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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Kinetically stabilized ferroelectricity in bulk single-crystalline HfO 2 :Y

HfO 2 , a simple binary oxide, exhibits ultra-scalable ferroelectricity integrable into silicon technology. This material has a polymorphic nature, with the polar orthorhombic (Pbc2 1 ) form in ultrathin films regarded as the plausible cause of ferroelectricity but thought not to be attainable in bulk crystals. In this work, using a state-of-the-art laser-diode-heated floating zone technique, we report the Pbc2 1 phase and ferroelectricity in bulk single-crystalline HfO 2 :Y as well as the presence of the antipolar Pbca phase at different Y concentrations. Neutron diffraction and atomic imaging demonstrate (anti)polar crystallographic signatures and abundant 90°/180° ferroelectric domains in addition to switchable polarization with negligible wake-up effects. Density-functional-theory calculations indicate that the yttrium doping and rapid cooling are the key factors for stabilization of the desired phase in bulk. Our observations provide insights into the polymorphic nature and phase control of HfO 2 , remove the upper size limit for ferroelectricity and suggest directions towards next-generation ferroelectric devices.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Atomic structural mechanism for ferroelectric-antiferroelectric transformation in perovskite NaNbO 3

Sodium niobate (NaNbO 3 or NN) is described as “the most complex perovskite system,” which exhibits transitions between, as well as coexistence of, several ferroelectrics (FE) and antiferroelectric (AFE) phases at different temperatures. Recently, solid solutions of NN with stabilized AFE phases(s) have gained attention for energy-related applications, such as high-density energy storage and electrocaloric cooling. A better understanding of the atomic mechanisms responsible for AFE/FE phase transitions in NaNbO 3 can enable a more rational design of its solid-solution systems with tunable functional properties. In this work, we have investigated changes in the average and local atomic structure of NN using a combination of x-ray/neutron diffraction and neutron pair-distribution function (PDF) analyses. The Rietveld refinement of the x-ray/neutron-diffraction patterns indicates a coexistence of the FE Q (P2 1 ma) and AFE P (Pbma) phases in the temperature range of 300 K ≤ T ≤ 615K, while PDF analysis indicated that the local structure (r < 8Å) is better described by a P2 1 ma symmetry. Above 615 K, the average structure transitions to an AFE R phase (Pmmn or Pnma), while PDF analysis shows an increased disordering of the octahedral distortions and Na displacements at the local scale. These results indicate that the average P/Q/R phase transitions in NN can be described as a result of complex ordering of distorted octahedral tilts at the nanoscale and off-centered displacements of the Na atoms.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Magnetic structure and magnetoelectric properties of the spin-flop phase in LiFePO 4

We investigate the magnetic structure and magnetoelectric(ME) effect in the high-field phase of the antiferromagnet LiFePO 4 above the critical field of 31 T. A neutron diffraction study in pulsed magnetic fields reveals the propagation vector to be q = 0 for the high-field magnetic structure. Pulsed-field electric polarization measurements show that, at the critical field, the low-field off-diagonal ME coupling α ab is partially suppressed, and the diagonal element α bb emerges. These results are consistent with a spin-flop transition where the spin direction changes from primarily being along the easy b axis below the transition to being along a above. The persistence of off-diagonal ME tensor elements above the critical field suggests a lowering of the magnetic point-group symmetry and hence a more complex magnetic structure in the high-field phase. In addition, neutron diffraction measurements in low magnetic fields show no observable field-induced spin canting, which indicates a negligible Dzyaloshinskii-Moriya interaction. The observed spin-flop field supports the Hamiltonian recently deduced from inelastic neutron studies and indicates that the system is less frustrated and with a larger single-ion anisotropy than originally thought. Our results demonstrate the effectiveness of combining pulsed-field neutron diffraction and electric polarization measurements to elucidate the magnetic structures and symmetries at the highest attainable field strengths.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Complex spin structure in co-trimer-chain Li 2 Co 3 Se 4 O 12

Complex magnetic materials are extremely attractive for revealing unconventional spin states and novel magnetic excitations. Here, we report the structural, thermodynamic, and magnetic properties of a novel magnetic material Li 2 Co 3 Se 4 O 12 based on x-ray and neutron diffraction, specific heat, magnetization, and x-ray photoelectron spectroscopy measurements. X-ray and neutron diffraction refinements reveal two Co sites Co (1) and Co (2) even though both are in the octahedral environment. While they are not connected along the b and c directions, these octahedra are edge-shared forming the Co (2) – Co (1) – Co (2) trimer chain along the a direction. The magnetic susceptibility exhibits the Curie-Weiss (CW) temperature dependence at high temperatures (above ∼50 K) with the negative CW temperature, a dip centered at T ⁎ ∼ 8.0 K, and an antiferromagnetic transition at T N = 3.3 K. The specific heat confirms that there is a phase transition at T N and a hump at T ⁎ . The long-range magnetic transition at T N implies that, in addition to the intra-chain interaction, there is strong inter-chain interaction, which is likely due to polarized SeO 3 bridging between chains. Single crystal neutron diffraction refinement reveals a complex magnetic structure with the angle between Co (1) and Co (2) moments ∼105°. Within the Co (2) – Co (1) – Co (2) trimer, two Co (2) moments are parallelly aligned. Surprisingly, the Co (1) moment (1.92μB) is only half of the Co (2) moment (3.96μB). There is likely the spin-state change for Co (1) from the high-spin state at T > T ⁎ to the low-spin state at T < T ⁎ , causing a dip in the magnetic susceptibility and a hump in the specific heat. When the magnetic field is applied, multiple metamagnetic transitions are found in all directions, implying field-driven magnetic excitations. Our results demonstrate rich magnetic properties of Li 2 Co 3 Se 4 O 12 that are sensitive to the external stimuli such as the magnetic field.

Antiferromagnetism↗
DOE OSTI2025

Structural Distortions and Uniaxial Negative Thermal Expansion in the Polar Dion–Jacobson Oxide RbNdTa 2 O 7

We provide deeper insight into the crystal structures, sequential structural phase transitions (I2cm → Cmce → I4/mcm → P4/mmm), thermal expansion, and electronic properties of the n = 2 Dion–Jacobson polar oxide RbNdTa 2 O 7 , through X-ray powder diffraction, neutron powder diffraction, Raman studies, and density functional theory calculations. We observed a uniaxial negative thermal expansion (NTE) across the first-order transition, I2cm → Cmce, where the unit cell contracts along the c-axis, which is driven by a contraction of the NdTa 2 O 6 layer. Here, this NTE occurs within the temperature range of the first-order phase transition and contrasts with the corkscrew mechanism typically observed in Ruddlesden–Popper phases. In RbNdTa 2 O 7 , the I2cm (hybrid improper ferroelectric) → Cmce (antipolar) transition involves crucial changes in the bond lengths of Nd and Ta polyhedra, coupled with polar to antipolar displacement of the Nd ions, leading to a net contraction in the NdTa 2 O 6 layer along the c-axis, while preserving the overall octahedral tilting magnitude. This transition highlights the intricate interplay between the Nd and Ta coordination and the associated TaO 6 distortions. Temperature-dependent Raman spectra analysis further confirms the first-order structural transition and associated NTE, providing evidence for increased bond stiffness across this transition. Additionally, using neutron powder diffraction, we have determined that the transition I4/mcm → P4/mmm occurs at approximately 1150 K. Finally, we have calculated from DFT + U, the partial density of states, the energy bandgaps, and effective masses of the charge carriers of the polar ground structure.

Chemical structure↗
DOE OSTI2024

Microstructural Underpinnings of Giant Intrinsic Exchange Bias in Epitaxial NiCo 2 O 4 Thin Films

Understanding intrinsic exchange bias in nominally single-component ferromagnetic or ferrimagnetic materials is crucial for simplifying related device architectures. However, the mechanisms behind this phenomenon and its tunability remain elusive, which hinders the efforts to achieve unidirectional magnetization for widespread applications. Inspired by the high tunability of ferrimagnetic inverse spinel NiCo 2 O 4 , the origin of intrinsic exchange bias in NiCo 2 O 4 (111) films deposited on Al 2 O 3 (0001) substrates are investigated. The comprehensive characterizations, including electron diffraction, X-ray reflectometry and spectroscopy, and polarized neutron reflectometry, reveal that intrinsic exchange bias in NiCo 2 O 4 (111)/Al 2 O 3 (0001) arises from a reconstructed antiferromagnetic rock-salt Ni x Co 1-x O layer at the interface between the film and the substrate due to a significant structural mismatch. Remarkably, by engineering the interfacial structure under optimal growth conditions, it can achieve exchange bias larger than coercivity, leading to unidirectional magnetization. Such giant intrinsic exchange bias can be utilized for realistic device applications. This work establishes a new material platform based on NiCo 2 O 4 , an emergent spintronics material, to study tunable interfacial magnetic and spintronic properties.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Complex magnetic phases in the polar tetragonal intermetallic NdCoGe 3

Polar materials can host a variety of topologically significant magnetic phases, which often emerge from a modulated magnetic ground state. Relatively few noncentrosymmetric tetragonal materials have been shown to host topological spin textures and new candidate materials are necessary to expand the current theoretical models. This manuscript reports on the anisotropic magnetism in the polar, tetragonal material NdCoGe 3 via thermodynamic and neutron diffraction measurements. The previously reported H - T phase diagram is updated to include several additional phases, which exist for both H = 0 and with an applied field H ⊥ c . Neutron diffraction data reveal that the magnetic structures below T N 1 = 3.70 K and T N 2 = 3.50 K are incommensurate, with a ground-state magnetic order that is incommensurate in all directions with the propagation vector $\vec{k}$ = (0.494, 0.0044, 0.385) at 1.8 K. A unique magnetic structure solution is not achievable, but the possible single-$\vec{k}$ and $\vec{k}$ spin models are discussed. These results demonstrate that NdCoGe 3 hosts complicated magnetic order derived from modulated magnetic moments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Strain-induced majority carrier inversion in ferromagnetic epitaxial LaCo O 3 - δ thin films

Tensile-strained LaCoO 3-δ thin films are ferromagnetic, in sharp contrast to the zero-spin bulk, although no clear consensus has emerged as to the origin of this phenomenon. While magnetism has been heavily studied, relatively little attention has been paid to electronic transport, due to the insulating nature of the strain-stabilized ferromagnetic state. Here, structure, magnetism, and transport are studied in epitaxial LaCoO 3-δ films (10–22-nm thick) on various substrates (from 1.4% compressive to 2.5% tensile strain), using synchrotron x-ray diffraction, scanning probe and transmission electron microscopy, magnetometry, polarized neutron reflectometry, resistivity, and Hall effect. High quality, smooth films are obtained, exhibiting superstructures associated with both oxygen vacancy ordering and periodic in-plane ferroelastic domains. Consistent with prior work, ferromagnetism with an approximately 80–85 K Curie temperature is observed under tension; polarized neutron reflectometry confirms a relatively uniform magnetization depth profile, albeit with interfacial dead layer formation. Electrical transport is found to have similar semiconducting nature to bulk, but with reduced resistivity and activation energy. Hall effect measurements, however, reveal a striking inversion of the majority carrier type, from p-type in the bulk and under compression to n-type under tension. While thus far overlooked, ferromagnetism in epitaxial LaCoO 3-δ films is thus directly correlated with n-type behavior, providing important insight into the ferromagnetic state in this system. Here, aided by density functional theory calculations, these results are interpreted in terms of tensile-strain-induced orbital occupation and band structure changes, including a rapid decrease in effective mass at the e g -derived conduction band minimum, and corresponding increase at the valence band maximum.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Field-induced partial disorder in a Shastry-Sutherland lattice

Abstract A 2-Q antiferromagnetic order of the ferromagnetic dimers was found below T N = 2.9 K in the Shastry-Sutherland lattice BaNd 2 ZnS 5 by single crystal neutron diffraction. The magnetic order can be understood by the orthogonal arrangement of local Ising Nd spins, identified by polarized neutrons. A field was applied along [1 -1 0] to probe the observed metamagnetic transition in the magnetization measurement. The field decouples two magnetic sublattices corresponding to the propagation vectors q 1 = (½, ½, 0) and q 2 = (−½, ½, 0), respectively. Each sublattice shows a “stripe” order with a Néel-type arrangement in each single layer. The “stripe” order with q 1 remains nearly intact up to 6 T, while the other one with q 2 is suppressed at a critical field H c ~1.7 T, indicating a partial disorder. The H c varies with temperature and is manifested in the H - T phase diagram constructed by measuring the magnetization in BaNd 2 ZnS 5 .

36 MATERIALS SCIENCE↗
DOE OSTI2020

Interlayer magnetism in Fe 3-x GeTe 2

Fe 3 - x GeTe 2 is a layered van der Waals magnetic material with a relatively high ordering temperature and large anisotropy. While most studies have concluded the interlayer ordering to be ferromagnetic, there have also been reports of interlayer antiferromagnetism in Fe 3 - x GeTe 2 . In this work, we investigate the interlayer magnetic ordering by neutron diffraction experiments, scanning tunneling microscopy (STM) and spin-polarized STM measurements, density functional theory plus U calculations, and STM simulations. We conclude that the layers of Fe 3 - x GeTe 2 are coupled ferromagnetically and that in order to capture the magnetic and electronic properties of Fe 3 - x GeTe 2 within density functional theory, Hubbard U corrections need to be taken into account.

2-dimensional systems↗
DOE OSTI2025

Altermagnetic Band Splitting in 10 nm Epitaxial CrSb Thin Films

Altermagnets are a newly identified family of collinear antiferromagnets with a momentum-dependent spin-split band structure of non-relativistic origin, derived from spin-group symmetry-protected crystal structures. Among candidate altermagnets, CrSb is attractive for potential applications because of a large spin-splitting near the Fermi level and a high Néel transition temperature of around 700 K. Molecular beam epitaxy is used to synthesize CrSb (0001) thin films with thicknesses ranging from 10 to 100 nm. Structural characterization, using reflection high energy electron diffraction, scanning transmission electron microscopy, and X-ray diffraction, demonstrates the growth of epitaxial films with good crystallinity. Polarized neutron reflectometry shows the absence of any net magnetization, consistent with antiferromagnetic order. In vacuo angle resolved photoemission spectroscopy (ARPES) measurements probe the band structure in a previously unexplored regime of film thickness, down to 10 nm. These ARPES measurements show a bulk-type, 3D momentum-dependent band splitting of up to 0.7 eV with g-wave symmetry, consistent with that seen in prior studies of bulk single crystals. The distinct altermagnetic band structure required for potential spin-transport applications survives down to the ∼10 nm thin film limit at room temperature.

Santhosh, Sandra↗
DOE OSTI2020

Thermodynamics of Uranium Tri-Iodide from Density-Functional Theory

Density-functional theory (DFT) is employed to investigate the thermodynamic and ground-state properties of bulk uranium tri-iodide, UI3. The theory is fully relativistic and electron correlations, beyond the DFT and generalized gradient approximation, are addressed with orbital polarization. The electronic structure indicates anti-ferromagnetism, in agreement with neutron diffraction, with band gaps and a non-metallic system. Furthermore, the formation energy, atomic volume, crystal structure, and heat capacity are calculated in reasonable agreement with experiments, whereas for the elastic constants experimental data are unavailable for comparison. The thermodynamical properties are modeled within a quasi-harmonic approximation and the heat capacity and Gibbs free energy as functions of temperature agree with available calculation of phase diagram (CALPHAD) thermodynamic assessment of the experimental data.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Room temperature polar and weak-ferromagnetic oxide with low dielectric loss

Single-phase materials that are simultaneously ferroelectric and ferromagnetic at room temperature are promising for devices such as non-volatile random-access memory. Perovskite BiFeO 3 which crystallizes in the polar rhombohedral structure (R3c) is ferroelectric and antiferromagnetic at room temperature. Here, we report a family of perovskite oxides in the BiFeO 3 – Bi 2/3 TiO 3 – ATiO 3 (where A 2+ is divalent alkaline earth metal ions e.g., Ca 2+ , Sr 2+ , Ba 2+ ) ternary phase diagram that is polar as well as weak ferromagnetic above room temperature. The composition (Bi 0.9167 A 0.075 )(Fe 0.9 Ti 0.1 )O 3 crystallizes in the polar rhombohedral structure space group R3c as corroborated by powder X-ray and neutron diffraction analysis. The nearly pure A-site perovskite possesses a long-range magnetic ordering above room temperature. Finally, these perovskites show a low dielectric loss, and the electrical response is dominated by grain contributions below 723 K.

42 ENGINEERING↗
DOE OSTI2023

Conceptual Polarization Setup at CENTAUR, the SANS/WANS Instrument at the Second Target Station of SNS

CENTAUR is a multifunctional general purpose small-angle and wide-angle neutron scattering instrument with diffraction and spectroscopic capability in the future Second Target Station at the Spallation Neutron Source of the Oak Ridge National Laboratory. To fill a gap in neutron polarization capability, the instrument will be designed to provide polarization analysis. Here we present the conceptual polarization setup at CENTAUR, as well as the Spin Echo Modulated Small-Angle Neutron Scattering setup which will further expand the length scale covered by the instrument.

Qian, Shuo↗
DOE OSTI2021

The influence of the 6s 2 configuration of Bi 3+ on the structures of A′BiNb 2 O 7 (A′ = Rb, Na, Li) layered perovskite oxides

Solid state compounds which exhibit non-centrosymmetric crystal structures are of great interest due to the physical properties they can exhibit. Here, the ‘hybrid improper’ mechanism – in which two non-polar distortion modes couple to, and stabilize, a further polar distortion mode, yielding an acentric crystal structure – offers opportunities to prepare a range of novel non-centrosymmetric solids, but examples of compounds exhibiting acentric crystal structures stabilized by this mechanism are still relatively rare. Here we describe a series of bismuth-containing layered perovskite oxide phases, RbBiNb 2 O 7 , LiBiNb 2 O 7 and NaBiNb 2 O 7 , which have structural frameworks compatible with hybrid-improper ferroelectricity, but also contain Bi 3+ cations which are often observed to stabilize acentric crystal structures due to their 6s 2 electronic configurations. Neutron powder diffraction analysis reveals that RbBiNb 2 O 7 and LiBiNb 2 O 7 adopt polar crystal structures (space groups I2cm and B2cm respectively), compatible with stabilization by a trilinear coupling of non-polar and polar modes. The Bi 3+ cations present are observed to enhance the magnitude of the polar distortions of these phases, but are not the primary driver for the acentric structure, as evidenced by the observation that replacing the Bi 3+ cations with Nd 3+ cations does not change the structural symmetry of the compounds. In contrast the non-centrosymmetric, but non-polar structure of NaBiNb 2 O 7 (space group P2 1 2 1 2 1 ) differs significantly from the centrosymmetric structure of NaNdNb 2 O 7 , which is attributed to a second-order Jahn-Teller distortion associated with the presence of the Bi3+ cations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

A high-efficiency cryogenic neutron spin flipper for IMAGINE-X at the high flux isotope reactor

The Laue neutron macromolecular crystallography beamline, IMAGINE, at the High Flux Isotope Reactor (HFIR) is undergoing a major upgrade to incorporate the dynamic nuclear polarization (DNP) technique. Upon completion, the new IMAGINE-X instrument is expected to enhance the signal-to-noise ratio of the diffraction data by an order of magnitude. To take full advantage of the benefits of DNP, both a highly polarized neutron beam and a high-efficiency neutron spin flipper are required. We have developed a compact cryogenic spin flipper utilizing the Meissner effect in high-Tc yttrium–barium–copper–oxide superconducting films. The flipper has been successfully tested at two HFIR neutron development beamlines, Larmor and Poplar, with neutron wavelengths of 5.3 and 2.4 Å respectively. At Larmor, a flipping efficiency of 0.995 ± 0.004 was achieved for 5.3 Å neutrons, and at Poplar, efficiency of up to 0.9987 ± 0.0004 was obtained for 2.4 Å neutrons. Both tests demonstrated the flipper’s excellent performance and suitability for integration into IMAGINE-X.

Fu, Sichao [Oak Ridge National Laboratory (ORNL), ↗
DOE OSTI2024

Magnetic properties of the quasi-XY Shastry-Sutherland magnet ER 2 Be 2 SiO 7

Polycrystalline and single-crystal samples of the insulating Shastry-Sutherland compound Er 2 ⁢Be 2 ⁢SiO 7 were synthesized via a solid-state reaction and the floating zone method, respectively. The crystal structure, Er single-ion anisotropy, zero-field magnetic ground state, and magnetic phase diagrams along high-symmetry crystallographic directions were investigated with bulk measurement techniques, x-ray and neutron diffraction, and neutron spectroscopy. Here, we establish that Er 2 ⁢Be 2 ⁢SiO 7 crystallizes in a tetragonal space group with planes of orthogonal Er dimers and a strong preference for the Er moments to lie in the local plane perpendicular to each dimer bond. We also find that this system has a noncollinear ordered ground state in zero field with a transition temperature of 0.841 K consisting of antiferromagnetic dimers and in-plane moments. Finally, we mapped out the H-T phase diagrams for Er 2 ⁢Be 2 ⁢SiO 7 along the directions H ∥ [001], [100], and [110]. While an increasing in-plane field simply induces a phase transition to a field-polarized phase, we identify three metamagnetic transitions in the H ∥ [001] case. Single-crystal neutron diffraction results reveal that the H ∥ [001] phase diagram can be explained predominantly by the expected field-induced behavior of classical, anisotropic moments, although the microscopic origin of one phase requires further investigation.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Magnetic structure and multiferroicity of Sc-substituted hexagonal YbFeO 3

The hexagonal rare-earth ferrite RFeO 3 family represents a unique class of multiferroics exhibiting weak ferromagnetism, and a strong coupling between magnetism and structural trimerization is predicted. However, the hexagonal structure for RFeO 3 remains metastable in conventional conditions. We have succeeded in stabilizing the hexagonal structure of polycrystalline YbFeO 3 by partial Sc substitution of Yb. Using bulk magnetometry and neutron diffraction, we find that Yb 0.42 Sc 0.58 FeO 3 orders into a canted antiferromagnetic state with the Néel temperature T N ~ 165K, below which the Fe 3+ moments form the triangular configuration in the ab plane and their in-plane projections are parallel to the [100] axis, consistent with magnetic space group P6 3 c'm'. It is determined that the spin canting is aligned along the c axis, giving rise to the weak ferromagnetism. Furthermore, the Fe 3+ moments reorient toward a new direction below reorientation temperature T R ~ 40K, satisfying magnetic subgroup P6 3 , while the Yb 3+ moments order independently and ferrimagnetically along the c axis at the characteristic temperature T Yb ~ 15K. Interestingly, reproducible modulation of electric polarization induced by magnetic field at low temperature is achieved, suggesting that the delicate structural distortion associated with two-up/one-down buckling of the Yb/Sc planes and tilting of the FeO 5 bipyramids may mediate the coupling between ferroelectric and magnetic orders under magnetic field. Furthermore, the present work represents substantial progress to search for high-temperature multiferroics in hexagonal ferrites and related materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗