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Results for “Single crystal neutron diffraction”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Suppressed-moment 2-k order in the canonical frustrated antiferromagnet Gd 2 Ti 2 O 7

In partially ordered magnets, order and disorder coexist in the same magnetic phase, distinct from both spin liquids and spin solids. Here, we determine the nature of partial magnetic ordering in the canonical frustrated antiferromagnet Gd 2 Ti 2 O 7 , in which Gd 3+ spins occupy a pyrochlore lattice. Using single-crystal neutron-diffraction measurements in applied magnetic field, magnetic symmetry analysis, inelastic neutron-scattering measurements, and spin-wave modeling, we show that its low-temperature magnetic structure involves two propagation vectors (2-k structure) with suppressed ordered magnetic moments and enhanced spin-wave fluctuations. Our experimental results are consistent with theoretical predictions of thermal fluctuation-driven order in Gd 2 Ti 2 O 7 , and reveal that inelastic neutron-scattering measurements on powder samples can solve the longstanding problem of distinguishing single-k and multi-k magnetic structures.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Pressure‐Induced Structural and Magnetic Evolution in Layered Antiferromagnet YbMn 2 Sb 2

Electronic states under pressure exhibit unconventional spin and charge dynamics that provide a powerful route to uncover exotic phases in quantum materials. Here, we present the structural, magnetic, and electronic evolution of YbMn 2 Sb 2 under pressure. Single-crystal X-ray diffraction reveals a pressure-induced structural transition from the space group trigonal P$\overline{3}$m1 to the monoclinic P2 1 /m phase near 3.5 GPa, which remains stable up to 10 GPa. Magnetization measurements display an anomalously weak net magnetic moment and the absence of Curie–Weiss behavior up to 400 K, suggesting the formation of short-range Mn moment pairs that cancel macroscopically and subsequently evolve into long-range order upon cooling. Temperature-dependent resistivity shows semiconducting behavior with a transition at ∼119 K at ambient pressure, while pressure induces a dramatic suppression of resistance and the emergence of metallic-like temperature dependence, stabilized beyond 5 GPa. This pressure-driven semiconductor-metal transition is consistent with our density functional theory calculations, confirming the closing of the band gap under compression. Neutron diffraction under pressure identifies an incommensurate magnetic structure with antiparallel correlations between paired spins. Together, these results demonstrate how pressure-driven structural tuning and competing exchange interactions stabilize unconventional magnetic states in this low-dimensional magnetic semiconductor.

antiferromagnetic semiconductor↗
DOE OSTI2020

Isotropic parallel antiferromagnetism in the magnetic field induced charge-ordered state of $\mathrm{Sm Ru_4 P_{12}}$ caused by $p - f$ hybridization

Nature of the field-induced charge-ordered phase (phase II) of SmRu 4 P 12 has been investigated by resonant x-ray diffraction (RXD) and polarized neutron diffraction (PND), focusing on the relationship between the atomic displacements and the antiferromagnetic (AFM) moments of Sm. From the analysis of the interference between the nonresonant Thomson scattering and the resonant magnetic scattering, combined with the spectral function obtained from x-ray magnetic circular dichroism, it is shown that the AFM moment of Sm prefers to be parallel to the field (m AF ∥ H), giving rise to large and small moment sites around which the P 12 and Ru cage contract and expand, respectively. This is associated with the formation of the staggered ordering of the Γ 7 -like and Γ 8 -like crystal-field states, providing a strong piece of evidence for the charge order. PND was also performed to obtain complementary and unambiguous conclusion. In addition, isotropic and continuous nature of phase II is demonstrated by the field-direction invariance of the interference spectrum in RXD. Finally, crucial role of the p-f hybridization is shown by resonant soft x-ray diffraction at the P K edge (1s↔3p), where we detected a resonance due to the spin polarized 3p orbitals reflecting the AFM order of Sm.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Temperature-Dependent Structural Transition in Cu-Intercalated Trigonal CuYbSe 2

Rare-earth delafossites, ARCh 2 ; A = alkali metal, R = rare-earth, Ch = chalcogen which consist of intercalated rare-earth metal dichalcogenides, host frustrated triangular lattices that are fertile ground for exotic phenomena. In most cases, the triangular rare-earth sublattice arises from R-3m (No. 166) structures with three layers of rare-earth metal dichalcogenide octahedra or P6 3 /mmc (No. 194) structures with two such layers, analogous to those found in transition metal dichalcogenides. Substituting the alkali metal with Cu + yields a distinct trigonal crystal symmetry P-3m1 (No. 164) in these structures. This symmetry change alters the coordination environment from ASe 6 octahedra in R-3m AYbSe 2 to CuSe 4 tetrahedra in CuYbSe 2 , resulting in shortened rare-earth to rare-earth separations and significantly reduced interlayer distances. Using X-ray single-crystal diffraction, powder neutron diffraction, resistance, and specific heat measurements, a structural transition slightly below room temperature (258 K) is observed. The low-temperature structure is a lower-symmetry I2/m structure, accompanied by partial Cu-site vacancy ordering. The combination of Cu disorder and the triangular lattice geometry in CuYbSe 2 provides a promising platform for investigating frustrated magnetism and unconventional transport phenomena.

Chemical structure↗
DOE OSTI2019

Lattice disorder effect on magnetic ordering of iron arsenides

This study investigates magnetic ordering temperature in nano- and mesoscale structural features in an iron arsenide. Although magnetic ground states in quantum materials can be theoretically predicted from known crystal structures and chemical compositions, the ordering temperature is harder to pinpoint due to potential local lattice variations that calculations may not account for. In this work we find surprisingly that a locally disordered material can exhibit a significantly larger Néel temperature (T N ) than an ordered material of precisely the same chemical stoichiometry. Here, a EuFe 2 As 2 crystal, which is a ‘122’ parent of iron arsenide superconductors, is found through synthesis to have ordering below T N = 195 K (for the locally disordered crystal) or T N = 175 K (for the ordered crystal). In the higher T N crystals, there are shorter planar Fe-Fe bonds [2.7692(2) Å vs. 2.7745(3) Å], a randomized in-plane defect structure, and diffuse scattering along the [00 L] crystallographic direction that manifests as a rather broad specific heat peak. For the lower T N crystals, the a-lattice parameter is larger and the in-plane microscopic structure shows defect ordering along the antiphase boundaries, giving a larger T N and a higher superconducting temperature (T c ) upon the application of pressure. First-principles calculations find a strong interaction between c-axis strain and interlayer magnetic coupling, but little impact of planar strain on the magnetic order. Neutron single-crystal diffraction shows that the low-temperature magnetic phase transition due to localized Eu moments is not lattice or disorder sensitive, unlike the higher-temperature Fe sublattice ordering. This study demonstrates a higher magnetic ordering point arising from local disorder in 122.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Zero-field magnetic ground state of EuMg 2 Bi 2

Layered trigonal EuMg 2 Bi 2 is reported to be a topological semimetal that hosts multiple Dirac points that may be gapped or split by the onset of magnetic order. In this study, we report zero-field single-crystal neutron-diffraction and bulk magnetic susceptibility measurements versus temperature χ ( T ) of EuMg 2 Bi 2 that show the intraplane ordering is ferromagnetic ( Eu 2 + , S = 7 / 2 ) with the moments aligned in the a b plane while adjacent layers are aligned antiferromagnetically (i.e., A-type antiferromagnetism) below the Néel temperature.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Noncoplanar magnetic order in the breathing kagome lattice compound Pb⁡(OF)⁢Cu 3 ⁢(SeO 3 ) 2⁢ (NO 3 )

We report a comprehensive study investigating the magnetic ordering properties of the quasi-two-dimensional breathing kagome lattice compound Pb⁡(OF)⁢Cu 3 ⁢(SeO 3 ) 2 ⁢(NO 3 ) using neutron diffraction and thermodynamic measurements. A long-range magnetic order emerges below the Néel temperature, T N = 18K, characterized by a propagating vector k = (0,0,1.5). Refinement analysis reveals that the copper moments display a noncoplanar arrangement, with the c components parallelly aligned within the breathing kagome plane and antiparallelly aligned between the layers. In-plane moment components form a chiral “tail-chase” structure. The magnetic order is quickly suppressed under moderate external fields applied both within and perpendicular to the kagome plane. Potential magnetic interactions that may be associated with the noncoplanar chiral magnetic structure are discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Single-Crystal Diffuse Neutron Scattering Study of the Dipole-Octupole Quantum Spin-Ice Candidate Ce 2⁢ Zr 2 ⁢O 7 : No Apparent Octupolar Correlations Above 𝑇 = 0.05 K

The insulating magnetic pyrochlore Ce 2 ⁢Zr 2 ⁢O 7 has gained attention as a quantum spin-ice candidate with dipole-octupole character that arises from the crystal-electric-field ground-state doublet for the Ce 3+ Kramers ion. This dipole-octupole character permits both spin-ice phases based on magnetic dipoles and those based on more-exotic octupoles. This work reports low-temperature neutron diffraction measurements on single-crystal Ce 2 ⁢Zr 2⁢ O 7 with 𝑄 coverage both at low 𝑄, where the magnetic form factor for dipoles is near maximal, and at high 𝑄, covering the region where the magnetic form factor for Ce 3+ octupoles is near maximal. This study was motivated by recent powder neutron diffraction studies of other Ce-based dipole-octupole pyrochlores, Ce 2 ⁢Sn 2 ⁢O 7 and Ce 2 ⁢Hf 2 ⁢O 7 , which each showed temperature-dependent diffuse diffraction at high 𝑄, interpreted as arising from octupolar correlations. Our measurements use an optimized single-crystal diffuse scattering instrument that allows us to screen against strong Bragg scattering from Ce 2 ⁢Zr 2 ⁢O 7 . The temperature-difference neutron diffraction reveals a low-𝑄 peak consistent with dipolar spin-ice correlations reported in previous work, and an alternation between positive and negative net intensity at higher 𝑄. These features are consistent with our numerical-linked-cluster calculations using pseudospin interaction parameters previously reported for Ce 2 ⁢Zr 2⁢ O 7 , Ce 2 ⁢Sn 2 ⁢O 7 , and Ce 2 ⁢Hf 2 ⁢O 7 . Importantly, neither the measured data nor any of the NLC calculations show evidence for increased scattering at high 𝑄 resulting from octupolar correlations. We conclude that at the lowest attainable temperature for our measurements (𝑇 = 0.05 K), scattering from octupolar correlations in Ce 2 ⁢Zr 2 ⁢O 7 is not present in the neutron diffraction signal on the level of our observation threshold of around 0.1% of the low-𝑄 dipole scattering. We compare these results to those obtained earlier on powder Ce 2 ⁢Sn 2 ⁢O 7 and Ce 2⁢ Hf 2⁢ O 7 , and to low-energy inelastic neutron scattering from single-crystal Ce 2 ⁢Zr 2 ⁢O 7 .

36 MATERIALS SCIENCE↗
DOE OSTI2021

High Ammonia Adsorption in MFM-300 Materials: Dynamics and Charge Transfer in Host–Guest Binding

Ammonia (NH 3 ) is a promising energy resource owing to its high hydrogen density. However, its widespread application is restricted by the lack of efficient and corrosion-resistant storage materials. In this work, we report high NH 3 adsorption in a series of robust metal-organic framework (MOF) materials, MFM-300(M) (M = Fe, V, Cr, In). MFM-300(M) (M = Fe, V III , Cr) show fully reversible capacity for >20 cycles, reaching capacities of 16.1, 15.6, and 14.0 mmol g -1 , respectively, at 273 K and 1 bar. Under the same conditions, MFM-300(V IV ) exhibits the highest uptake among this series of MOFs of 17.3 mmol g -1 . In situ neutron powder diffraction, single-crystal X-ray diffraction, and electron paramagnetic resonance spectroscopy confirm that the redox-active V center enables host-guest charge transfer, with V IV being reduced to V III and NH 3 being oxidized to hydrazine (N 2 H 4 ). A combination of in situ inelastic neutron scattering and DFT modeling has revealed the binding dynamics of adsorbed NH 3 within these MOFs to afford a comprehensive insight into the application of MOF materials to the adsorption and conversion of NH 3 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Sawtooth lattice multiferroic BeCr 2 O 4 : Noncollinear magnetic structure and multiple magnetic transitions

Noncollinear magnetic structures and multiple magnetic phase transitions in a sawtooth lattice antiferromagnet consisting of Cr 3+ are experimentally identified in this work, thereby proposing the scenario of magnetism-driven ferroelectricity in a sawtooth lattice. The title compound, BeCr 2 O 4 , displays three magnetic phase transitions at low temperatures—at T N1 ≈ 7.5 K, at T N2 ≈ 25 K, and at T N3 ≈ 26 K—revealed through magnetic susceptibility, specific heat, and neutron diffraction in this work. These magnetic phase transitions are found to be influenced by externally applied magnetic fields. Isothermal magnetization curves at low temperatures below the magnetic transitions indicate the antiferromagnetic nature of BeCr 2 O 4 with two spin-flop-like transitions occurring at H c1 ≈ 29 kOe and H c2 ≈ 47 kOe. Our high-resolution x-ray and neutron diffraction studies, performed on single crystal and powder samples, unambiguously determined the crystal structure as orthorhombic Pbnm. By performing the magnetic superspace group analysis of the neutron diffraction data at low temperatures, the magnetic structure in the temperature range T N3,N2 < T < T N1 is determined to be the polar magnetic space group P21nm. 1' (00g) 0s0s with a cycloidal magnetic propagation vector k 1 = (0, 0, 0.090 (1)) . The magnetic structure in the newly identified phase below T N1 is determined as P21/b.1' [b] (00 g) 00s with the magnetic propagation vector k 2 = (0, 0, 0.908 (1)). Finally, the cycloidal spin structure determined in our work is usually associated with electric polarization, thereby making BeCr 2 O 4 a promising multiferroic belonging to the sparsely populated family of sawtooth lattice antiferromagnets.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Unraveling magneto-structural coupling of Ni 2 MnGa alloy under the application of stress and magnetic field using in situ polarized neutron diffraction

The magneto-structural evolution of a Ni 2 MnGa single crystal was investigated by in situ polarized neutron diffraction under both magnetic field and mechanical loading. The ability to separate the nuclear and magnetic scatterings by polarized neutrons enables simultaneous observations of the twin reorientation (through twin boundary motion) and magnetic moment configuration. It is found that under a 1.0 T saturating magnetic field, twin reorientation can be activated by compressive stress and is accompanied by a realignment of the magnetic moment, which follows the easy axis of the twin variant. On the other hand, compressive stress as small as 1.0 MPa can freeze the twin reorientation. The evolution of the magnetic scattering amplitudes suggests that the change in magnetization was mainly achieved through the magnetic domain wall motion, while the twin boundary motion was blocked.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Competing magnetic phases in Cr 3+𝛿 ⁢Te 4 are spatially segregated

Cr 1+𝑥⁢ Te 2 is a self-intercalated van der Waals system that is of current interest for its room-temperature room-temperature ferromagnetic (FM) phases and tunable topological properties. In bulk samples, the strain from the interstitial Cr ions leads to distinct structural phases for different ranges of 𝑥. Early neutron powder diffraction (NPD) measurements on the monoclinic phase Cr 3 ⁢Te 4 (𝑥=0.5) presented evidence for competing FM and antiferromagnetic (AFM) phases. Here we apply neutron diffraction to a single crystal of Cr 3+𝛿 ⁢Te 4 with 𝛿=−0.10 and discover that it consists of two distinct monoclinic phases, one with FM order below 𝑇 C ≈321 K and another that develops AFM order below 𝑇 N ≈86 K. In contrast, we find that a crystal with 𝛿=−0.26 exhibits only FM order below 𝑇 C ≈285 K. The single-crystal analysis is complemented by results obtained with NPD, x-ray powder diffraction, and transmission electron microscopy (TEM) measurements on the 𝛿=−0.10 composition. From observations of spontaneous magnetostriction of opposite sign at 𝑇 C and 𝑇 N , along with the TEM evidence for both monoclinic phases in a single thin ( ≈100 nm) grain, we conclude that the two phases must have a fine-grained ( ≲100 nm) intergrowth character, as might occur from high-temperature spinodal decomposition during the growth process. Calculations of the relaxed lattice structures for the FM and AFM phases with density functional theory provide a rationalization of the observed spontaneous magnetostrictions. Correlations between the magnitude and orientation of the magnetic moments with lattice parameter variation demonstrate that the magnetic orders are sensitive to strain, thus explaining why magnetic ordering temperatures and anisotropies can be different between bulk and thin-film samples, when the latter are subject to epitaxial strain. Our results point to the need to investigate the supposed coexistence FM and AFM phases reported elsewhere in the Cr 1+𝑥 ⁢Te 2 system, such as in the Cr 5 ⁢Te 8 phase (𝑥=0.25).

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Fast Li-Ion Conductivity in Superadamantanoid Lithium Thioborate Halides

Lithium thioborates are promising fast Li-ion conducting materials, with similar properties to their lithium thiophosphate counterparts that have enabled the development of solid-state Li-ion batteries. By comparison, thioborates have scarcely been developed, however, offering new space for materials discovery. In this work, we report a new class of lithium thioborate halides that adopt a so-called supertetrahedral adamantanoid structure that houses mobile lithium ions and halide anions within interconnected 3D structural channels. Investigation of the structure using single-crystal XRD, neutron powder diffraction, and neutron PDF reveals significant lithium and halide anion disorder. The phases are non-stoichiometric, adopting slightly varying halide contents within the materials. These new superadamantanoid materials exhibit high ionic conductivities up to 1.4 mS cm -1 , which can be effectively tuned by the polarizability of the halide anion within the channels.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Nature of the ferromagnetic-antiferromagnetic transition in Y 1- x La x TiO 3

In this work, we explore the magnetically ordered ground state of the isovalently substituted Mott insulator Y 1- x La x TiO 3 for x≤ 0.3 via single-crystal growth, magnetometry, neutron diffraction, x-ray magnetic circular dichroism, muon spin rotation, and small-angle neutron scattering (SANS). We find that the decrease in the magnetic transition temperature on approaching the ferromagnetic-antiferromagnetic phase boundary at the La concentration xc ≈ 0.3 is accompanied by a strong suppression of both bulk and local ordered magnetic moments, along with a volume wise separation into magnetically ordered and paramagnetic regions. The thermal phase transition does not show conventional second-order behavior since neither a clear signature of dynamic critical behavior nor a power-law divergence of the magnetic correlation length is found for the studied substitution range; this finding becomes increasingly obvious with increasing La substitution. We find no evidence for a spin-glass phase. Finally, from SANS and magnetometry measurements, we discern a crossover from easy-axis to easy-plane magnetocrystalline anisotropy with increasing La substitution. These results indicate complex changes in magnetic structure upon approaching the phase boundary.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Neutron diffraction: a primer

Because of the neutron’s special properties, neutron diffraction may be considered one of the most powerful techniques for structure determination of crystalline and related matter. Neutrons can be released from nuclear fission, from spallation processes, and also from low-energy nuclear reactions, and they can then be used in powder, time-of-flight, texture, single crystal, and other techniques, all of which are perfectly suited to clarify crystal and magnetic structures. With high neutron flux and sufficient brilliance, neutron diffraction also excels for diffuse scattering, for in situ and operando studies as well as for high-pressure experiments of today’s materials. For these, the wave-like neutron’s infinite advantage (isotope specific, magnetic) is crucial to answering important scientific questions, for example, on the structure and dynamics of light atoms in energy conversion and storage materials, magnetic matter, or protein structures. In this primer, we summarize the current state of neutron diffraction (and how it came to be), but also look at recent advances and new ideas, e.g., the design of new instruments, and what follows from that.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Magnetic properties of the Ising-like rare earth pyrosilicate: D-Er 2 Si 2 O 7

Ising-like spin-1/2 magnetic materials are of interest for their ready connection to theory, particularly in the context of quantum critical behavior. In this work we report detailed studies of the magnetic properties of a member of the rare earth pyrosilicate family, D-Er 2 Si 2 O 7 , which is known to display a highly anisotropic Ising-like g-tensor and effective spin-1/2 magnetic moments. We used powder neutron diffraction, powder inelastic neutron spectroscopy (INS), and single crystal AC susceptibility to characterize its magnetic properties. Neutron diffraction enabled us to determine the magnetic structure below the known transition temperature (T N = 1.9 K) in zero field, confirming that the magnetic state is a four-sublattice antiferromagnetic structure with two non-collinear Ising axes, as was previously hypothesized. Our powder INS data revealed a gapped excitation at zero field, consistent with anisotropic (possibly Ising) exchange. An applied field of 1 T produces a mode softening, which is consistent with a field-induced second order phase transition. To assess the relevance of D-Er 2 Si 2 O 7 to the transverse field Ising model, we performed AC susceptibility measurements on a single crystal with the magnetic field oriented in the direction transverse to the Ising axes. This revealed a transition at 2.65 T at 0.1 K, a field significantly higher than the mode-softening field observed by powder INS, showing that the field-induced phase transitions are highly field-direction dependent as expected. Furthermore, these measurements suggest that D-Er 2 Si 2 O 7 may be a candidate for further exploration related to the transverse field Ising model.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

K-space algorithmic reconstruction (KAREN): a robust statistical methodology to separate Bragg and diffuse scattering

Diffuse scattering occurring in the Bragg diffraction pattern of a long-range-ordered structure represents local deviation from the governing regular lattice. However, interpreting the real-space structure from the diffraction pattern presents a significant challenge because of the dramatic difference in intensity between the Bragg and diffuse components of the total scattering function. In contrast to the sharp Bragg diffraction, the diffuse signal has generally been considered to be a weak expansive or continuous background signal. In this paper, using 1D and 2D models, it is demonstrated that diffuse scattering in fact consists of a complex array of high-frequency features that must not be averaged into a low-frequency background signal. To evaluate the actual diffuse scattering effectively, an algorithm has been developed that uses robust statistics and traditional signal processing techniques to identify Bragg peaks as signal outliers which can be removed from the overall scattering data and then replaced by statistically valid fill values. This method, described as a 'K-space algorithmic reconstruction' (KAREN), can identify Bragg reflections independent of prior knowledge of a system's unit cell. KAREN does not alter any data other than that in the immediate vicinity of the Bragg reflections, and reconstructs the diffuse component surrounding the Bragg peaks without introducing discontinuities which induce Fourier ripples or artifacts from underfilling `punched' voids. The KAREN algorithm for reconstructing diffuse scattering provides demonstrably better resolution than can be obtained from previously described punch-and-fill methods. The superior structural resolution obtained using the KAREN method is demonstrated by evaluating the complex ordered diffuse scattering observed from the neutron diffraction of a single plastic crystal of CBr 4 using pair distribution function analysis.

36 MATERIALS SCIENCE↗