Neutron Polarization Analysis Research Articles

Wide-angle neutron polarisation analysis to study energy and quantum materials

Neutron sources have an important role to play in the development of new materials for storing sustainable energy, allowing researchers to gain deeper insights into their functionality. We spoke to Professor Elizabeth Blackburn about how she and her team are using neutron scattering techniques to investigate energy and quantum materials.

Design, calibration, and performance of a uniaxial pressure cell for neutron scattering studies of quantum magnetism.

We provide an overview of a pressure cell designed to apply uniaxial pressure to single crystals for the study, by neutron scattering techniques, of strongly correlated magnetic systems and, in particular, quantum magnets. A detailed overview of the pressure cell components, their requirements, and links to the scientific and technical specifications are presented. The pressure cell is able to accommodate a 200 mm3 single crystal that can be pressurized up to 2GPa at cryogenic temperatures. The pressure cell is consistent with the requirements of inelastic neutron scattering and, importantly, neutron polarization analysis. A particular strength of the uniaxial pressure cell is the highly uniform and low background for a wide scattering angle of 360° horizontally and ±20° vertically. We show the performance of the uniaxial pressure cell using a relevant neutron scattering instrument, the polarized diffuse scattering instrument, D7. The experiments confirm that the cell complies with the scientific and technical requirements. This uniaxial pressure cell will provide a useful additional tool in the sample environment suite available for the study of quantum magnetism.

Neutron polarization analysis of the anisotropic spin wave excitations in multiferroic BiFeO3

A multiferroic material BiFeO3 shows a cycloidal spin structure below 640 K. Anisotropy of the magnetic excitations below 6 meV was previously studied using neutron polarization analysis (Zhang et al. 2022 Phys. Rev. B 105 144426). The magnetic excitations in and out of the cycloidal plane were separated and compared to those calculated based on the linear spin-wave theory. The overall feature of the observed excitations was found to be consistent with those calculated. Further polarized neutron study with extended energy range has been performed. The anisotropy of the magnetic excitations is present at least up to 15 meV. The out-of-plane mode is constantly more intense by ∼50% than the in-plane mode in the energy range between 3 and 15 meV. The anisotropic excitations in the wide energy range are unexpected since multiple in-plane and out-of-plane modes are mixed at higher energies and the excitations are expected to become more isotropic.

Magnetic pair distribution function data using polarized neutrons and ad hoc corrections

We report the first example of magnetic pair distribution function (mPDF) data obtained through the use of neutron polarization analysis. Using the antiferromagnetic semiconductor MnTe as a test case, we present high-quality mPDF data collected on the HYSPEC instrument at the Spallation Neutron Source using longitudinal polarization analysis to isolate the magnetic scattering cross section. Clean mPDF patterns are obtained for MnTe in both the magnetically ordered state and the correlated paramagnet state, where only short-range magnetic order is present. We also demonstrate significant improvement in the quality of high-resolution mPDF data through the application of ad hoc corrections that require only minimal human input, minimizing potential sources of error in the data processing procedure. We briefly discuss the current limitations and future outlook of mPDF analysis using polarized neutrons. Overall, this work provides a useful benchmark for mPDF analysis using polarized neutrons and provides an encouraging picture of the potential for routine collection of high-quality mPDF data.

Anisotropic spin-wave excitations in multiferroic BiFeO3

Polarized inelastic neutron-scattering experiments have been performed to elucidate the anisotropic behavior of the low-energy spin-wave excitations in a multiferroic ${\mathrm{BiFeO}}_{3}$, which shows a cycloidal spin structure below 640 K. Using neutron polarization analysis for single magnetic domain crystals, magnetic excitation modes in and out of the cycloidal plane below 6 meV were separated successfully. The magnetic excitation spectra were analyzed using linear spin-wave theory. The low-energy magnon density of states consist of several magnon modes, including the two anisotropic modes, $\mathrm{\ensuremath{\Phi}}$ and $\mathrm{\ensuremath{\Psi}}$ modes, distributed in and out of the cycloidal plane, respectively, which were previously observed using optical spectroscopies. Furthermore, there are other magnon modes that are not active in optical measurements. A model spin Hamiltonian, which reproduces the spin-wave frequencies observed using optical spectroscopies, explains the overall spectra reasonably well.

Development of a Spin-Exchange Optical Pumping-Based Polarized 3He System at the China Spallation Neutron Source (CSNS)Supported by the National Key Research and Development Program of China (Grant No. 2020YFA0406000), the National Natural Science Foundation of China (Grant No. 11875265), the Scientific Instrument Developing Project of the Chinese Academy of Sciences (Grant No. 284(2018)), Guangdong Basic and Applied Basic Research Foundation

Polarized 3He neutron spin filters (NSFs) can be used as a vital tool for neutron polarization production and analysis. The China Spallation Neutron Source (CSNS), as one of the major neutron facilities in China, has committed resources to the development of a polarized 3He NSF program to support its growing polarized neutron research. A spin-exchange optical pumping (SEOP)-based polarized 3He system and other necessary hardware for NSF transport has been recently developed. The performance of the system is benchmarked using an in-house developed cell named “Trident”. Neutron beam measurements yield a 3He polarization of 77% with over 200 h of on-beam relaxation time. Combining this newly developed SEOP system with the recently reported cell fabrication station, CSNS is now capable of the fully self-sustained production of 3He NSFs that shall support its future neutron polarization research.

Polarization analysis for small-angle neutron scattering with a 3He spin filter at a pulsed neutron source

Neutron polarization analysis (NPA) for small-angle neutron scattering (SANS) experiments using a pulsed neutron source was successfully achieved by applying a 3He spin filter as a spin analyzer for the neutrons scattered from the sample. The cell of the 3He spin filter gives a weak small-angle scattering intensity (background) and covers a sufficient solid angle for performing SANS experiments. The relaxation time of the 3He polarization is sufficient for continuous use for approximately 2 days, thus reaching the typical duration required for a complete set of SANS experiments. Although accurate evaluation of the incoherent neutron scattering, which is predominantly attributable to the extremely large incoherent scattering cross section of hydrogen atoms in samples, is difficult using calculations based on the sample elemental composition, the developed NPA approach with consideration of the influence of multiple neutron scattering enabled reliable decomposition of the SANS intensity distribution into the coherent and incoherent scattering components. To date, NPA has not been well established as a standard technique for SANS experiments at pulsed neutron sources such as the Japan Proton Accelerator Research Complex (J-PARC) and the US Spallation Neutron Source. It is anticipated that this work will contribute significantly to the accurate determination of the coherent neutron scattering component for scatterers in various types of organic sample systems in SANS experiments at J-PARC, particularly for systems involving competition between the coherent and incoherent scattering intensity.

In-plane uniaxial pressure-induced out-of-plane antiferromagnetic moment and critical fluctuations in BaFe2As2

A small in-plane external uniaxial pressure has been widely used as an effective method to acquire single domain iron pnictide BaFe2As2, which exhibits twin-domains without uniaxial strain below the tetragonal-to-orthorhombic structural (nematic) transition temperature Ts. Although it is generally assumed that such a pressure will not affect the intrinsic electronic/magnetic properties of the system, it is known to enhance the antiferromagnetic (AF) ordering temperature TN ( < Ts) and create in-plane resistivity anisotropy above Ts. Here we use neutron polarization analysis to show that such a strain on BaFe2As2 also induces a static or quasi-static out-of-plane (c-axis) AF order and its associated critical spin fluctuations near TN/Ts. Therefore, uniaxial pressure necessary to detwin single crystals of BaFe2As2 actually rotates the easy axis of the collinear AF order near TN/Ts, and such effects due to spin-orbit coupling must be taken into account to unveil the intrinsic electronic/magnetic properties of the system.

Polarization analysis on the LET cold neutron spectrometer using a 3He spin-filter: first results

We report on the design and construction of a neutron polarization analyzer based on a 3He spin filter for the LET spectrometer at the ISIS facility. Its commissioning completes the uniaxial polarized mode of the instrument. Besides the 3He spin filter cell, the analyzer consists of a set of electromagnetic coils to provide a uniform magnetic field, and a collimator to eliminate background from the sample environment and analyzer infrastructure. The 3He cell is separated from the LET main tank vacuum by means of a gas tank, which permits rapid cell changeovers and guarantees safe operation. In addition to the analyzer hardware, software has been written to reduce and correct polarized data. The successful operation of the polarized mode was realized for the separation of coherent and incoherent dynamics in an organic solar cell polymer blend.

Wide-angle polarization analysis on the multi-axis crystal spectrometer for the study of collective and single particle dynamics of methanol at its prepeak

Neutron polarization analysis capability with a large scattering angle and momentum transfer coverage has not been widely implemented for the separation of coherent and incoherent quasi-elastic neutron scattering (QENS) spectra. A feasibility test for soft condensed matter applications was performed on the Multi-Axis Crystal Spectrometer (MACS) at the NIST Center for Neutron Research (NCNR). This capability benefitted from the high flux wide angle polarization analysis capability recently developed on MACS for hard condensed matter investigations. The experimental procedure is thoroughly described on how to take data and perform polarization efficiency correction before further data analysis is done. This capability was employed to unambiguously separate the coherent and incoherent signal from the QENS spectra for the investigation of both the collective and the single particle dynamics in partially deuterated (CH3OD, D 99.5% purity) methanol. By studying a Q range encompassing the prepeak position, it was possible to directly measure the dynamics of the h-bonding associates which originate the prepeak signal, without contamination from the incoherent scattering, in spite of the relative weakness of the coherent scattering.

Quenching of Long Range Order and the Mn3+ Ordered Moment in the Layered Antiferromagnet, Ba xSr1- xLaMnO4. A Polarized Neutron Scattering Study.

SrLaMnO4 is a layered antiferromagnetic (AF) oxide with the tetragonal ( I4/ mmm) n = 1 Ruddlesden-Popper phase structure (also known as the K2NiF4 structure) with TN = 128 K. Remarkably, substitution of Sr2+ by Ba2+, forming the solid solution Ba1- xSr xLaMnO4, results in the destruction of long-range magnetic order and of the ordered moment on Mn3+ for x > 0.35, although the effective paramagnetic moment remains unchanged, an unprecedented behavior for this class of magnetic materials. Four members, x = 0.0, 0.25, 0.35, and 1.0, have been studied using XYZ neutron polarization analysis which permits isolation of the magnetic, nuclear and nuclear spin components of the scattering and the measurement of the absolute value of the magnetic cross section. Data analysis is done using model independent reverse Monte Carlo methods (SPINVERT). The results for x = 0.0 (SrLaMnO4), T > TN(128 K), show an asymmetric diffuse peak which evolves into resolution limited Bragg peaks below T N and a fully ordered AF ground state with a Mn3+ moment of 3.06 μB. For x = 0.25 the magnetic scattering below T N displays a remarkable phase separation-Bragg reflections coexisting with diffuse scattering. The ordered Mn3+ moment is 1.1 μB, much reduced from that obtained via unpolarized neutrons. There are no Bragg peaks for x = 0.35 at any measured temperature ( T > 3 K) but there is highly structured diffuse scattering indicating strong short-range order reminiscent of x = 0 and 0.25 above their respective transition temperatures. For x = 1.00 (BaLaMnO4) the diffuse scattering roughly follows a paramagnetic form-factor indicating no short or long-range magnetic correlations. It is argued that the observed phenomena are due to a competition between AF and ferromagnetic (F) superexchange interactions for the 180° Mn3+-O-Mn3+ geometry within the ab plane and that the changes in the local geometry of the Mn-O octahedron leads to reduction of the AF interaction with a likely enhancement of the F interaction with increasing Ba content, ultimately giving rise to a glassy ground state. Analysis of the diffuse magnetic components show clear 2D AF spin correlations above TN for x = 0.00, 0.25, and 0.35 with correlation lengths, ξ ∼ 14-7 Å and no spin correlations for x = 1.00.

Transverse and longitudinal spin-fluctuations in INVAR Fe0.65Ni0.35

The presence of spin-fluctuations deep within the ordered state of ferromagnetic alloy has long been suspected but seldom directly observed. Inhomogeneities of one type or another have been cited as important in stabilizing behaviour—either longitudinal spin-fluctuations associated with the -state (local environment) model or transverse magnetisation arising from non-collinear spin structures. In this study we employ small-angle neutron scattering with neutron polarization analysis to distinguish between the two possibilities. Surprisingly we in fact find evidence of dominant but uncorrelated longitudinal spin-fluctuations coexisting with transverse magnetisation which exists in short-range clusters of size ~. This finding supports recent first principles calculations of in which both longitudinal spin-fluctuations and magnetic short-range order are identified as important ingredients in reproducing the equilibrium lattice.

Polarized neutron scattering study of the multiple order parameter system NdB4

Neutron polarization analysis has been carried out in order to clarify the magnetic structures of multiple order parameter $f$-electron system ${\mathrm{NdB}}_{4}$. We confirmed the noncollinear ``all-in all-out'' structure (${\mathrm{\ensuremath{\Gamma}}}_{4}$) of the in-plane moment, which is in good agreement with our previous neutron powder diffraction study. We found that the magnetic moment along the $c$-axis ${m}_{c}$ showed diagonally antiferromagnetic structure (${\mathrm{\ensuremath{\Gamma}}}_{10}$), inconsistent with previously reported ``vortex'' structure (${\mathrm{\ensuremath{\Gamma}}}_{2}$). The microscopic mixture of these two structures with ${\stackrel{P\vec}{q}}_{0}=(0,0,0)$ appears in phase II and remains stable in phases III and IV, where an incommensurate modulation coexists. The unusual magnetic ordering is phenomenologically understood via Landau theory with the primary order parameter ${\mathrm{\ensuremath{\Gamma}}}_{4}$ coupled with higher-order secondary order parameter ${\mathrm{\ensuremath{\Gamma}}}_{10}$. The magnetic moments were estimated to be $1.8\ifmmode\pm\else\textpm\fi{}0.2$ and $0.2\ifmmode\pm\else\textpm\fi{}0.05{\ensuremath{\mu}}_{\mathrm{B}}$ at $T=7.5\phantom{\rule{0.16em}{0ex}}\mathrm{K}$ for ${\mathrm{\ensuremath{\Gamma}}}_{4}$ and ${\mathrm{\ensuremath{\Gamma}}}_{10}$, respectively. We also found a long-period incommensurate modulation of the ${\stackrel{P\vec}{q}}_{1}=(0,0,1/2$) antiferromagnetic structure of ${m}_{c}$ with the propagation ${\stackrel{P\vec}{q}}_{s1}\phantom{\rule{0.16em}{0ex}}=(0.14,0.14,0.1)$ and ${\stackrel{P\vec}{q}}_{s2}=(0.2,0,0.1)$ in phase III and IV, respectively. The amplitude of sinusoidal modulation was about ${m}_{c}=1.0\ifmmode\pm\else\textpm\fi{}0.2{\ensuremath{\mu}}_{\mathrm{B}}$ at $T=1.5$ K. The local ($0,0,1/2$) structure consists of in-plane ferromagnetic and out-of-plane antiferromagnetic coupling of ${m}_{c}$, opposite to the coexisting ${\mathrm{\ensuremath{\Gamma}}}_{10}$. The ${m}_{c}$ of ${\mathrm{\ensuremath{\Gamma}}}_{10}$ is significantly enhanced up to $0.6{\ensuremath{\mu}}_{\mathrm{B}}$ at $T=1.5$ K, which is accompanied by the incommensurate modulations. The Landau phenomenological approach indicates that the higher-order magnetic and/or multipole interactions based on the pseudoquartet $f$-electron state play important roles.

Magnetic ground state and magnon-phonon interaction in multiferroic h−YMnO3

Inelastic neutron scattering has been used to study the magneto-elastic excitations in the multiferroic manganite hexagonal YMnO$_3$. An avoided crossing is found between magnon and phonon modes close to the Brillouin zone boundary in the $(a,b)$-plane. Neutron polarization analysis reveals that this mode has mixed magnon-phonon character. An external magnetic field along the $c$-axis is observed to cause a linear field-induced splitting of one of the spin wave branches. A theoretical description is performed, using a Heisenberg model of localized spins, acoustic phonon modes and a magneto-elastic coupling via the single-ion magnetostriction. The model quantitatively reproduces the dispersion and intensities of all modes in the full Brillouin zone, describes the observed magnon-phonon hybridized modes, and quantifies the magneto-elastic coupling. The combined information, including the field-induced magnon splitting, allows us to exclude several of the earlier proposed models and point to the correct magnetic ground state symmetry, and provides an effective dynamic model relevant for the multiferroic hexagonal manganites.

A new magnetic field system for 3He polarization

The nuclear spin-polarized 3He gas has been in depth studied and widely used in various scientific experiments. The polarized 3He gas can be used as a polarized neutron target to study the reaction of neutrons with charged particles or photon beams. On the other hand, spin polarized 3He gas is a good probe for detecting the new interactions in the supernormal model, and has many other applications as follows:the spin-dependent interaction can be studied quantitatively by measuring the NMR frequency shift but the spin-dependent interaction can also be studied by measuring the relaxation time of polarized 3He gas; the polarized 3He gas can be applied to magnetometers and magnetic resonance imaging (MRI); the highly polarized 3He gas can be used as a neutron spin filter for neutron polarization and polarization analysis because of the high correlation between the absorption cross section of the neutron in polarized 3He nucleus and the spin orientation. At present, the three major domestic sources of neutron, CMRR, CARR, and CSNS, are used to study the neutron polarization and polarization analysis techniques based on spin polarized 3He gas. The longitudinal (or spin-lattice) relaxation time (i.e., T1) of 3He is a key parameter that limits the polarizability of 3He gas. In order to reduce the effect of magnetic field gradient on the longitudinal relaxation time of polarized 3He gas, large-sized Helmholtz coils are usually constructed to provide the main magnetic field where the uniformity in the magnetic field central region reaches 10-4 cm-1. To obtain enough magnetic field uniformity, some magnetic field systems even exceed 1.5 m in size. However, it is expected to have a small magnetic field configuration from the view of practicality and convenience. For the common size (3He cells, Merritt coil and Saddle coil can effectively reduce the size of the magnetic field apparatus. However, for electron scattering experiments of 3He cells, the chamber length can be 40 cm. The system length exceeds 1 m even by using the Merritt coil. In this work, a new six-coil system for 3He polarization is obtained. Within the coils, the magnetic field gradient satisfies the requirement that √|▽Bx|2+|▽By|2/B0 -4 cm-1 in more than 30% area, which is better than all the existing coils used in polarized 3He experiments and can be applied to the future 3He instruments. For other experiments that require magnetic field to have a large uniform area, the new six-coil system is also a good option.

Spin excitation anisotropy in the optimally isovalent-doped superconductor BaFe2(As0.7P0.3)2

We use neutron polarization analysis to study spin excitation anisotropy in the optimal-isovalent-doped superconductor BaFe2(As0.7P0.3)2 (Tc = 30 K). Different from optimally hole and electron-doped BaFe2As2, where there is a clear spin excitation anisotropy in the paramagnetic tetragonal state well above Tc, we find no spin excitation anisotropy for energies above 2 meV in the normal state of BaFe2(As0.7P0.3)2. Upon entering the superconducting state, significant spin excitation anisotropy develops at the antiferromagnetic (AF) zone center QAF = (1, 0, L = odd), while magnetic spectrum is isotropy at the zone boundary Q = (1, 0, L = even). By comparing temperature, wave vector, and polarization dependence of the spin excitation anisotropy in BaFe2(As0.7P0.3)2 and hole-doped Ba0.67K0.33Fe2As2 (Tc = 38 K), we conclude that such anisotropy arises from spin-orbit coupling and is associated with the nearby AF order and superconductivity.

Novel type of neutron polarization analysis using the multianalyzer-equipment of the three-axes spectrometer PUMA

The combination of polarization analysis and multianalyzer system available at the three axes spectrometer PUMA@FRM II allows the simultaneous determination of both spin states of the scattered neutrons and the absolute value of the polarization. The present paper describes the technical details along with the basic formalism used for the precise calibration. Moreover, the performance of this method is illustrated by several test experiments including first polarized inelastic studies of the magnetic excitations of CuO in the multiferroic and the uniaxial antiferromagnetic phases.

Spin excitation anisotropy in the paramagnetic tetragonal phase of BaFe2As2

We use neutron polarization analysis to study temperature dependence of the spin excitation anisotropy in BaFe$_2$As$_2$, which has a tetragonal-to-orthorhombic structural distortion at $T_s$ and antiferromagnetic (AF) phase transition at $T_N$ with ordered moments along the orthorhombic $a$-axis below $T_s\approx T_N\approx 136$ K. In the paramagnetic tetragonal state at 160 K, spin excitations are isotropic in spin space with $M_a=M_b=M_c$, where $M_a$, $M_b$, and $M_c$ are spin excitations polarized along the $a$, $b$, and $c$-axis directions of the orthorhombic lattice, respectively. On cooling towards $T_N$, significant spin excitation anisotropy with $M_a>M_b\approx M_c$ develops below 3 meV with a diverging $M_a$ at $T_N$. The in-plane spin excitation anisotropy in the tetragonal phase of BaFe$_2$As$_2$ is similar to those seen in the tetragonal phase of its electron and hole-doped superconductors, suggesting that spin excitation anisotropy is a direct probe of doping dependence of spin-orbit coupling and its connection to superconductivity in iron pnictides.

Recent on-beam tests of wide angle neutron polarization analysis with a 3He spin filter: Magic PASTIS on V20 at HZB

A complete XYZ polarization analysis solution is under development for the new thermal time of flight spectrometer TOPAS [1], to be operated in the coming east neutron guide hall at the MLZ. Polarization Analysis Studies on a Thermal Inelastic Spectrometer, commonly called PASTIS [2], is based on polarized 3He neutron spin filters and an XYZ field configuration for the sample environment and a polarization-preserving neutron guide field. The complete system was designed to provide adiabatic transport of the neutron polarization to the sample position while maintaining the homogeneity of the XYZ field. This system has now been tested on the polarized time-of-flight ESS test beam line V20 at HZB [3]. Down to the minimum wavelength of 1.6 Å on the instrument, the magnetic configuration worked ideally for neutron spin transport while giving full experimental freedom to change between the X, Y or Z field configuration. The 3He cell used was polarized at the 3He lab of the JCNS at the MLZ in Garching and transported to HZB in Berlin via car showing that such a transport is indeed feasible for such experiments. We present results of this test and the next steps forward.

Neutron multimonochromator-bipolarizer based on magnetic multilayer Fe/Co and new scheme for the total neutron polarization analysis

In this paper, we present a new neutron-optical element, Neutron Multimonochromator-Bipolarizer (NMB). It consists of a multimultilayer structure made of 12 periodic multilayer Fe/Co magnetic nanostructures whose period increases with distance from the substrate. Results are presented of calculations of the reflection coefficients from the NMB. We propose a new scheme of the total neutron polarization analysis for the time-of-flight method in the reflectometry. In this scheme, double NMB is used as a polarizer and there is no spin-flipper before the sample. NMB can be used in polarized neutron reflectometry, in SESANS, and for research of low-angle and inelastic scattering of polarized neutrons.