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DOE OSTI2025

Interface‐Induced Stability of Nontrivial Topological Spin Textures: Unveiling Room‐Temperature Hopfions and Skyrmions

Topological spin configurations, such as soliton-like spin texture and Dirac electron assemblies, have recently emerged in fundamental science and technology. Achieving stable topological spin textures at room temperature is crucial for their use as long-range information carriers. However, their creation and manipulation are hindered by multi-step field training and competing interactions. Thus, a spontaneous ground state for multidimensional topological spin textures is desirable, with skyrmions forming swirling, hedgehog-like spin structures in two dimensions and hopfions as their twisted 3D counterparts. Here, the first observation of robust and reproducible topological spin textures of hopfions and skyrmions observed at room temperature and in zero magnetic field is reported, which are stabilized by geometric confinement and protected by interfacial magnetism in a ferromagnet/topological insulator/ferromagnet trilayer heterostructure. These skyrmion-hopfion configurations are directly observed at room temperature with Lorenz transmission electron microscopy. Using micromagnetic modeling, the experimental observations of hopfion-skyrmion assemblies are reproduced. This model reveals a complete picture of how spontaneously organized skyrmion lattices encircled by hopfion rings are controlled by surface electrons, uniaxial anisotropy, and Dzyaloshinskii-Moriya interaction. This study provides evidence that topological chiral spin textures can facilitate the development of magnetic topological carriers, paving the way for ultralow-power and high-density information processing.

hopfions↗

DOE OSTI2025

Reduction in Nuclear Size and Quadrupole Deformation of High-Spin Isomers of 127,129 In

We employed laser spectroscopy of atomic transitions to measure the nuclear charge radii and electromagnetic properties of the high-spin isomeric states in neutron-rich indium isotopes (𝑍 =49) near the closed proton and neutron shells at 𝑍 = 50 and 𝑁 = 82. Our data reveal a reduction in the nuclear charge radius and intrinsic quadrupole moment when protons and neutrons are fully aligned in 129 In ⁢(𝑁 = 80), to form the high spin isomer. Such a reduction is not observed in 127 In ⁢(𝑁 = 78), where more complex configurations can be formed by the existence of four neutron holes. These observations are not consistently described by nuclear theory.

high spin states↗

DOE OSTI2020

Structure-Spin-Transport Anomaly in Quasi-One-Dimensional Ba9Fe3Te15 under High Pressure

Recently, a series of novel compounds Ba3MX5 (M= Fe, Ti, V; X=Se, Te) with hexagonal crystal structures composed of quasi-1-dimensional (1D) magnetic chains has been synthesized by our research team using high-pressure and high-temperature methods. The initial hexagonal phases persist to the maximum achievable pressure, while spin configurations and magnetic interactions may change dramatically as a result of considerable reductions in interchain separations upon pressurization. These compounds therefore offer unique possibilities for studying the evolution of intrinsic electronic structures in quasi-1D magnetic systems. Here we present a systematic investigation of Ba9Fe3Te15, in which the interchain separations between trimerized 1D chains (~10.2 Å) can be effectively modulated by external high pressure. The crystal structure especially along the 1D chains exhibits an abnormal expansion at ~5GPa, which accompanies trimerization entangled anomalous mixed-high-low spin transition. An insulator-metal transition has been observed under high pressure as a result of charge-transfer gap closing. Pressure-induced superconductivity emerges at 26GPa, where the charge-transfer gap fully closes, 3D electronic configuration forms and local spin fully collapses.

Zhang, Jun↗

DOE OSTI2021

Magnetic exchange interactions in the van der Waals layered antiferromagnet MnPSe 3

Two-dimensional van der Waals compounds with magnetic ions on a honeycomb lattice are hosts to a variety of exotic behavior. The magnetic interactions in one such compound, MnPSe 3 , are investigated with elastic and inelastic neutron scattering. Magnetic excitations are observed in the magnetically ordered regime and persist to temperatures well above the ordering temperature, T N =74K, consistent with low dimensional magnetic interactions. The inelastic neutron scattering results allow a model spin Hamiltonian to be presented that includes dominant intralayer interactions of J 1ab =0.45 meV, J 2ab =0.03 meV, J 3ab =0.19 meV, consistent with theoretical predictions. Furthermore, despite the quasi-2D behavior, appreciable interlayer interactions of J c =0.031(5) meV are required to model the data. No evidence for anisotropy in the form of a spin gap is observed in the data collected. The measurements on MnPSe 3 are contrasted with those on MnPS 3 and reveal a large increase in the interlayer exchange interaction in MnPSe 3 that may stabilize the similar ordering temperatures in the bulk compounds.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Phenomenological theory of the magnetic 90° helical state

We explore a phenomenological phase diagram for the magnetic helical state with 90° turn angle between neighboring spins in the external magnetic field. Such a state is formed by the Eu spin layers in the superconducting iron arsenide RbEuFe 4 As 4 . The peculiarity of this spin configuration is that it is not realized in the standard Heisenberg model with bilinear exchange interactions. A minimum model allowing for such a state requires the biquadratic nearest-neighbor interaction term. In addition, in tetragonal materials, the 90° helix state may be stabilized by the in-plane fourfold anisotropy term, which also fixes helix orientation with respect to the crystal lattice. Such a system has a very rich behavior in the external magnetic field. The magnetic field induces the metamagnetic transition to the double-periodic state with the moment angles (α α -α,-α) with respect to the field for the four subsequent spins. The transition field to this state from the deformed helix is determined by the strength of biquadratic interaction. The transition is second-order for small biquadratic coupling and becomes first-order when this coupling exceeds the critical value. On the other hand, the aligned state at high magnetic field becomes unstable with respect to the formation of an incommensurate fan state, which transforms into the double-periodic state with decreasing magnetic field. The range of this incommensurate state near the saturation field is proportional to square of the biquadratic coupling. In addition, when the magnetic field is applied along one of four the equilibrium moment directions, the deformed helix state experience the first-order rotation transition at the field determined by the fourfold anisotropy.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Large–scale asymmetry in galaxy spin directions: Analysis of galaxies with spectra in DES, SDSS, and DESI Legacy Survey

Multiple previous studies using several different probes have shown considerable evidence for the existence of cosmological–scale anisotropy and a Hubble–scale axis. One of the probes that show such evidence is the distribution of the directions toward which galaxies spin. The advantage of the analysis of the distribution of galaxy spin directions compared to the cosmic microwave background anisotropy is that the ratio of galaxy spin directions is a relative measurement, and therefore less sensitive to background contamination such as Milky Way obstruction. Another advantage is that many spiral galaxies have spectra, and therefore allow to analyze the location of such axis relative to Earth. This paper shows an analysis of the distribution of the spin directions of over 90K galaxies with spectra. That analysis is also compared to previous analyses using the Earth–based Sloan Digital Sky Survey, Panoramic Survey Telescope and Rapid Response System, and Dark Energy Spectroscopic Instrument Legacy Survey, as well as space–based data collected by Hubble Space Telescope. Finally, the results show very good agreement between the distribution patterns observed with the different telescopes. The dipole or quadrupole axes formed by the spin directions of the galaxies with spectra do not necessarily go directly through Earth.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2024

Assessing spin-density wave formation in La 3 Ni 2 O 7 from electronic structure calculations

Here, we employ correlated density-functional theory methods (DFT + Hubbard U) to investigate the spin-density wave state of the bilayer Ruddlesden-Popper (RP) nickelate La 3 Ni 2 O 7 which becomes superconducting under pressure. We predict that the ground state of this bilayer RP material has traits of both the double spin-stripe and the single spin-charge stripe phases proposed in the literature as it corresponds to in-plane up/up′/down/down′ diagonal stripes with up/down being high spin (formally Ni 2+ : d 8 ), and up′ /down′ being low spin (formally Ni 3+ : d 7 ). The main feature of this solution (that is insulating even at U = 0) is the dominant role of the d x 2 −y 2 bands around the Fermi level, which would become doped with the introduction of electrons via oxygen vacancies. In spite of the similarity with cuprates in terms of the dominant role of d x 2 −y 2 bands, some differences are apparent in the magnetic ground state of La 3 Ni 2 O 7 : the antiferromagnetic out-of-plane coupling within the bilayer (linked to the d z 2 orbitals forming a spin-singlet-like configuration) is found to be the dominant one while in-plane interactions are reduced due to the stripe order of the ground state. With pressure, this striped magnetic ground state remains similar in nature but the increase in bandwidth quickly transitions La 3 Ni 2 O 7 into a metallic state with all the activity close to the Fermi level involving, to a large extent, d x 2 −y 2 orbitals. This is reminiscent of the cuprates and may provide key insights into how superconductivity arises in this material under pressure.

LaBollita, Harrison↗

DOE OSTI2025

ZnO quantum dot–molecule conjugates: Chemical interactions, charge dynamics, and spin polarization

Conjugates between molecules and quantum dots (QDs) have been explored for a range of potential applications from photocatalysis and photovoltaics to quantum information science technologies. A particularly ubiquitous material in many of these applications are ZnO QDs since they can accept and transport electrons and can also act as hosts for unique spin states. Conjugates between molecular light absorbers and ZnO QDs have been explored for decades as components in dye-sensitized solar cells. Recently, these materials have also attracted interest for their ability to produce spin-polarized states upon photoexcitation. The current paper employs a series of light absorbing perylene molecules with different ZnO QD sizes to explore key features of these QD–molecule conjugates: (1) chemical interactions, (2) charge dynamics, and (3) spin polarization. The chemical interactions between the molecules and QDs are determined with binding equilibria and reveal dramatic impact of ligand size. The charge transfer dynamics from photoexcited perylenes to ZnO QDs were found to depend exponentially on the linker length. Finally, time-resolved electron paramagnetic resonance experiments reveal that these conjugates generate spin-polarized states in the form of radical pairs and triplets. These spin states hold promise as potential qubits and also offer an avenue to efficiently sensitize molecular triplets.

Hernandez, Frida S. [Amherst College, MA (United S↗

DOE OSTI2020

Proton form factor ratio μ p G E p / G M p from double spin asymmetry

We report the ratio of the electric and magnetic form factor of the proton, $\mu_p G_E^p/G_M^p$, has been measured for elastic electron-proton scattering with polarized beam and target up to four-momentum transfer squared, $Q^2=5.66$ (GeV/c)$^2$ using the double spin asymmetry for target spin orientation aligned nearly perpendicular to the beam momentum direction. This measurement of $\mu_p G_E^p/G_M^p$ agrees with the $Q^2$ dependence of previous recoil polarization data and reconfirms the discrepancy at high $Q^2$ between the Rosenbluth and the polarization-transfer method with a different measurement technique and systematic uncertainties uncorrelated to those of the recoil-polarization measurements. The form factor ratio at $Q^2$=2.06 (GeV/c)$^2$ has been measured as $\mu_p G_E^p/G_M^p = 0.720 \pm 0.176_{stat} \pm 0.039_{sys}$, which is in agreement with an earlier measurement with the polarized target technique at similar kinematics. The form factor ratio at $Q^2$=5.66 (GeV/c)$^2$ has been determined as $\mu_p G_E^p/G_M^p=0.244\pm0.353_{stat}\pm0.013_{sys}$, which represents the highest $Q^2$ reach with the double spin asymmetry with polarized target to date.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

Ubiquitous spin freezing in the superconducting state of UTe 2

In most superconductors electrons form Cooper pairs in a spin-singlet state mediated by either phonons or by long-range interactions such as spin fluctuations. The superconductor UTe 2 is a rare material wherein electrons are believed to form pairs in a unique spin-triplet state with potential topological properties. While spin-triplet pairing may be mediated by ferromagnetic or antiferromagnetic fluctuations, experimentally, the magnetic properties of UTe 2 are unclear. By way of muon spin rotation/relaxation (μSR) measurements on independently grown UTe 2 single crystals we demonstrate the existence of magnetic clusters that gradually freeze into a disordered spin frozen state at low temperatures. Our findings suggest that inhomogeneous freezing of magnetic clusters is linked to the ubiquitous residual linear term in the temperature dependence of the specific heat (C) and the low-temperature upturn in C/T versus T. The omnipresent magnetic inhomogeneity has potential implications for experiments aimed at establishing the intrinsic low-temperature properties of UTe 2 .

36 MATERIALS SCIENCE↗

DOE OSTI2023

Solution phase high repetition rate laser pump x-ray probe picosecond hard x-ray spectroscopy at the Stanford Synchrotron Radiation Lightsource

We present a dedicated end-station for solution phase high repetition rate (MHz) picosecond hard x-ray spectroscopy at beamline 15-2 of the Stanford Synchrotron Radiation Lightsource. A high-power ultrafast ytterbium-doped fiber laser is used to photoexcite the samples at a repetition rate of 640 kHz, while the data acquisition operates at the 1.28 MHz repetition rate of the storage ring recording data in an alternating on-off mode. The time-resolved x-ray measurements are enabled via gating the x-ray detectors with the 20 mA/70 ps camshaft bunch of SPEAR3, a mode available during the routine operations of the Stanford Synchrotron Radiation Lightsource. As a benchmark study, aiming to demonstrate the advantageous capabilities of this end-station, we have conducted picosecond Fe K-edge x-ray absorption spectroscopy on aqueous [FeII(phen)3]2+, a prototypical spin crossover complex that undergoes light-induced excited spin state trapping forming an electronic excited state with a 0.6–0.7 ns lifetime. In addition, we report transient Fe Kβ main line and valence-to-core x-ray emission spectra, showing a unique detection sensitivity and an excellent agreement with model spectra and density functional theory calculations, respectively. Notably, the achieved signal-to-noise ratio, the overall performance, and the routine availability of the developed end-station have enabled a systematic time-resolved science program using the monochromatic beam at the Stanford Synchrotron Radiation Lightsource.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Chiral Dirac Fermion in a Collinear Antiferromagnet

In a Dirac semimetal, the massless Dirac fermion has zero chirality, leading to surface states connected adiabatically to a topologically trivial surface state as well as vanishing anomalous Hall effect. Recently, it is predicted that in the nonrelativistic limit of certain collinear antiferromagnets, there exists a type of chiral "Dirac-like" fermion, whose dispersion manifests four-fold degenerate crossing points formed by spin-degenerate linear bands, with topologically protected Fermi arcs. Such an unconventional chiral fermion, protected by a hidden SU(2) symmetry in the hierarchy of an enhanced crystallographic group, namely spin space group, is not experimentally verified yet. Here, by angle-resolved photoemission spectroscopy measurements, we reveal the surface origin of the electron pocket at the Fermi surface in collinear antiferromagnet CoNb 3 S 6 . Combining with neutron diffraction and first-principles calculations, we suggest a multidomain collinear antiferromagnetic configuration, rendering the the existence of the Fermi-arc surface states induced by chiral Dirac-like fermions. Finally, our work provides spectral evidence of the chiral Dirac-like fermion caused by particular spin symmetry in CoNb 3 S 6 , paving an avenue for exploring new emergent phenomena in antiferromagnets with unconventional quasiparticle excitations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Identification of a new isomeric state in 76 Zn following the β decay of 76 Cu

Background: The evolution of nuclear shell structure far from stability can be explored by identifying and measuring the properties of isomers. Neutron-rich nuclei between the Z = 28 and Z = 50 closed shells have been the subject of recent studies which have identified a number of 0.1 - 10 µs isomers and measured detailed spectroscopic properties. Purpose: The purpose of this analysis was to identify and measure the properties of short-lived isomeric states populated following β decay in Z ≈ 30, N ≈ 50 nuclei near the doubly magic nucleus 78 Ni. Methods: Here, radioactive ions produced by beam fragmentation at the National Superconducting Cyclotron Laboratory were implanted into a CeBr 3 scintillator coupled to a pixelated photomultiplier tube. Ancillary arrays of HPGe clover and LaBr 3 detectors were positioned around the implantation detector to measure β-delayed γ rays. Results: The previously observed 2634-keV level in 76 Zn, populated following the β decay of 76 Cu, was identified as isomeric with a half-life of 25.4(4) ns. A combination of timing and γ-ray spectroscopy was used to confirm this assignment. Shell-model calculations were performed and indicate that this state may be a high-spin negativeparity state formed by the occupation of the ν0g 9/2 orbital. Conclusions: A new isomeric state in 76 Zn has been identified and its half-life was measured. Ambiguity about the structure of this state could be resolved with further experiments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2025

Electrically controlled interlayer trion fluid in electron-hole bilayers

Here, the combination of repulsive and attractive Coulomb interactions in a quantum electron-hole (e-h) fluid can produce correlated phases of multiparticle charge complexes, such as excitons, trions, and biexcitons. We report an experimental realization of an electrically controlled interlayer trion fluid in van der Waals heterostructures. In strongly coupled e-h bilayers, electrons and holes spontaneously form three-particle trion bound states. The interlayer trions can assume 1e-2h and 2e-1h configurations. We show that the two holes in 1e-2h trions form a spin-singlet with a spin gap of approximately one milli–electron volt. By electrostatic gating, the equilibrium state can be continuously tuned into an exciton fluid, a trion fluid, an exciton-trion mixture, or a trion-charge mixture. Our work demonstrates a platform to study correlated phases of tunable Bose-Fermi mixtures.

Qi, Ruishi [University of California, Berkeley, CA↗

DOE OSTI2023

Carbon nanofibers based carbon–carbon composite fibers

Textile grade polyacrylonitrile (PAN) was used as a precursor material for carbon fiber preparation. E-beam irradiated polyacrylonitrile grafted carbon nanofibers were dispersed in polyacrylonitrile solution (dissolved in dimethyl formamide). Carbon nanofibers (CNF) infused polyacrylonitrile solution was wet spun on a lab-scale wet-spinning setup to form 50 to 70 µm diameter fibers with 3.2 wt.% CNF-PAN, 6.4 wt.% CNF-PAN, and neat PAN. Precursor fibers were characterized for thermal, mechanical and morphological properties using various techniques. Drawing the precursor fibers further enhanced polymer chain orientation and coalesced the voids, enhancing tensile strength and modulus by more than 150% compared to those of the undrawn fibers. Precursor composite fibers on carbonization showed enhanced strength, compared to that of pristine PAN fibers, by four times and stiffness by 14 times. The carbon–carbon composite fibers were further characterized with SEM/FIB, XRD and tensile strength. The property improvements were dependent on the uniform distribution of carbon nanofibers, and surface modification of carbon nanofibers further enabled their dispersion in the composite fibers. Furthermore, 3.2 wt.% CNFs in PAN fibers showed maximum improvement in properties compared to 6.4 wt.% CNF in PAN fibers, indicating that the property enhancements go through a maximum and then drop off due to challenge in getting uniform distribution of nanofibers.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Efficient Silicon Carbide (SiC) Fiber Manufacture: Continuous Processing of Novel Precursors via Modified Material Handling

General Atomics Electromagnetic Systems (GA-EMS) together with The Nonwovens Institute (NWI) and Harper International have executed on a development project to improve the production efficiency and reduce the production cost of silicon carbide (SiC) fiber – a critical material that advances US energy security and aerospace leadership. In the first budget period (BP1), the modified tow throughput (MTT) apparatus was developed, enabling fiber spinning in the form of loose coils rather than tightly packed spools (Figure 1) for batch processing of SiC fiber. This coil-based approach was proven to be capable of uniform fiber crosslinking and ceramic conversion, as well as demonstrating key process efficiencies while meeting the program fiber property targets.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Instanton Effects in Euclidean vacuum, Real Time Production, and in the Light-front Wave Functions

Nontrivial topological structures of non-Abelian gauge fields were discovered in the 1970s. Instanton solutions, describing vacuum tunneling through topological barriers, have fermionic zero modes which are at the origin of ‘t Hooft effective Lagrangian. In the 1980s, instanton ensembles have been used to explain chiral symmetry breaking. In the 1990s, a large set of numerical simulations were performed deriving Euclidean correlation functions. The special role of scalar diquarks in nucleons and color superconductivity in dense quark matter has been elucidated. In these lectures, we discuss further developments of physics related to gauge topology. We show that the instanton–anti-instanton “streamline” configurations describe “sphaleron transitions” in high-energy collisions, which result in production of hadronic clusters with nontrivial topological/chiral charges. (They are not yet observed, but discussions of dedicated experiments at the LHC and RHIC are ongoing.) Another new direction is instanton effects in hadronic spectroscopy, both in the rest frame and on the light front. We will discuss their role in central and spin-dependent potentials, form factors and antiquark nuclear “sea”. Finally, we summarize the advances in the semiclassical theory of deconfinement, and chiral phase transitions at finite temperature, in QCD, and in some of its “deformed” versions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

Tracking the Light-Induced Excited-State Dynamics and Structural Configurations of an Extraordinarily Long-Lived Metastable State at Room Temperature

Time-resolved X-ray (Tr-XAS) and optical transient absorption (OTA) spectroscopy in the pico-microsecond time scale coupled with Density Functional theory calculations are applied to study the light-induced spin crossover processes of a Fe-based macrocyclic complex in solution. Tr-XAS analysis after light illumination shows the formation of a seven-coordinated high spin quintet metastable state which relaxes to a six-coordinated high spin configuration before decaying to ground state. Kinetic analysis of the macrocyclic complex reveals an unprecedented long-lived decay lifetime of ~42.6 µs. Comparative studies with a non-macrocyclic counterpart illustrate a significantly shortened ~568-old decay lifetime of ~75 ns, and highlight the importance of the ligand arrangement in stabilizing the reactivity of the excited state. Lastly, OTA analysis shows the seven-coordinated high spin state to be formed within ~6.2 ps. Finally, these findings provide a complete understanding of the spin crossover reaction and relaxation pathways of the macrocyclic complex, and reveal the importance of a flexible coordination environment for their rational design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗