Neutron Diffraction Measurements Research Articles

Absence of magnetic order in RuO2: insights from μSR spectroscopy and neutron diffraction

Altermagnets are a novel class of magnetic materials, where magnetic order is staggered both in coordinate and momentum space. The metallic rutile oxide RuO2, long believed to be a textbook Pauli paramagnet, recently emerged as a putative workhorse altermagnet when resonant X-ray and neutron scattering studies reported nonzero magnetic moments and long-range collinear order. While some experiments seem consistent with altermagnetism, magnetic order in RuO2 remains controversial. We show that RuO2 is nonmagnetic, both in bulk and thin film. Muon spectroscopy complemented by density-functional theory finds at most 1.14 × 10−4 μB/Ru in bulk and at most 7.5 × 10−4 μB/Ru in 11 nm epitaxial films, at our spectrometers’ detection limit, and dramatically smaller than previously reported neutron results that were used to rationalize altermagnetic behavior. Our own neutron diffraction measurements on RuO2 single crystals identify multiple scattering as the source for the false signal in earlier studies.

Dilution induced magnetic localization in Rb(Co[formula omitted]Ni[formula omitted])2Se2 single crystals

We report experimental studies on a series of Rb(Co1−xNix)2Se2 (0.02 ≤x≤ 0.9) powder and single crystal samples using x-ray diffraction, neutron diffraction, magnetic susceptibility, and electronic transport measurements. All compositions are metallic and adopt the body-centered tetragonal structure with I4/mmm space group. Anisotropic magnetic susceptibilities measured on single crystal samples suggest that Rb(Co1−xNix)2Se2 undergo an evolution from ferromagnetism to antiferromagnetism, and finally to paramagnetism with increasing Ni concentration. Neutron diffraction measurements on the samples with x = 0.1, 0.4, and 0.6 reveal an A-type antiferromagnetic order with moments lying in the ab plane. The moment size changes from 0.69 (x=0.1) to 2.80μB (x=0.6) per Co ions. Our results demonstrate that dilution of the magnetic Co ions by substitution of nonmagnetic Ni ions induces magnetic localization and evolution from itinerant to localized magnetism in Rb(Co1−xNix)2Se2.

Freezing of short-range ordered antiferromagnetic clusters in the CrFeTi2O7system.

We report on the CrFeTi2O7(CFTO) system using a combination of x-ray diffraction, dc magnetization, ac susceptibility, specific heat and neutron diffraction measurements. CFTO is seen to crystallize in a monoclinic P21/a symmetry. It shows a glassy freezing at Tf ~ 22 K, characterized by the observation of bifurcation between ZFC and FC χ (T) curves, frequency dispersion across Tf in ac susceptibility, and follows Vogel-Fulcher and power law type critical dynamics, very slow relaxation of iso-thermal remanent magnetization with time and the absence of an anomaly in the temperature dependence of specific heat measurements. The microscopic neutron diffraction analysis of CFTO not only confirms the absence of long-range antiferromagnetic ordering but also exhibits diffuse scattering due to the presence of short-range ordered antiferromagnetically correlated spin clusters.&#xD.

Tuning structural modulation and magnetic properties in metal-organic coordination polymers [CH3NH3]CoxNi1-x(HCOO)3.

Three solid solutions of [CH3NH3]CoxNi1-x(HCOO)3, with x = 0.25 (1), x = 0.50 (2) and x = 0.75 (3), were synthesized and their nuclear structures and magnetic properties were characterized using single-crystal neutron diffraction and magnetization measurements. At room temperature, all three compounds crystallize in the Pnma orthorhombic space group, akin to the cobalt and nickel end series members. On cooling, each compound undergoes a distinct series of structural transitions to modulated structures. Compound 1 exhibits a phase transition to a modulated structure analogous to the pure Ni compound [Cañadillas-Delgado, L., Mazzuca, L., Fabelo, O., Rodríguez-Carvajal, J. & Petricek, V. (2020). Inorg. Chem. 59, 17896-17905], whereas compound 3 maintains the behaviour observed in the pure Co compound reported previously [Canadillas-Delgado, L., Mazzuca, L., Fabelo, O., Rodriguez-Velamazan, J. A. & Rodriguez-Carvajal, J. (2019). IUCrJ, 6, 105-115], although in both cases the temperatures at which the phase transitions occur differ slightly from the pure phases. Monochromatic neutron diffraction measurements showed that the structural evolution of 2 diverges from that of either parent compound, with competing hydrogen bond interactions that drive the modulation throughout the series, producing a unique sequence of phases. It involves two modulated phases below 96 (3) and 59 (3) K, with different q vectors, similar to the pure Co compound (with modulated phases below 128 and 96 K); however, it maintains the modulated phase below magnetic order [at 22.5 (7) K], resembling the pure Ni compound (which presents magnetic order below 34 K), resulting in an improper modulated magnetic structure. Despite these large-scale structural changes, magnetometry data reveal that the bulk magnetic properties of these solid solutions form a linear continuum between the end members. Notably, doping of the metal site in these solid solutions allows for tuning of bulk magnetic properties, including magnetic ordering temperature, transition temperatures and the nature of nuclear phase transitions, through adjustment of metal ratios.

Magnetic ordering in the frustrated pyrochlore Yb2Ru2O7

Yb2Ru2O7 was studied using neutron diffraction and muon spin relaxation measurements to investigate the effect of the Yb anisotropy and Yb-Ru exchange interaction on the magnetic ordering transitions in this material. The Ru moments order into a long range ordered state below 85 K, while the Yb moments start to freeze/order below 20 K, which is at a higher temperature as suggested by previous reported bulk measurements. No structural distortions are observed at the magnetic transitions. Representational analysis shows that the ordering of the Ru and Yb moments can be described by the same irreducible representation. The two magnetic sublattices are, however, antiferromagnetically coupled. Unlike what has been suggested by bulk measurements and has been observed in other members of this family of Ru pyrochlores, the Yb single ion planar anisotropy, surprisingly, does not influence the Ru moment ordering. The ordering of the Ru moments, on the other hand, does influence freezing/ordering of the Yb moments.

Ferrimagnetic structure in the high-pressure phase of α−Mn

The α−Mn phase exhibits a large anomalous Hall effect (AHE) in its pressure-induced weak ferromagnetic (WFM) state, despite its relatively small spontaneous magnetization of ∼0.02μB/Mn. To understand the underlying mechanism behind this AHE, we performed single crystal neutron diffraction measurements at 2.0 GPa to determine the magnetic structure of the WFM phase. Our investigation reveals a ferrimagnetic structure characterized by nearly collinear magnetic moments aligned along the [001] direction at sites I, II, III-1, and IV-1. In contrast, the small moments at sites III-2 and IV-2 lie within the (001) plane. The calculated net magnetization of this magnetic structure, (−0.08±0.10)μB/Mn atom, is in agreement with the experimentally determined spontaneous magnetization. The observation of a magnetic reflection at q=(0,0,0) satisfies a key condition for the emergence of the AHE. Published by the American Physical Society 2024

Finite element modeling of thermal residual stresses in functionally graded aluminum-matrix composites using X-ray micro-computed tomography

Metal-ceramic composites by their nature have thermal residual stresses at the micro-level, which can compromise the integrity of structural elements made from these materials. The evaluation of thermal residual stresses is therefore of continuing research interest both experimentally and by modeling. In this study, two functionally graded aluminum alloy matrix composites, AlSi12/Al2O3 and AlSi12/SiC, each consisting of three composite layers with a stepwise gradient of ceramic content (10, 20, 30 vol%), were produced by powder metallurgy. Thermal residual stresses in the AlSi12 matrix and the ceramic reinforcement of the ungraded and graded composites were measured by neutron diffraction. Based on the X-ray micro-computed tomography (micro-XCT) images of the actual microstructure, a series of finite element models were developed to simulate the thermal residual stresses in the AlSi12 matrix and the reinforcing ceramics Al2O3 and SiC. The accuracy of the numerical predictions is high for all cases considered, with a difference of less than 5 % from the neutron diffraction measurements. It is shown numerically and validated by neutron diffraction data that the average residual stresses in the graded AlSi12/Al2O3 and AlSi12/SiC composites are lower than in the corresponding ungraded composites, which may be advantageous for engineering applications.

Phase analysis of near equiatomic bulk FeRh alloys: X-ray versus neutron diffraction and magnetization measurements

The information obtained by X-ray diffraction (XRD) by impinging the X-ray beam onto the flat surface of bulk Fe–Rh alloys is contrasted with that provided by the thermomagnetic analysis curves measured under a magnetic field of 5 mT and 2 T, and the neutron diffraction (ND) patterns. The experiments were performed on slices cut from bulk Fe50Rh50 and Fe49Rh51 alloys prepared by induction melting followed by 48 h of thermal annealing at 1273 K. Whereas ND patterns and magnetization curves, directly and indirectly point out that the samples are single-phase with a CsCl-type crystal structure undergoing a magnetoelastic transition that changes the magnetic structure from antiferromagnetic to ferromagnetic on heating, multiple phases are identified in the XRD patterns, which modify upon polishing or etching the surface with a mixture of hydrochloric (HCl) and nitric acid (HNO3) at a volume ratio of 90:10 from 30 to 210 min. The limitation of XRD for accurately characterizing the phase constitution within the bulk of Fe–Rh alloys is underlined.

Neutron diffraction analysis of microstructural evolution and mechanical behavior in an additively manufactured multiphase alloy

Abstract Additive manufacturing (AM) involves an unprecedented thermal history during solidification and post-melt high-temperature exposure, leading to unique microstructural evolution. In this study, we employed neutron-diffraction-based microstructural analysis to better understand the microstructural evolution and mechanical behavior of AM alloys, with a particular focus on multiphase alloys. Samples of Ti−6Al−4V alloy used as a model material were prepared using electron beam powder bed fusion (EB-PBF) under varying building conditions. Time-of-flight neutron diffraction (TOF-ND) measurements were performed using an iMATERIA (BL20), J-PARC, Japan. Using Rietveld texture analysis (RTA), we revealed the textural evolution during hierarchical microstructural development from solidification to solid-state phase transformations in the EB-PBF process. The effects of building conditions on the textures in the as-built states and their evolution during subsequent tensile loading were analyzed.

Pearlite Growth Kinetics in Fe-C-Mn Eutectoid Steels: Quantitative Evaluation of Energy Dissipation at Pearlite Growth Front Via Experimental Approaches

Essential understanding of the pearlite growth kinetics is of great significance to predict the lamellar spacing and the resultant mechanical properties of pearlitic steels. In this study, a series of eutectoid steels with Mn addition up to 2 mass pct were isothermally transformed at various temperatures from 873 K to 973 K to clarify the pearlite growth kinetics and the underlying thermodynamics at its growth front. The microscopic observation indicates the acceleration in pearlite growth rate and refinement in lamellar spacing by decreasing the transformation temperature or the amount of Mn addition. After analyzing the solute distribution at pearlite growth front via three-dimensional atom probe, no macroscopic Mn partitioning across pearlite/austenite interface is detected, whereas Mn segregation is only observed at ferrite/austenite interface. Furthermore, in-situ neutron diffraction measurements performed at elevated temperatures reveal that the magnitude of elastic strain generated during pearlite transformation is very small. Based on the thermodynamic model, these experimental results are used to estimate the contribution of various factors to the total energy dissipation. Compared with the Mn-free alloy, the retardation effect of Mn addition on pearlite growth kinetics, which is partly due to the reduced driving force for pearlite growth, can be well explained by further considering the solute drag effect of Mn.

Chemical pressure induced spin reorientation in the magnetic structure of Ca3Mn2−xSnxO7 ( x=0,0.03,0.05 )

The effect of partially substituting Tin (Sn) at the Manganese (Mn) site of Ca3Mn2O7 , viz. Ca3Mn2−xSnxO7 with x=0.03,0.05 , on its structural and magnetic properties have been investigated using synchrotron diffraction, neutron diffraction, and bulk magnetization measurements. It is observed that with a substitution of x=0.03 , the minor (≈8%) tetragonal ( I4/mmm ) structural phase that is present in the predominantly orthorhombic ( Cmc21 ) undoped Ca3Mn2O7 , completely disappears. The compounds order antiferromagnetically, the ordering temperature decreases with increasing Sn-content, indicating a weakening of the antiferromagnetic exchange interactions. Interestingly, in the ordered state, the spin magnetic moments which were aligned along the a-axis of the unit cell in the undoped compound, are observed to have reoriented with their major components lying in the b − c plane in the Sn-doped compounds. The above influence of Sn-doping is seen to be stemming from a significant modification of the octahedral rotation and tilt mode geometry in the unit cell, that is known to be responsible for driving ferroelectricity in these compounds.

Giant Room-Temperature Topological Hall Effect in a Square-Net Ferromagnet LaMn2Ge2.

A topological magnetic material showcases a multitude of intriguing properties resulting from the compelling interplay between topology and magnetism. These include notable phenomena such as a large anomalous Nernst effect (ANE), an anomalous Hall effect (AHE), and a topological Hall effect (THE). In most cases, topological transport phenomena are prevalent at temperatures considerably lower than room temperature, presenting a challenge for practical applications. However, the noncollinear ferromagnetic (FM) LaMn2Ge2, characterized by a Mn square-net lattice and a notably high Curie temperature (TC) of approximately 325 K, defies this trend as a topological semimetal. This work observes a giant topological Hall resistivity, , of ≈4.5 µΩ cm at room temperature when the angle between the applied field and the c-axis is 75°, which is significantly higher than state-of-the-art materials with noncoplanar spin structures. The single crystal neutron diffraction measurements agree with an incommensurate conical magnetic structure as the ground state. This observation suggests the enhanced spin chirality resulting from the noncoplanar spin configuration when the applied field is away from the magnetic easy axis as the origin of a large contribution to the observed THE. The findings unequivocally demonstrate that the FM LaMn2Ge2 holds great promise as a potential topological semimetal for spintronic applications even at room temperature.

Strong interlayer magnetic exchange coupling in La3Ni2O7−δ revealed by inelastic neutron scattering

After several decades of studies of high-temperature superconductivity, there is no compelling theory for the mechanism yet; however, the spin fluctuations have been widely believed to play a crucial role in forming the superconducting Cooper pairs. The recent discovery of high-temperature superconductivity near 80 K in the bilayer nickelate La3Ni2O7 under pressure provides a new platform to elucidate the origins of high-temperature superconductivity. We perform elastic and inelastic neutron scattering studies on a polycrystalline sample of La3Ni2O7−δ at ambient pressure. No magnetic order can be identified down to 10 K. The absence of long-range magnetic order in neutron diffraction measurements may be ascribed to the smallness of the magnetic moment. However, we observe a weak flat spin-fluctuation signal in the inelastic scattering spectra at ∼ 45 meV. The observed spin excitations could be interpreted as a result of strong interlayer and weak intralayer magnetic couplings for stripe-type antiferromagnetic orders. Our results provide crucial information on the spin dynamics and are thus important for understanding the superconductivity in La3Ni2O7.

Single-crystal neutron diffraction study on the Ho13.6Au61.1Al25.3 quasicrystal approximant

A single-crystal neutron diffraction study was conducted on a Ho13.6Au61.1Al25.3 Tsai-type quasicrystal approximant synthesised by the self-flux method. The magnetisation measurements reveal a ferrimagnetic behaviour with a transition below 6 K. In agreement with the magnetometry data, a non-coplanar whirling spin order in the icosahedral clusters around the crystallographic [1 1 1] direction with a ferrimagnetic arrangement was observed from single-crystal neutron diffraction measurements below 5.5 K. The magnetic structure of Ho13.6Au61.1Al25.3 is compared to the previously published magnetic structures of related RE-Au-SM (RE = Tb and Ho; SM = Al, Si and Ga) systems.

Neutron Diffraction Measurements of Residual Stresses for Ferritic Steel Specimens over 80 mm Thick

The maximum thickness for ferritic steel specimens’ residual stress measurements using neutron diffraction is known to be about 80 mm. This paper proposes a new neutron diffraction configuration of residual stress measurements for cases that are over 80 mm thick. The configuration utilizes a neutron beam with a wavelength of 1.55 Å diffracted from the (220) plane with a diffraction angle (2θ) of 99.4°. The reason for the deep penetration capability is attributed to the chosen wavelength having enough intensities due to the low cross-section near the Bragg edge and the reduced beam path length (~16 mm) reflected by the large diffraction angle. Neutron diffraction experiments with this configuration can decrease strain errors up to ±150 με, corresponding to a stress of about ±30 MPa.

Magnetic order in holmium and erbium formate: Parent frameworks for a potential random spin chain paramagnet

This work uses a combination of neutron diffraction and bulk property measurements to establish the low temperature magnetic states in the dense metal-organic frameworks Ho(HCO2)3 and Er(HCO2)3; whose structures feature chains of face-sharing LnO9 polyhedra packed into a triangular lattice. Below 0.7 K Ho(HCO2)3 is found to adopt a state in which the magnetic moment on its ferromagnetic chains vary from neighbouring chains but the sum around each triangle is constant. Er(HCO2)3 is found to be the first lanthanide formate to adopt an ordered magnetic state with antiferromagnetic coupling within its chains near 50 mK. The potential to combine the ferromagnetic and antiferromagnetic coupling within chains associated with Ho and Er cations, respectively, in the same compound has also been explored via the series Ho1-xErx(HCO2)3. Ho0.5Er0.5(HCO2)3 remains paramagnetic to 0.4 K, suggesting it may be a starting point to search for a random spin chain paramagnet.

Long-range magnetic order in CePdAl3 enabled by orthorhombic deformation

We investigate the effect of structural deformation on the magnetic properties of orthorhombic CePdAl3 in relation to its tetragonal polymorph. Utilizing x-ray and neutron diffraction, we establish that the crystal structure has the Cmcm space-group symmetry and exhibits pseudotetragonal twinning. According to density functional calculations, the tetragonal-orthorhombic deformation mechanism has its grounds in the relatively small free enthalpy difference between the polymorphs, allowing either phase to be quenched, and fully accounts for the twinned microstructure of the orthorhombic phase. Neutron diffraction measurements show that orthorhombic CePdAl3 establishes long-range magnetic order below TN=5.29(5) K characterized by a collinear, antiferromagnetic arrangement of magnetic moments. Magnetic anisotropies of orthorhombic CePdAl3 arise from strong spin-orbit coupling as evidenced by the crystal-field splitting of the 4f multiplet, fully characterised with neutron spectroscopy. We discuss the potential mechanism of frustration posed by antiferromagnetic interactions between nearest neighbors in the tetragonal phase, which hinders the formation of long-range magnetic order in tetragonal CePdAl3. We propose that orthorhombic deformation releases the frustration and allows for long-range magnetic order. Published by the American Physical Society 2024

Stroboscopic time-of-flight neutron diffraction in long pulsed magnetic fields

We present proof-of-principle experiments of stroboscopic time-of-flight (TOF) neutron diffraction in long pulsed magnetic fields. By utilizing electric double-layer capacitors, we developed a long pulsed magnet for neutron diffraction measurements, which generates pulsed magnetic fields with the full widths at half maximum of >102 ms. The field variation is slow enough to be approximated as a steady field within the time scale of a polychromatic neutron pulse passing through a sample placed in a distance of the order of 101 m from the neutron source. This enables us to efficiently explore the reciprocal space using a wide range of neutron wavelength in high magnetic fields. We applied this technique to investigate field-induced magnetic phases in the triangular lattice antiferromagnets CuFe1−xGaxO2 (x=0,0.035). Published by the American Physical Society 2024

Noncentrosymmetric Triangular Magnet CaMnTeO6: Strong Quantum Fluctuations and Role of s0 versus s2 Electronic States in Competing Exchange Interactions.

Noncentrosymmetric triangular magnets offer a unique platform for realizing strong quantum fluctuations. However, designing these quantum materials remains an open challenge attributable to a knowledge gap in the tunability of competing exchange interactions at the atomic level. Here, a new noncentrosymmetric triangular S=3/2 magnet CaMnTeO6 is created based on careful chemical and physical considerations. The model material displays competing magnetic interactions and features nonlinear optical responses with the capability of generating coherent photons. The incommensurate magnetic ground state of CaMnTeO6 with an unusually large spin rotation angle of 127°(1) indicates that the anisotropic interlayer exchange is strong and competing with the isotropic interlayer Heisenberg interaction. The moment of 1.39(1)µB, extracted from low-temperature heat capacity and neutron diffraction measurements, is only 46% of the expected value of the static moment 3µB. This reduction indicates the presence of strong quantum fluctuations in the half-integer spin S=3/2 CaMnTeO6 magnet, which is rare. By comparing the spin-polarized band structure, chemical bonding, and physical properties of AMnTeO6 (A=Ca, Sr, Pb), how quantum-chemical interpretation can illuminate insights into the fundamentals of magnetic exchange interactions, providing a powerful tool for modulating spin dynamics with atomically precise control is demonstrated.

Real-time evolution of texture and temperature during friction stir processing of a magnesium alloy: An operando neutron diffraction study

The real-time development of texture and the evolution of temperature during friction stir processing (FSP) of a Mg alloy were investigated using an operando neutron diffraction measurement. A novel approach was applied in this study where the real-time, quasi-steady state measurements performed as a function of position during FSP are converted to a Lagrangian dataset that reveals the transient behavior as a function of time. The in-situ FSP was carried out under two different thermo-mechanical processing conditions represented by the Zener-Hollomon parameter, Z. The results show that: (i) a shear texture develops from the initial strong basal texture with the peak temperature reaching about 774 K during a low-Z processing and (ii) a strong off-normal texture develops with a peak temperature of 616 K during a high-Z processing. Moreover, time-temperature-texture diagrams were established to reveal the real-time development of the texture during the processing for both the low Z and high Z processing conditions. The changes in texture will be discussed in terms of plastic deformation mechanisms active during various stages of the FSP under the two different processing conditions.