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.     

Self-oscillations of electronic and nuclear polarization during optical excitation of an Si/CaF2 nanostructure in a transverse magnetic field

We examine theoretically low-frequency and high-frequency self-oscillations of electronic and nuclear polarization in an Si/CaF₂ nanostructure in a transverse magnetic field. We show that the low-frequency self-oscillations are stable in zero field, and the analogous high-frequency oscillations are stable beyond the region of the maximum on the Hanle curve. The frequency of the low-frequency oscillations is 0.001–0.500 of the reciprocal nuclear longitudinal relaxation time; the frequency of the high-frequency oscillations is 10⁸–10⁹ Hz, and their amplitude reaches 50% of the initial electronic spin polarization. __________ Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 73, No. 3, pp. 363–369, May–June, 2006.     

Microwave-induced optical nuclear polarization in Si:P:B

The first successful experiments of microwave-induced optical nuclear polarization in compensated silicon are presented. Bound holes are created at the boron sites using band-gap light of 1.047 μm. Subsequently, the high spin polarization of these bound holes is transferred to the ²⁹Si nuclei using microwave irradiation, resulting in an enhancement of the nuclear magnetic resonance signal. It is shown that a long lifetime of the nuclear spin polarization thus created is obtained, once the excitation light is shut off.     

NMR of 29Si and 25Mg In Mg2SiO4 with dynamic polarization technique

Nuclear magnetic resonance of ²⁹Si and ²⁵Mg in natural abundance has been observed in Cr³⁺ doped Mg₂SiO₄ after cooling the nuclear spin system by dynamic nuclear polarization. The quadrupole coupling tensors of ²⁵Mg at the 4a and 4c positions have been determined.     

A wide angle neutron spin filter system using polarized He

Polarized ³He neutron spin filters can operate over a wide neutron energy range and provide a large angular acceptance. A compact ³He neutron spin filter system has been developed for the Multi-Axis Crystal Spectrometer at the National Institute of Standards and Technology (NIST) Center for Neutron Research. Sealed ³He cells, polarized by spin-exchange optical pumping, are used as polarizer and analyzer. The polarization of the neutrons incident on the sample is inverted by flipping the polarization of the ³He gas in the polarizer, with only a small effect on the analyzer cells. The cell fabrication process, ³He spin flipper, and the holding magnetic field are discussed and we present the results of a first on-linetest.     

Solid-state NMR investigations of Si-29 and N-15 enriched silicon nitride

We compare ²⁹Si magic-angle spinning (MAS) nuclear magnetic resonance (NMR) spectra from the two modifications of silicon nitride, α-Si₃N₄ and β-Si₃N₄, with that of a fully (²⁹Si, ¹⁵N)-enriched sample ²⁹Si₃¹⁵N₄, as well as ¹⁵N NMR spectra of Si₃¹⁵N₄ (having ²⁹Si at natural abundance) and ²⁹Si₃¹⁵N₄. We show that the ¹⁵N NMR peak-widths from the latter are dominated by J(²⁹Si–¹⁵N) through-bond interactions, leading to significantly broader NMR signals compared to those of Si₃¹⁵N₄. By fitting calculated ²⁹Si NMR spectra to experimental ones, we obtained an estimated coupling constant J(²⁹Si–¹⁵N) of 20 Hz. We provide ²⁹Si spin-lattice (T₁) relaxation data for the ²⁹Si₃¹⁵N₄ sample and chemical shift anisotropy results for the ²⁹Si site of β-Si₃N₄. Various factors potentially contributing to the ²⁹Si and ¹⁵N NMR peak-widths of the various silicon nitride specimens are discussed. We also provide powder X-ray diffraction (XRD) and mass spectrometry data of the samples.     

129Xe NMR – highly polarized thin films

We studied the macroscopic effects of nuclear magnetization. Highly polarized xenon is often used to increase the sensitivity in NMR investigations of porous media, diluted liquids or for imaging in the gas phase. In the condensed phase, however, highly nuclear spin polarized xenon also possesses a sizable magnetization due to the nuclear spin density. This results in an additional magnetic field, that is used to measure the polarization of the sample, when only the particle density is known. Here we find P_z≈0.8 corresponding to a spin temperature of 0.5 mK. We use isotopically enriched xenon with a ¹²⁹Xe abundance of 0.71. At high abundance of ¹²⁹Xe and high nuclear polarization the dipolar linewidth is considerably reduced. We find for small angle excitation a reduction from 650 Hz to 400 Hz. We investigate this using a thin film geometry. The susceptibility effects of the substrate and the Xe film are treated. The macroscopic angle between the normal of the film and the external field strongly changes the polarization induced line shift and line width. The first follows an expected cos²θ dependence with an understood amplitude the latter however is not understood up to now. Relaxation of ¹²⁹Xe in the condensed film is observed to be T₁=15±1.8 min, much faster than expected. To cite this article: P. Gerhard et al., C. R. Physique 5 (2004).     

Polarization of Luminescence in the Nanostructure Si/CaF<Subscript>2</Subscript> Upon Polarization of the Nuclear Spins of Fluorine

The laws governing polarization of luminescence in the nanostructure Si/CaF₂ upon polarization of the spins of the fluorine nuclei by means of optical excitation of charge carriers are considered theoretically. The possibility of studying experimentally the properties of nuclear spins in analyzing luminescence is shown. The polarization of luminescence is most informative in the range of excitation rates of charge carriers from 3⋅10⁷ to 3⋅ 10⁸ sec⁻¹ with the CaF₂ layer of thickness from 0.6 to 0.8 nm and optical excitation polarization degree of 0.1. __________ Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 72, No. 4, pp. 524–529, July–August, 2005.     

Imaging of laser-polarized solid xenon

The enhanced spin polarization produced by optical pumping of gaseous rubidium/xenon samples has made possible a number of recent experiments in nuclear magnetic resonance (NMR) spectroscopy and magnetic resonance imaging (MRI). Here we report MRI of laser-polarized xenon in the solid phase at low temperature. Due to the high xenon density in the solid phase and the enhanced spin polarization, it is possible to achieve high intensity and spatial resolution of the image. Signals were observed from xenon films solidified onto the glass container walls and not from an enclosed chili pepper.     

Resonant-Optical Detection of Nuclear Magnetization in the Si/CaF<Subscript>2</Subscript> Nanostructure

We have considered theoretically the characteristic features of optical detection of nuclear magnetization in the Si/CaF₂ structure under the conditions of EPR and NMR by measuring luminescence polarization. We show that application of EPR makes it possible to detect weak nuclear fields, but the time of spin relaxation of electrons imposes its constraint. The application of NMR is limited by nuclear fields of no less than 15–20 Gs. The possibility of using optical NMR for direct measurement of the nuclear field from changes in the luminescence polarization spectrum is shown. __________ Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 72, No. 5, pp. 644–649, September–October, 2005.     

Spin Polarization of Fluorine Nuclei in the Si/CaF<Subscript>2</Subscript> Nanostructure Under Optical Excitation

The laws of fluorine nuclear spin polarization in the Si/CaF₂ nanostructure under optical excitation of the charge carriers in it has been considered theoretically. It has been shown that maximum values (up to 3% of the concentration of nuclei in the lattice) are attained under a high rate of optical excitation (>10⁻⁹ sec⁻¹) when the nuclear spin diffusion process and the Auger recombination prevail. In this case, the nuclear relaxation time in an individual layer reaches 100–300 sec and the spin diffusion radius decreases to 0.3 nm. __________ Translated from Zhurnal Prikladnoi Spektroskopii, Vol. 72, No. 3, pp. 397–403, May–June, 2005.     

Production of nitrogen-free, hyperpolarized 129Xe gas

129 Xe with a nuclear polarization far above the thermal equilibrium value (hyperpolarized) is used in NMR studies to increase sensitivity. Gaseous, adsorbed, or dissolved xenon is utilized in physical, chemical, and medical applications. With the aim in mind to study single-crystal surfaces by NMR of adsorbed hyperpolarized ¹²⁹Xe, three problems have to be solved. The reliable production of ¹²⁹Xe with highest nuclear polarization possible, the separation of the xenon gas from the necessary quench gas nitrogen without polarization loss, and the dosing/delivery of small amounts of polarized xenon gas to a sample surface. Here we describe an optical pumping setup that regularly produces xenon gas with a ¹²⁹Xe nuclear polarization of 0.7(±0.07). We show that a freeze–pump–thaw separation of xenon and nitrogen is feasible without a significant loss in xenon polarization. The nitrogen partial pressure can be suppressed by a factor of 400 in a single separation cycle. Dosing is achieved by using the low vapor pressure of a frozen hyperpolarized xenon sample. Received: 12 June 1998     

Measurement of the neutron beam polarization of BL05/NOP beamline at J-PARC

We measured the neutron beam polarization of the BL05/NOP (Neutron Optics and Physics) beamline at J-PARC with an accuracy of less than 10⁻³ using polarized ³He gas as a neutron spin analyzer. Precise polarimetry of the neutron beam is necessary to understand the beamline optics as well as for the asymmetry measurements of the neutron beta decay, which are planned in this beamline.     

Critical factors in obtaining meaningful fast MAS NMR spectra of non-integral spin quadrupolar nuclei. A review with particular emphasis on27Al MAS NMR of catalysts and minerals

In the last decade, magic angle spinning (MAS) NMR has become an extremely important method for studying the structure of inorganic solids. Advances in NMR technology have greatly aided in understanding the structure of catalysts, minerals, clays, ceramics, glasses, etc. Obtaining meaningful MAS spectra of spin-1/2 nuclei such as²⁹Si and³¹P is relatively straightforward and well understood. In contrast, obtaining meaningful MAS spectra is far from simple with non-integral spin quadrupolar nuclei such as¹¹B (I=3/2),¹⁷O (I=5/2),²³Na (I=3/2),²⁷Al (I=5/2),⁶⁹Ga (I=3/2), and⁷¹Ga (I=3/2)?to name some of the most commonly studied nuclei. Many additional factors have to be considered. This paper will deal with these factors and the utility of very fast MAS for studying non-integral spin quadrupolar nuclei in inorganic solids.     

Isotopically engineered Si and Ge for spintronics and quantum computation

Si, Ge as well as SiGe structures are the promising materials for spintronics and quantum computation due to the fact that in both crystals only one isotope (²⁹Si and ⁷³Ge) has nuclear spin. As a result, isotope engineering of Si and Ge permits to control the density of nuclear spins and vary the spin coherence time, a crucial parameter in spintronics. In the first part we discuss the NMR study of nuclear spin decoherence in Ge single crystals with different abundance of the ⁷³Ge isotope. It was observed that the slow component of the dephasing process is elongated with depletion of Ge crystal with isotope ⁷³Ge. The second part is devoted to the development of the Kane's model of nuclear spin-based quantum computer, which uses the nuclear spin of ³¹P impurity atoms in a ²⁸Si matrix as quantum bits (qubits). We discuss a new method of placing ³¹P atoms in a ²⁸Si based on neutron-transmutation-doping of isotopically engineered Si and Ge. In the proposed structure, interqubit coupling is due to indirect hyperfine interaction of ³¹P nuclear spins with electrons localized in a ²⁸Si quasi-one-dimensional nanowire, which allows one to control the coupling between distant qubits.     

2D CP/MASC Isotropic Chemical Shift Correlation Established byH Spin Diffusion

A new 2D solid-state CP/MAS¹³C NMR exchange experiment for through-space isotropic chemical shift correlation is proposed and demonstrated. Through-space correlation is established via a second cross polarization from¹³C to¹H and subsequent¹H spin diffusion. A third cross polarization results in the final¹³C–¹³C isotropic chemical shift correlation. The¹H spin diffusion time is a variable parameter allowing different mean square magnetization displacements to be probed. Experimental results on mixtures of differently¹³C-labeled alanine and polyethylene indicate that this site-selective 2D technique can be used to characterize domain sizes and proximities over a wide range of length scales (1–200 nm) in solids such as polymers or biological materials.     

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 P_Xe = 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.     

Temperature Dependence of the Magnetic Hyperfine Field at 140Ce on Gd Sites in GdAg Compound

Perturbed gamma–gamma angular correlation technique was used to measure the magnetic hyperfine field at Gd sites in the intermetallic compound GdAg using the ¹⁴⁰La→¹⁴⁰Ce nuclear probe. A major and well-defined magnetic interaction is observed at ¹⁴⁰Ce substituting Gd sites in GdAg below 130 K, corresponding to a ferromagnetic ordering of Gd moments. The temperature dependence of magnetic hyperfine field, however, shows a sharp deviation from an expected Brillouin-like behavior for temperatures below 75 K. This additional magnetic interaction is believed to result from the polarization of Ce spin moments induced by the magnetic field from Gd atoms.     

Control of the nuclear spin of the <Superscript>129</Superscript>Xe and <Superscript>131</Superscript>Xe isotopes in the spin-exchange interaction with <Superscript>87</Superscript>Rb atoms

Nuclear spin dynamics of the ¹²⁹Xe and ¹³¹Xe isotopes in an external magnetic field B ₀ is considered. Nuclear spin is pumped by the laser through ⁸⁷Rb, which transfers the electron spin to the ¹²⁹Xe and ¹³¹Xe nuclei in the spin-exchange interaction. The nuclear spin dynamics is controlled with a transverse magnetic field that causes nuclear magnetic resonance in both ¹²⁹Xe and ¹³¹Xe isotopes. Numerical calculations are performed to find conditions at which the transverse component of the nuclear spin in the established motion is of maximum and the slope angle relative to the vector of the constant magnetic field B ₀ is 45°. This regime is taken to be optimal for simulation of practical applications. It is also found that the pump of the nuclear spin of xenon is strongly attenuated when the rubidium polarization vector is turned to the plane perpendicular to the external magnetic field vector B ₀.     

Research on glass cells for He neutron spin filters

Glass cells play an important role in polarized ³He neutron spin filters. To evaluate the scattering and absorption contribution from glass cells during neutron scattering experiments, we measured small-angle scattering and neutron transmission in GE180 and other glasses. The small-angle neutron scattering measurements revealed that the glasses used for ³He spin filters have acceptably lower scattering: dΣ(Q)/dΩ=4-7×10⁻⁴ cm⁻¹ at Q=0.03-0.12 Å⁻¹. The transmission measurement was performed at J-PARC. Neutron transmission of about 92% through empty GE180 cells was observed over a wide wavelength range 0.014-7.0 Å. To pursue the possibility of being a structural influence on ³He spin relaxation in GE180 glass cells, we performed precise X-ray diffraction measurement using synchrotron radiation at SPring-8. From these measurements, a structural difference was observed among GE180 glasses with different thermal treatments.