Metastability exchange optical pumping of <Superscript>3</Superscript>He at high pressure and high magnetic field for medical applications

Systematic studies of the metastability exchange optical pumping (MEOP) process in ³He gas at high magnetic fields (0.45, 0.9, 1.5, and 2 T) and pressures (32 and 64 mbar) are performed. The impact of experimental parameters such as laser power, beam profile, and shape of the pumping cell is evaluated. By varying the discharge intensity in the cell, the density of metastable state atoms and the plasma-induced nuclear relaxation rate are also controlled, and their effect on the MEOP efficiency can be investigated. Very accurate experimental results are obtained, opening the way to quantitative tests of a recently proposed model of the MEOP process at high magnetic field. We report selected MEOP results with nuclear polarizations exceeding 50 % at 64 mbar and 2 T, which represents a dramatic improvement in performances over MEOP at low magnetic field. The present findings suggest that still higher polarizations can be achieved in higher magnetic fields, and motivate investigations at higher gas pressures. New ways of producing hyperpolarized ³He for magnetic resonance imaging and medical applications can be envisaged, as most clinical whole-body scanners operate at 1.5 T.     

Optical measurement of <Superscript>3</Superscript>He nuclear polarization for metastable exchange optical pumping studies at high magnetic field

An accurate optical method to measure the nuclear polarization of ³He atoms in the 1¹S ground state is described. The absorption of a weak, probe laser beam is used to measure the relative populations of two hyperfine sublevels of the 2³S metastable state that are not addressed by the pumping laser beam. Since a common spin temperature between the ground and metastable states is established by metastable exchange collisions, the nuclear polarization can be derived from these absorption measurements. The method is highly sensitive, robust, and can be used to monitor the dynamics of optical pumping and relaxation processes without interfering with them. It was successfully implemented and tested in the 0.45–2.0 T magnetic field range at the ³He gas pressure up to 67 mbar.     

Increasing the pump-up rate to polarize He gas using spin-exchange optical pumping method

In recent years, polarized ³He gas has increasingly been used as neutron polarizers and polarization analyzers. Two of the leading methods to polarize the ³He gas are the spin-exchange optical pumping (SEOP) method and the meta-stable exchange optical pumping (MEOP) method. At present, the SEOP setup is comparatively compact due to the fact that it does not require the sophisticated compressor system used in the MEOP method. The temperature and the laser power available determine the speed, at which the SEOP method polarizes the ³He gas. For the quantity of gas typically used in neutron scattering work, this speed is independent of the quantity of the gas required, whereas the polarizing time using the MEOP method is proportional to the quantity of gas required. Currently, using the SEOP method to polarize several bar-liters of ³He to 70% polarization would require 20−40 h. This is an order of magnitude longer than the MEOP method for the same quantity of gas and polarization. It would therefore be advantageous to speed up the SEOP process. In this article, we analyze the requirements for temperature, laser power, and the type of alkali used in order to shorten the time required to polarize ³He gas using the SEOP method.     

Free precession and transverse relaxation of hyperpolarized <Superscript>129</Superscript>Xe gas detected by SQUIDs in ultra-low magnetic fields

We studied the free precession of the nuclear magnetization of hyperpolarized ¹²⁹Xe gas in external magnetic fields as low as B₀ = 4.5 nT, using SQUIDs as magnetic flux detectors. The transverse relaxation was mainly caused by the restricted diffusion of ¹²⁹Xe in the presence of ambient magnetic field gradients. Its pressure dependence was measured in the range from 30 mbar to 850 mbar and compared quantitatively to theory. Motional narrowing was observed at low pressure, yielding transverse relaxation times of up to 8000 s.     

An open-access, very-low-field MRI system for posture-dependent 3He human lung imaging

We describe the design and operation of an open-access, very-low-field, magnetic resonance imaging (MRI) system for in vivo hyperpolarized ³He imaging of the human lungs. This system permits the study of lung function in both horizontal and upright postures, a capability with important implications in pulmonary physiology and clinical medicine, including asthma and obesity. The imager uses a bi-planar B₀ coil design that produces an optimized 65 G (6.5 mT) magnetic field for ³He MRI at 210 kHz. Three sets of bi-planar coils produce the x, y, and z magnetic field gradients while providing a 79-cm inter-coil gap for the imaging subject. We use solenoidal Q-spoiled RF coils for operation at low frequencies, and are able to exploit insignificant sample loading to allow for pre-tuning/matching schemes and for accurate pre-calibration of flip angles. We obtain sufficient SNR to acquire 2D ³He images with up to 2.8 mm resolution, and present initial 2D and 3D ³He images of human lungs in both supine and upright orientations. ¹H MRI can also be performed for diagnostic and calibration reasons.     

Polarized He spin-filters using MEOP for wide-angle polarization analysis

Polarized ³He spin-filters are currently employed on a wide range of neutron instruments at the ILL, primarily for diffraction, reflectometry and fundamental physics. A wide range of recent and ongoing improvements are enabling the implementation of this technique for wide-angle polarization analysis for inelastic measurements. These include

• Progress in metastability-exchange optical pumping (MEOP), resulting in on-beam polarization levels of up to 80%.

• 1st generation “Pastis-1” coils for rotating the neutron polarization at the sample position, allowing for “XYZ” polarization analysis.

• 2nd generation “Pastis-2” coils with no blind angles in the equatorial plane.

• Spin-filter cells with glued silicon windows, allowing for wide-angle “banana” cells with very low background scattering.

• Polarization-preserving capillaries for transferring polarized ³He gas into the cell without manual access.

The development of capillary transfer also allows for a completely new way of working with ³He spin-filters: connecting the cells on the instruments directly to the MEOP filling station several tens of meters away and allowing for quasi-continuous operation.     

A system for low field imaging of laser-polarized noble gas

We describe a device for performing MRI with laser-polarized noble gas at low magnetic fields (<50 G). The system is robust, portable, inexpensive, and provides gas-phase imaging resolution comparable to that of high field clinical instruments. At 20.6 G, we have imaged laser-polarized (3)He (Larmor frequency of 67 kHz) in both sealed glass cells and excised rat lungs, using approximately 0.1 G/cm gradients to achieve approximately 1 mm(2) resolution. In addition, we measured (3)He T(2)(*) times greater than 100 ms in excised rat lungs, which is roughly 20 times longer than typical values observed at high ( approximately 2 T) fields. We include a discussion of the practical considerations for working at low magnetic fields and conclude with evidence of radiation damping in this system.     

High pressure-high field Mössbauer spectroscopy on pure and magnetically diluted europium-monochalcogenides

By simultaneously applying pressures up to 19.6 kbar and magnetic fields up to 13 T, the magnetic hyperfine (hf) fields of the Eu-monochalcogenides Eu X (X = S, Se, Te) and of the magnetic dilution system Eu_xSr_1-xS were studied using the ¹⁵¹Eu Mössbauer effect. Expected relations between the magnetic exchange interactions and the transferred hyperfine (thf) fields have been confirmed. The pressure dependence of the total hf field in the ferromagnetically saturated state of EuS, EuSe and EuTe has been shown to be due mainly to the pressure response of the thf field of the nearest Eu-neighbours. Except with EuO the thf fields of the next nearest Eu-neighbours and the Eu-core polarization field are nearly insensitive to pressure. The results are discussed in terms of the exchange model proposed by T. Kasuya.     

Applications of He neutron spin filters at the NCNR

At the NIST Center for Neutron Research (NCNR), we have applied ³He neutron spin filters (NSFs) to the instruments where ³He NSFs are advantageous, such as thermal triple-axis spectrometry, small-angle neutron scattering, and diffuse reflectometry. We present the status of our development and application of this method, including polarized gas production by spin-exchange optical pumping, magnetostatic cavities for storage of the polarized gas on the beam line, and nuclear magnetic resonance (NMR)-based, on-line monitoring and reversal of the ³He polarization. We present the status of developing user-friendly interfaces incorporated into the instrument software to handle these ³He neutron spin filters while taking data and performing data analysis. Finally we discuss the status of development of a polarization capability on the multi-axis crystal spectrometer, which requires polarization analysis over a 220° angular range.     

Low field CIDNP of amino acids and proteins: characterization of transient radicals and NMR sensitivity enhancement

A new method for measuring and exploiting the magnetic field dependence of chemically induced dynamic nuclear polarization (CIDNP) is described. A solution of an amino acid or protein together with a flavin photosensitizer is irradiated with laser light at a position in the bore of a superconducting NMR magnet where the field is between 0.1 T and 7.0 T. The polarized sample is then transferred by rapid injection into an NMR tube at the centre of the magnet (at 9.4 T), where the spectrum is recorded. The observed ¹H CIDNP field dependence of tyrosine agrees well with the diffusion model of the radical pair mechanism. The field dependence of histidine, tryptophan and methionine CIDNP allows the g values of the transient radicals responsible for the polarization to be determined. Experiments in which amino acids compete for the photoexcited flavin indicate that methionine residues could be used as probes of surface accessibility, especially if the polarization is generated in low fields (～ 0.7 T) and detected in high fields (≥ 9.4 T). Possible extensions of the technique to study protein folding and the structures of partially denatured states of proteins are discussed.     

Frequency-selective laser optical pumping and spin exchange of cesium with129Xe and131Xe in a high magnetic field

We report the experimental results of frequency-selective laser optical pumping and spin exchange of Cs with¹²⁹Xe and¹³¹Xe in a high magnetic field of 11.74 T. Our results show that hyperpolarized¹²⁹Xe and¹³¹Xe nuclear magnetic resonance (NMR) signals exhibit alternating phases when the laser frequency for pumping the cesium atoms is changed, which is explained on the basis of the high-field optical pumping of Cs. We obtain about 3% polarization of the¹²⁹Xe. The electron-spin polarization of the Cs atoms has been measured to be about 22% with a simple NMR method.     

On the electric activity of superfluid systems

The Keldysh theory of the superfluidity of a diluted electron-hole gas has been generalized to the case of the possible polarization of the pairs. It has been shown that the inhomogeneity of the system induces the dipole moment, which appears near the system boundaries and is proportional to the gradient of the particle density. It has been found that the quantized vortices in the magnetic field carry a real electric charge. The charge density in He II rotating at a rate of 10²s⁻¹ in a magnetic field of 10 T is about 10⁴ e cm⁻³, where e is the elementary charge.     

In-situ SEOP polarizer and initial tests on a high flux neutron beam

Polarized ³He has shown its unique characteristics in many areas of polarized neutron scattering, its ability to polarize neutrons at short wavelengths, accept wide-angle and divergent beams and low backgrounds enable new classes of experiments. While polarized ³He is not a steady state solution as commonly applied, the benefits have been shown to offset the drawbacks of polarizing and refreshing the polarization in the neutron spin filter cells. As an extension of this work, in-situ polarization using the spin-exchange optical pumping (SEOP) method was explored as a means to construct a system which could be used to polarize ³He in the state used for an effective neutron spin filter to constant polarization while on the neutron beam. An in-situ SEOP polarizer was constructed. This device utilized many devices and principles developed for neutron spin filters which are polarized off the beam line using either SEOP or metastability exchange optical pumping (MEOP) under the same research program. As a collimation of this work effects of extremely high neutron capture flux density incident on the in-situ polarizer were explored.     

Influence of in-plane magnetic field on spin polarization in the presence of the oft-neglected k-Dresselhaus spin-orbit coupling

The influence of in-plane magnetic field on spin polarization in the presence of the oft-neglected k³-Dresselhaus spin-orbit coupling was investigated. The k³-Dresselhaus term can produce a limited spin polarization. The in-plane magnetic field plays a great role in the tunneling process. It can generate the perfect spin polarization of the electrons and the ideal transmission coefficient for spin up and down simultaneously. In energy scale, complete separation between spin up and down resonance was obtained by a relatively higher in-plane magnetic field while a comparatively lower in-plane magnetic field vanishes the spin separation. On the other hand, the spin relaxation can be suppressed by compensating the oft-neglected k³-Dresselhaus spin orbit coupling using a relatively lower in-plane magnetic field.     

Resolving 3D magnetism in nanoparticles using polarization analyzed SANS

Utilizing a polarized ³He cell as an analyzer we were able to perform a full polarization analysis on small-angle neutron scattering (SANS) data from an ensemble of 7 nm magnetite nanoparticles. The results led to clear separation of magnetic and nuclear scattering plus a 3D vectorial decomposition of the magnetism observed. At remanence variation in long-range magnetic correlation length was found to be highly dependent on temperature from 50 to 300 K. Additionally, we were able to compare the magnetic scattering from moments along and perpendicular to an applied field at saturation and in remanence.     

Interrelationship between the polarization moments of different parity upon optical pumping of atoms under magnetic resonance conditions: III. Comparison of theory with experiment

The optical pumping of Cs atoms with light of the D ₁ line under magnetic resonance conditions is numerically calculated. This calculation is done to check the suggestion that an unexpectedly strong influence of the polarization of the pumping light on the resonance signals of transverse alignment, which we observed experimentally, is caused by the coupling between orientation and alignment by means of the magnetic field and/or the pumping light. This suggestion has been confirmed: upon circularly polarized pumping, the shape of the signal line of transverse alignment proved to be similar, as well as in the experiment, to the shape of the signal line of transverse orientation and was sharply different from the shape of the line of alignment observed upon linearly polarized pumping. For metastable 2³ S ₁ ⁴He atoms, in accordance with the experimental data, the calculated shape of the signal line of transverse alignment is found to be independent of the polarization of the pumping light. The calculations also confirm the possibility of a reverse effect: the influence of alignment on orientation, which manifests itself in the occurrence of orientation upon pumping with unpolarized light under magnetic resonance conditions. For Cs atoms exposed to a field of ～0.6 Oe, the largest contribution to this effect is yielded by the field coupling of orientation and alignment, whereas, for metastable 2³ S ₁ ⁴He atoms, the largest contribution is made by the light coupling of these polarization moments.     

Recent results on hyperpolarized<Superscript>3</Superscript>He−<Superscript>4</Superscript>He liquid mixtures

Laser optical pumping in low magnetic field provides very high nuclear polarizations in gaseous helium mixtures, and is used to prepare polarized liquid. Wall relaxation in glass cells is effiently reduced using cesium coatings, and bulk longitudinal relaxation times are measured. In highly magnetized samples, dipolar fields control the spin dynamics in anisotropic volumes and weak external magnetic field inhomogeneities. Long lived magnetostatic modes are observed by pulsed NMR. Detailed analysis of their frequency and damping gives information on magnetization density and spin diffusion coefficient in polarized mixtures. Experiments are performed above 0.2 K on mixtures with³He concentrations of order a few percents or larger. When phase separation occurs, the³He-rich phase retains a high polarization.     

In vivo natural-abundance17O/1H MRI of rhesus monkey body in a whole-body scanner

In vivo natural-abundance¹⁷O and¹H magnetic resonance imaging (MRI) techniques were combined to image the whole body of a rhesus monkey. The results demonstrate the feasibility of acquiring consecutive fast¹⁷O and¹H images with a standard MRI scanner. The method has applications in the field of functional MRI and in¹⁷O MRI measurements of metabolism rate.     

High-pressure Mössbauer spectroscopy using synchrotron radiation and radioactive sources

A high-pressure ⁵⁷Fe Mössbauer study of SrFeO₃ up to 74 GPa has been performed with diamond-anvil-cell (DAC) using synchrotron radiation and a radioactive point source of ⁵⁷Co in Rh. SrFeO₃ is known as a typical cubic perovskite with a high-valence state of Fe⁴⁺ and shows metallic conductivity at 0.1 MPa down to 4.2 K. Applying an external high pressure, SrFeO₃ has not shown any structural transformation up to 74 GPa keeping an Fe⁴⁺ state but the Néel temperature increases up to 300 K at 18 GPa. The external high pressure may induce the ferromagnetism in SrFeO₃ by a decrease of the interatomic distance of Fe or an increase of the d-band width. ⁵⁷Fe Mössbauer measurements under externally applied longitudinal magnetic field using radioactive ⁵⁷Co in Rh source and also nuclear forward scattering measurements with a linearly polarized synchrotron radiation under external magnetic field indicate the existence of the pressure induced ferromagnetism in SrFeO₃. In this work we compare high-pressure Mössbauer spectroscopy using synchrotron and radioactive sources and summarize the advantages and disadvantages of each method.     

Intravascular delivery of hyperpolarized129Xenon forin vivo MRI

The nuclear polarization of¹²⁹Xe and³He can be enhanced by several orders of magnitude by using optical pumping techniques, thus allowing NMR detection of xenon and helium in very low concentrations. The benefits of optically enhanced magnetic resonance (MR) are already exploited in MR imaging of the lungs using optically polarized³He. The high solubility of xenon in blood and lipids suggests a variety ofin vivo MR applications, for instance perfusion measurements or functional MR studies. This article reviews some current work directed towards delivery of optically polarized xenon forin vivo MR applications.