Engineering topics

Ye, Feng

Publications and source records attributed to Ye, Feng.

14 records

DOE OSTI2024

Role of stacking defects on the magnetic behavior of CrCl 3

Here, in the study of van der Waals–layered magnetic materials, the properties of CrCl 3 continue to attract attention. This compound is reported to undergo antiferromagnetic ordering below ~14 K, with a ferromagneticlike region proposed to exist between 14 and 17 K. Ideally, the crystal structure is rhombohedral (R) below ~235 K, separated from a higher-temperature monoclinic (M) phase by a layer-sliding structural phase transition. However, the structural transition is often inhibited even in bulk single crystals, allowing M-type layer stacking, reported to have a 10-fold greater interlayer magnetic coupling than R-type stacking, to be present at low temperature. To clarify the effect of stacking defects on CrCl 3 , we report magnetization measurements on samples of varying crystalline quality. At low applied magnetic field, some crystals predominantly show the T N = 14 K peak, but other crystals show hysteretic behavior and a magnetization enhancement at a slightly higher temperature (14 < T ≲ 17 K.) Samples with anomalous behavior exhibit a transition around ~2 T in isothermal magnetization-field data, evidence that M-type stacking defects are the source of these anomalies. Ground powder samples are especially likely to show strongly anomalous behavior. We suggest that the anomalous behavior arises from few-layer magnetic domains that form just above T N in an environment of mixed interlayer magnetic coupling strength. We argue that the influence of M-type stacking boundaries on sublattice magnetization is already observable in reported neutron scattering data, and may be responsible for an enhancement near 17 K in reported specific heat data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Thermal evolution of spin excitations in honeycomb Ising antiferromagnetic FePSe 3

We use elastic and inelastic neutron scattering (INS) to study the antiferromagnetic (AF) phase transitions and spin excitations in the two-dimensional (2D) zig-zag antiferromagnet FePSe 3 . By determining the magnetic order parameter across the AF phase transition, we conclude that the AF phase transition in FePSe 3 is first-order in nature. In addition, our INS measurements reveal that the spin waves in the AF ordered state have a large easy-axis magnetic anisotropy gap, consistent with an Ising Hamiltonian, and possible biquadratic magnetic exchange interactions. On warming across T N , we find that dispersive spin excitations associated with three-fold rotational symmetric AF fluctuations change into FM spin fluctuations above T N . These results suggest that the first-order AF phase transition in FePSe 3 may arise from the competition between C 3 symmetric AF and C 1 symmetric FM spin fluctuations around T N , in place of a conventional second-order AF phase transition.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Optimization of neutron chopper and optics for CENTAUR, the SANS/WANS diffractometer at the spallation neutron source second target station

Herein this report presents the physics design and optimization of the neutron chopper and optics systems for the CENTAUR instrument, a multifunctional small-angle and wide-angle neutron scattering diffractometer for the Spallation Neutron Source Second Target Station. This instrument will offer a wide range of capabilities, including small-angle neutron scattering with wide Q coverage (e.g., 0.001–20 Å –1 ), providing a tool to investigate structures from atomic to mesoscopic scales simultaneously. To efficiently transport desired neutrons from the compact high-brightness cold source, several innovative designs are utilized: a time-zero chopper with a straight guide system for short-wavelength neutrons, octagonal guides for higher flux, and a correlation chopper to reduce inelastic scattering. The optimization process considers factors such as useable time-integrated flux, instrument resolution, brilliance transfer, divergence, and acceptance diagram uniformity. The overall design prioritizes flexibility to accommodate diverse user requirements.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

Symmetry Breaking and Ascending in the Magnetic Kagome Metal FeGe

Spontaneous symmetry breaking—the phenomenon in which an infinitesimal perturbation can cause the system to break the underlying symmetry—is a cornerstone concept in the understanding of interacting solid-state systems. In a typical series of temperature-driven phase transitions, higher-temperature phases are more symmetric due to the stabilizing effect of entropy that becomes dominant as the temperature is increased. However, the opposite is rare but possible when there are multiple degrees of freedom in the system. Here, we present such an example of a symmetry-ascending phenomenon upon cooling in a magnetic kagome metal FeGe by utilizing neutron Larmor diffraction and Raman spectroscopy. FeGe has a kagome lattice structure with simple A-type antiferromagnetic order below Néel temperature T N ≈ 400 K and a charge density wave (CDW) transition at T CDW ≈ 110 K , followed by a spin-canting transition at around 60 K. In the paramagnetic state at 460 K, we confirm that the crystal structure is indeed a hexagonal kagome lattice. On cooling to around T N , the crystal structure changes from hexagonal to monoclinic with in-plane lattice distortions on the order of 10 − 4 and the associated splitting of the double-degenerate phonon mode of the pristine kagome lattice. Upon further cooling to T CDW , the kagome lattice shows a small negative thermal expansion, and the crystal structure gradually becomes more symmetric upon further cooling. A tendency of increasing the crystalline symmetry upon cooling is unusual; it originates from an extremely weak structural instability that coexists and competes with the CDW and magnetic orders. These observations are against the expectations for a simple model with a single order parameter and hence can only be explained by a Landau free energy expansion that takes into account multiple lattice, charge, and spin degrees of freedom. Thus, the determination of the crystalline lattice symmetry as well as the unusual spin-lattice coupling is a first step towards understanding the rich electronic and magnetic properties of the system, and it sheds new light on intertwined orders where the lattice degree of freedom is no longer dominant. Published by the American Physical Society 2024

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2024

Competing itinerant and local spin interactions in kagome metal FeGe

The combination of a geometrically frustrated lattice, and similar energy scales between degrees of freedom endows two-dimensional Kagome metals with a rich array of quantum phases and renders them ideal for studying strong electron correlations and band topology. The Kagome metal, FeGe is a noted example of this, exhibiting A-type collinear antiferromagnetic (AFM) order at T N ≈ 400 K, then establishes a charge density wave (CDW) phase coupled with AFM ordered moment below T CDW ≈ 110 K, and finally forms a c-axis double cone AFM structure around T Canting ≈ 60 K. Here we use neutron scattering to demonstrate the presence of gapless incommensurate spin excitations associated with the double cone AFM structure of FeGe at temperatures well above T Canting and T CDW that merge into gapped commensurate spin waves from the A-type AFM order. Commensurate spin waves follow the Bose factor and fit the Heisenberg Hamiltonian, while the incommensurate spin excitations, emerging below T N where AFM order is commensurate, start to deviate from the Bose factor around T CDW , and peaks at T Canting . This is consistent with a critical scattering of a second order magnetic phase transition with decreasing temperature. By comparing these results with density functional theory calculations, we conclude that the incommensurate magnetic structure arises from the nested Fermi surfaces of itinerant electrons and the formation of a spin density wave order.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Three-dimensional checkerboard spin structure on a breathing pyrochlore lattice

The standard approach to realize a spin-liquid state is through magnetically frustrated states, relying on ingredients such as the lattice geometry, dimensionality, and magnetic interaction type of the spins. While Heisenberg spins on a pyrochlore lattice with only antiferromagnetic nearest-neighbor interactions are theoretically proven disordered, spins in real systems generally include longer-range interactions. The spatial correlations at longer distances typically stabilize a long-range order rather than enhancing a spin-liquid state. Both states can, however, be destroyed by short-range static correlations introduced by chemical disorder. Here, using disorder-free specimens with a clear long-range antiferromagnetic order, we refine the spin structure of the Heisenberg spinel ZnFe 2 O 4 through neutron magnetic diffraction. The unique wave vector (1, 0, $\frac{1}{2}$) leads to a spin structure that can be viewed as alternatively stacked ferromagnetic and antiferromagnetic tetrahedra in a three-dimensional checkerboard form. Stable coexistence of these opposing types of clusters is enabled by the bipartite breathing pyrochlore crystal structure, leading to a second-order phase transition at 10 K. The diffraction intensity of ZnFe 2 O 4 is an exact complement to the inelastic scattering intensity of several chromate spinel systems which are regarded as model classical spin liquids. Our results challenge this attribution, and suggest instead of the six-spin ring mode, spin excitations in chromate spinels are closely related to the (1, 0, $\frac{1}{2}$) type of spin order and the four-spin ferromagnetic cluster locally at one tetrahedron.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Large magnetic anisotropy of a decorated spin-chain system K 2 Co 3 (MoO 4 ) 3 (OH) 2

The magnetic structure of K 2 Co 3 (MoO 4 ) 3 (OH) 2 is studied in detail. The material has a half-sawtooth one-dimensional (1-D) structure containing two unique Co 2+ ions, one in the chain backbone and one on the apex of the sawtooth creating a series of isosceles triangles along the b-axis. These triangles can be a source of magnetic frustration. The ability to grow large single crystals enables detailed magnetic measurements with the crystals oriented in a magnetic field along the respective axes. It has a Curie–Weiss temperature θ CW of 5.3(2) K with an effective magnetic moment of 4.8(3)μ B /Co. The material is highly anisotropic with a sharp antiferromagnetic ordering transition at 7 K with a metamagnetic transition at 2 kOe. Neutron diffraction was used to determine the magnetic structure and revealed a magnetic structure with canted spins along the backbone of the chain while spins along the sawtooth caps maintained a colinear orientation, arranging antiferromagnetically relative to the backbone spins. In conclusion, the parallel chains arrange antiferromagnetically relative to each other along the c-axis and ferromagnetically along the a-axis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Stacking disorder and thermal transport properties of α-RuCl 3

α-RuCl 3 , a well-known candidate material for Kitaev quantum spin liquid, is prone to stacking disorder due to the weak van der Waals bonding between the honeycomb layers. After a decade of intensive experimental and theoretical studies, the detailed correlation between stacking degree of freedom, structure transition, magnetic, and thermal transport properties remains unresolved. In this work, we reveal the effects of a small amount of stacking disorder inherent even in high quality α-RuCl 3 crystals. This small amount of stacking disorder results in the variation of the magnetic ordering temperature, and it suppresses the structure transition and thermal conductivity. Crystals with a minimal amount of stacking disorder have a T N > 7.4 K and exhibit a well-defined structure transition around 140 K upon cooling. For those with more stacking faults and a T N below 7 K, the structure transition occurs well below 140 K upon cooling and is incomplete, manifested by the diffuse streaks and the coexistence of both high-temperature and low-temperature phases down to the lowest measurement temperature. Both types of crystals exhibit oscillatory field-dependent thermal conductivity and a plateaulike feature in thermal Hall resistivity in the field-induced quantum spin liquid state. However, α-RuCl 3 crystals with a minimal amount of stacking disorder have a higher thermal conductivity that pushes the thermal Hall conductivity to be closer to the half-integer quantized value. Importantly, these findings demonstrate a strong correlation between layer stacking, structure transition, magnetic, and thermal transport properties, underscoring the importance of interlayer coupling in α-RuCl3 despite the weak van der Waals bonding.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Stabilization of collinear ferromagnetic order in Ir-doped triple-layer ruthenate Sr 4 Ru 3 O 10

The triple-layer Sr 4 Ru 3 O 10 is a spin-orbit-coupled metal featuring an intriguing combination of ferromagnetic and metamagnetic states. Here we report a comprehensive study of single-crystal neutron and x-ray diffraction on Sr 4 Ru 3 O 10 with 4% iridium doping. The system crystallizes in an orthorhombic Bbem structure in which two triple layers are related by a base centering symmetry operation within one unit cell. The 4% Ir doping at the Ru site sensitively alters the structural balance between the RuO 6 layers, as such the two outer-layer octahedra rotate 6.7° about the c axis, while the central-layer one rotates in the opposite direction by 11.0°. The increased lattice distortion stabilizes a collinear ferromagnetic state with magnetic moments fully aligned along the c axis. The emerging perpendicular magnetic anisotropy naturally increases the critical field for the inplane metamagnetic transition to 4.5 Tesla. All results highlight the critical linkage between the magnetic properties and underlying lattice through orbital degrees of freedom, as well as the enhanced spin orbit coupling due to heavier 5d ions. Our observation provides a viable route for an efficient manipulation of the magnetic states with functionalities.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Short-range magnetic correlations in quasicrystalline i -Tb-Cd

Here, we report on elastic and inelastic neutron scattering from single-grain isotopically enriched samples to elucidate the local magnetic correlations between Tb 3+ moments in quasicrystalline i -Tb-Cd. The inelastic neutron scattering measurements of the crystalline electric field excitations demonstrated that the Tb 3+ moments are directed primarily along the local fivefold axes of the Tsai-type cluster as was found for the TbCd 6 approximant phase. Based on the inelastic measurements, we consider a simple Ising-type model for the moment configurations on a single Tb 3+ icosahedron and enumerate the lowest energy moment configurations. We then calculate the diffuse scattering from these configurations and compare with the experimental magnetic diffuse scattering measurements to identify the most likely single cluster moment configurations and find reasonable agreement between the broad features observed in our scattering simulations. We further use a heuristic glass model as well as large-scale Monte-Carlo simulations of a multicluster model to consider the role of higher-order (longer-range) intercluster correlations for magnetic frustration and the magnetic scattering.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Structural changes induced by electric currents in a single crystal of Pr 2 CuO 4

We demonstrate an approach to the structural and electronic property modification of perovskites, focusing on Pr 2 CuO 4 , an undoped parent compound of a class of electron-doped copper-oxide superconductors. Currents were passed parallel or perpendicular to the copper oxygen layers with the voltage ramped up until a rapid drop in the resistivity was achieved, a process referred to as “flash.” The current was then further increased tenfold in current-control mode. This state was quenched by immersion into liquid nitrogen. Flash can drive many compounds into different atomic structures with new properties, whereas the quench freezes them into a long-lived state. Single-crystal neutron diffraction of as-grown and modified Pr 2 CuO 4 revealed a √10 ×√10 superlattice due to oxygen-vacancy order. The diffraction peak intensities of the superlattice of the modified sample were significantly enhanced relative to the pristine sample. Raman-active phonons in the modified sample were considerably sharper. Measurements of electrical resistivity, magnetization, and two-magnon Raman scattering indicate that the modification affected only the Pr-O layers, but not the Cu-O planes. These results point to enhanced oxygen-vacancy order in the modified samples well beyond what can be achieved without passing electrical current. Our work opens a new avenue toward electric field/quench control of structure and properties of layered perovskite oxides.

36 MATERIALS SCIENCE↗

DOE OSTI2023

NiSi: A New Venue for Antiferromagnetic Spintronics

Envisaging antiferromagnetic spintronics pivots on two key criteria of high transition temperature and tuning of underlying magnetic order using straightforward application of magnetic field or electric current. Here, it is shown that NiSi metal can provide suitable new platform in this quest. First, the study unveils high-temperature antiferromagnetism in single-crystal NiSi with Néel temperature, T N $\geqslant$ 700 K. Antiferromagnetic order in NiSi is accompanied by non-centrosymmetric magnetic character with small ferromagnetic component in the a–c plane. Second, it is found that NiSi manifests distinct magnetic and electronic hysteresis responses to field applications due to the disparity in two moment directions. While magnetic hysteresis is characterized by one-step switching between ferromagnetic states of uncompensated moment, electronic behavior is ascribed to metamagnetic switching phenomena between non-collinear spin configurations. Importantly, the switching behaviors persist to high temperature. In conclusion, the properties underscore the importance of NiSi in the pursuit of antiferromagnetic spintronics.

36 MATERIALS SCIENCE↗

DOE OSTI2023

The nature of dynamic local order in CH 3 NH 3 PbI 3 and CH 3 NH 3 PbBr 3

Hybrid organic-inorganic lead-halide perovskites (LHPs) are a class of semiconductors with remarkable properties relevant to optoelectronic applications. The structure-property-function relationship in LHPs, however, is poorly understood, leading to incomplete descriptions of optoelectronic properties and a persistent problem of device degradation due to ion migration. Here, we reveal the true structure to contain an assembly of dynamic, two-dimensional short-range structural correlations in the lead-halide octahedral sublattice, with additional correlations between organic molecules. Here, we propose that these correlations are the origin of large-amplitude halide displacements, which govern charge carrier mobility and the sharpness of the absorption edge. Correlations between organic molecules may introduce regions of transient ferroelectricity or antiferroelectricity, which increase charge carrier lifetime. Finally, the correlations introduce an ion diffusion barrier that is static on the timescale of diffusive jumps.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Diffusive excitonic bands from frustrated triangular sublattice in a singlet-ground-state system

Magnetic order in most materials occurs when magnetic ions with finite moments arrange in a particular pattern below the ordering temperature. Intriguingly, if the crystal electric field (CEF) effect results in a spin-singlet ground state, a magnetic order can still occur due to the exchange interactions between neighboring ions admixing the excited CEF levels. The magnetic excitations in such a state are spin excitons generally dispersionless in reciprocal space. Here we use neutron scattering to study stoichiometric Ni 2 Mo 3 O 8 , where Ni 2+ ions form a bipartite honeycomb lattice comprised of two triangular lattices, with ions subject to the tetrahedral and octahedral crystalline environment, respectively. We find that in both types of ions, the CEF excitations have nonmagnetic singlet ground states, yet the material has magnetic order. Furthermore, CEF spin excitons from the tetrahedral sites form a dispersive diffusive pattern around the Brillouin zone boundary, likely due to spin entanglement and geometric frustrations.

36 MATERIALS SCIENCE↗