, and this corresponds to an enhancement of 9· 10³ compared to the equilibrium value at 311 K and at the same magnetic field. The laser-enhanced¹²⁹Xe NMR signals can be used in MR imaging.     

Relaxation Behavior of Laser-Polarized Xe Gas: Size Dependency and Wall Effect of the T1 Relaxation Time in Glass and Gelatin Bulbs

Size dependency of the relaxation time T₁ was measured for laser-polarized ¹²⁹Xe gas encapsulated in different sized cavities made by glass bulbs or gelatin capsules. The use of laser-polarized gas enhances the sensitivity a great deal, making it possible to measure the longer ¹²⁹Xe relaxation time in quite a short time. The size dependency is analyzed on the basis of the kinetic theory of gases and a relationship is derived in which the relaxation rate is connected with the square inverse of the diameter of the cavity. Such an analysis provides a novel parameter which denotes the wall effect on the relaxation rate when a gas molecule collides with the surface once in a second. The relaxation time of ¹²⁹Xe gas is also dependent on the material which forms the cavity. This dependency is large and the relaxation study using polarized ¹²⁹Xe gas is expected to offer important information about the state of the matter of the cavity wall.     

Collisional 3He and 129Xe frequency shifts in Rb-noble-gas mixtures

The Fermi-contact interaction that characterizes collisional spin exchange of a noble gas with an alkali-metal vapor also gives rise to NMR and EPR frequency shifts of the noble-gas nucleus and the alkali-metal atom, respectively. We have measured the enhancement factor κ0 that characterizes these shifts for Rb-129Xe to be 493±31, making use of the previously measured value of κ0 for Rb-3He. This result allows accurate 129Xe polarimetry with no need to reference a thermal-equilibrium NMR signal.     

Nuclear spin resonance of (129)Xe doped with O(2)

Spin-lattice relaxation of (129)Xe nuclei in solid natural xenon has been investigated in detail over a large range of paramagnetic O(2) impurity concentrations. Direct measurements of the ground state magnetic properties of the O(2) are difficult because the ESR (electron spin resonance) lines of O(2) are rather unstructured, but NMR measurements in the liquid helium temperature region (1.4-4 K) are very sensitive to the effective magnetic moments associated with the spin 1 Zeeman levels of the O(2) molecules and to the O(2) magnetic relaxation. From these measurements, the value of the D[Sz(2)-(1/3)S(2)] spin-Hamiltonian term of the triplet spin ground state of O(2) can be determined. The temperature and magnetic field dependence of the measured paramagnetic O(2)-induced excess line width of the (129)Xe NMR signal agree well with the theoretical model with the spin-Hamiltonian D=0.19 meV (2.3 K), and with the reasonable assumption that the E[S(x)(2)-S(y)(2)] spin-Hamiltonian term is close to 0 meV. An anomalous temperature dependence between 1.4 K and 4.2K of the (129)Xe spin-lattice relaxation rate, T(1n)(-1)(T), is also accounted for by our model. Using an independent determination of the true O(2) concentration in the Xe-O(2) solid, the effective spin lattice relaxation time (which will be seen to be transition dependent) of the O(2) at 2.3 K and 0.96 T is determined to be approximately 1.4 x 10(-8)s. The experimental results, taken together with the relaxation model, suggest routes for bringing highly spin-polarized (129)Xe from the low temperature condensed phase to higher temperatures without excessive depolarization.     

Measurement of persistence in 1D diffusion

Using a novel NMR scheme we observed persistence in 1D gas diffusion. Analytical approximations and numerical simulations have indicated that for an initially random array of spins undergoing diffusion, the probability p(t) that the average spin magnetization in a given region has not changed sign (i.e., "persists") up to time t follows a power law t(-straight theta), where straight theta depends on the dimensionality of the system. Using laser-polarized 129Xe gas, we prepared an initial "quasirandom" 1D array of spin magnetization and then monitored the ensemble's evolution due to diffusion using real-time NMR imaging. Our measurements are consistent with analytical and numerical predictions of straight theta approximately 0.12.     

Hyperpolarized (131)Xe NMR spectroscopy

Hyperpolarized (hp) (131)Xe with up to 2.2% spin polarization (i.e., 5000-fold signal enhancement at 9.4 T) was obtained after separation from the rubidium vapor of the spin-exchange optical pumping (SEOP) process. The SEOP was applied for several minutes in a stopped-flow mode, and the fast, quadrupolar-driven T(1) relaxation of this spin I = 3/2 noble gas isotope required a rapid subsequent rubidium removal and swift transfer into the high magnetic field region for NMR detection. Because of the xenon density dependent (131)Xe quadrupolar relaxation in the gas phase, the SEOP polarization build-up exhibits an even more pronounced dependence on xenon partial pressure than that observed in (129)Xe SEOP. (131)Xe is the only stable noble gas isotope with a positive gyromagnetic ratio and shows therefore a different relative phase between hp signal and thermal signal compared to all other noble gases. The gas phase (131)Xe NMR spectrum displays a surface and magnetic field dependent quadrupolar splitting that was found to have additional gas pressure and gas composition dependence. The splitting was reduced by the presence of water vapor that presumably influences xenon-surface interactions. The hp (131)Xe spectrum shows differential line broadening, suggesting the presence of strong adsorption sites. Beyond hp (131)Xe NMR spectroscopy studies, a general equation for the high temperature, thermal spin polarization, P, for spin I ≥ 1/2 nuclei is presented.     

Single-Shot Diffusion Measurement in Laser-Polarized Gas

A single-shot pulsed gradient stimulated echo sequence is introduced to address the challenges of diffusion measurements of laser polarized 3He and 129Xe gas. Laser polarization enhances the NMR sensitivity of these noble gases by >10(3), but creates an unstable, nonthermal polarization that is not readily renewable. A new method is presented which permits parallel acquisition of the several measurements required to determine a diffusive attenuation curve. The NMR characterization of a sample's diffusion behavior can be accomplished in a single measurement, using only a single polarization step. As a demonstration, the diffusion coefficient of a sample of laser-polarized 129Xe gas is measured via this method.     

Study of gas-fluidization dynamics with laser-polarized 129Xe

We report initial NMR studies of gas dynamics in a particle bed fluidized by laser-polarized xenon (129Xe) gas. We have made preliminary measurements of two important characteristics: gas exchange between the bubble and emulsion phases and the gas velocity distribution in the bed. We used T2* contrast to differentiate the bubble and emulsion phases by choosing solid particles with large magnetic susceptibility. Experimental tests demonstrated that this method was successful in eliminating 129Xe magnetization in the emulsion phase, which enabled us to observe the time dependence of the bubble magnetization. By employing the pulsed field gradient method, we also measured the gas velocity distribution within the bed. These results clearly show the onset of bubbling and can be used to deduce information about gas and particle motion in the fluidized bed.     

流动系统中的激光增强固体和液体129Xe核磁共振信号

在流动系统中,用半导体阵列激光器在低磁场下抽运Cs原子,由自旋交换碰撞产生极化的129Xe气体,在SY80M核磁共振谱仪中,冻成固体和液体后的极化度分别为216%和145%,和相同条件下未光泵的129Xe极化度相比,分别增强6000和5000倍.为将激光增强固体和液体129Xe用于量子计算提供了基础和可能.并对输运和相变过程中极化损失作了讨论 关键词： 光泵 激光极化 核磁共振信号 光和原子相互作用     

Magnetic resonance imaging of convection in laser-polarized xenon

We demonstrate nuclear magnetic resonance (NMR) imaging of the flow and diffusion of laser-polarized xenon (129Xe) gas undergoing convection above evaporating laser-polarized liquid xenon. The large xenon NMR signal provided by the laser-polarization technique allows more rapid imaging than one can achieve with thermally polarized gas-liquid systems, permitting shorter time-scale events such as rapid gas flow and gas-liquid dynamics to be observed. Two-dimensional velocity-encoded imaging shows convective gas flow above the evaporating liquid xenon, and also permits the measurement of enhanced gas diffusion near regions of large velocity variation.     

Intermolecular dipole-dipole relaxation of (129)Xe dissolved in water

Intermolecular (129)Xe-(1)H nuclear Overhauser effects and (129)Xe longitudinal relaxation time measurements were used to demonstrate that the dipole-dipole coupling is the dominant relaxation mechanism for (129)Xe in water, at room temperature. (129)Xe-(1)H cross-relaxation rates were derived to be sigma(XeH) approximately 3.2 +/- 0.3 x 10(-3) s(-1), independent of xenon pressure (in the range of 1-10 bar) and of the presence of oxygen. Corresponding xenon-proton internuclear distances were calculated to be 2.69 +/- 0.12 A. Using the magnitude of the dipole-dipole coupling and the spin density ratio between dissolved xenon and bulk water, it is estimated that (129)Xe-(1)H spin polarization-induced nuclear Overhauser effects would yield little net proton signal enhancement in water.     

High capacity production of >65% spin polarized xenon-129 for NMR spectroscopy and imaging

A rubidium spin exchange optical pumping system for high capacity production of >65% spin polarized 129Xe gas is described. This system is based on a fiber coupled multiple laser diode array capable of producing an unprecedented 210 W of circularly polarized light at the pumping cell with a laser line width of 1.6 nm. The 129Xe nuclear spin polarization is measured as a function of flow rate, pumping cell pressure, and laser power for varying pumping gas compositions. A maximum 129Xe nuclear polarization of 67% was achieved using a 0.6% Xe mixture at a Xe flow rate of 2.45 sccm. The ability to generate 12% polarized 129Xe at rates in excess of 1L-atm/h is also demonstrated. To achieve production of 129Xe gas at even higher polarization will rely on further optimization of the pumping cell and laser beam geometries in order to mitigate problems associated with temperature gradients that are encountered at high laser power and Rb density.