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At least 1,261 records · Page 70

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DOE OSTI2021

Conduction via surface states in antiferromagnetic Mott-insulating Ni S 2 single crystals

Pyrite structure transition-metal disulfides exhibit diverse ground states vs d-band filling, spanning diamagnetic semiconducting, ferromagnetic metallic, antiferromagnetic Mott insulating, and superconducting in FeS 2 , CoS 2 , NiS 2 , and CuS 2 . NiS is particularly interesting and poorly understood as its Mott insulating behavior is accompanied by complex antiferromagnetic ordering below ~38 K and perplexing weak ferromagnetism below ~30 K. Temperature-, pressure-, and composition-dependent insulator-metal transitions also occur, particularly in bandwidth-controlled NiS 2–x Se x , hole-doped Ni 1–x Co x S 2 , etc. Here, we use high-quality chemical-vapor-transport-grown NiS 2 single crystals characterized by x-ray diffraction, energy-dispersive x-ray spectroscopy, magnetometry, and extensive transport and magnetotransport measurements, to generate new insight into this system. In particular, resistivity, magnetoresistance, and Hall effect analyses vs temperature, thickness, and surface preparation, provide unequivocal evidence of surface conduction, where the more conductive surface shunts essentially all current at low temperatures. The surface transport changes from two dimensional and insulating to three dimensional and metallic as the surface preparation is varied (also displaying intriguing sensitivity to magnetic ordering), significantly clarifying literature ambiguities with respect to the electronic ground state. These results have immediate implications. First, the temperature-, pressure-, and composition-dependent insulator-metal transitions deduced in the extensive prior work on NiS 2-x Se x , Ni 1–x Co x S 2 , etc., must clearly be reexamined in light of rife metallic surface conduction, not previously taken into account. Second, NiS 2 now joins FeS 2 and CoS 2 as systems in which bulk and surface electronic behaviors are strikingly different, suggesting that metallic surface states could be a universal feature of pyrite structure transition-metal disulfides.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Magnetic polaron formation in EuZn2P2

Colossal magnetoresistance (CMR) has been observed across many Eu2+-based materials; however, its origin is not completely understood. Here we investigate the antiferromagnetic insulator EuZn2⁢P2 through single crystal x-ray diffraction, transmission electron microscopy, electrical transport, magnetization, dilatometry, and electron spin resonance measurements complemented by density functional theory calculations. Our electrical resistivity data reveal a large negative magnetoresistance, MR=[𝑅⁡(𝐻)−𝑅⁡(0)]/𝑅⁡(0), that reaches MR=−99.7% at 9 T near the antiferromagnetic ordering temperature 𝑇𝑁=23K. Dilatometry measurements show an accompanying field-induced lattice strain. Additionally, Eu2+ electron spin resonance reveals a strong ferromagnetic exchange interaction between Eu2+ and conduction electrons. Our experimental results in EuZn2⁢P2 are consistent with a magnetic polaron scenario and suggest magnetic polaron formation as a prevailing explanation of CMR in Eu2+-based compounds.

Cook, Matt [ORNL] (ORCID:0000000288777505)↗

DOE OSTI2014

Ferromagnetic-nonmagnetic and metal-insulator phase transitions at the interfaces of KTaO{sub 3} and PbTiO{sub 3}

We studied the electronic and magnetic properties of hole doped KTaO{sub 3}/PbTiO{sub 3} interface using density functional theory methods. Ferromagnetic-nonmagnetic phase transition and metal-insulator phase transition occur simultaneously at the interface with ferroelectric polarization reversal. Furthermore, these two transitions are coupled with each other because hole doping with large concentration of holes gives rise to ferromagnetism. The interfacial magnetization, which is proportional to hole concentration at the interface, can be tuned by ferroelectric polarization, leading to strong intrinsic magnetoelectric effect at the interface of originally nonmagnetic KTaO{sub 3} and PbTiO{sub 3}.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Competing Easy-Axis Anisotropies Impacting Magnetic Tunnel Junction-Based Molecular Spintronics Devices (MTJMSDs)

Molecular spintronics devices (MSDs) attempt to harness molecules’ quantum state, size, and configurable attributes for application in computer devices—a quest that began more than 70 years ago. In the vast number of theoretical studies and limited experimental attempts, MSDs have been found to be suitable for application in memory devices and futuristic quantum computers. MSDs have recently also exhibited intriguing spin photovoltaic-like phenomena, signaling their potential application in cost-effective and novel solar cell technologies. The molecular spintronics field’s major challenge is the lack of mass-fabrication methods producing robust magnetic molecule connections with magnetic electrodes of different anisotropies. Another main challenge is the limitations of conventional theoretical methods for understanding experimental results and designing new devices. Magnetic tunnel junction-based molecular spintronics devices (MTJMSDs) are designed by covalently connecting paramagnetic molecules across an insulating tunneling barrier. The insulating tunneling barrier serves as a mechanical spacer between two ferromagnetic (FM) electrodes of tailorable magnetic anisotropies to allow molecules to undergo many intriguing phenomena. Our experimental studies showed that the paramagnetic molecules could produce strong antiferromagnetic coupling between two FM electrodes, leading to a dramatic large-scale impact on the magnetic electrode itself. Recently, we showed that the Monte Carlo Simulation (MCS) was effective in providing plausible insights into the observation of unusual magnetic domains based on the role of single easy-axis magnetic anisotropy. Here, we experimentally show that the response of a paramagnetic molecule is dramatically different when connected to FM electrodes of different easy-axis anisotropies. Motivated by our experimental studies, here, we report on an MCS study investigating the impact of the simultaneous presence of two easy-axis anisotropies on MTJMSD equilibrium properties. In-plane easy-axis anisotropy produced multiple magnetic phases of opposite spins. The multiple magnetic phases vanished at higher thermal energy, but the MTJMSD still maintained a higher magnetic moment because of anisotropy. The out-of-plane easy-axis anisotropy caused a dominant magnetic phase in the FM electrode rather than multiple magnetic phases. The simultaneous application of equal-magnitude in-plane and out-of-plane easy-axis anisotropies on the same electrode negated the anisotropy effect. Our experimental and MCS study provides insights for designing and understanding new spintronics-based devices.

42 ENGINEERING↗

DOE OSTI2022

Absence of spin susceptibility decrease in a bulk organic superconductor with triangular lattice

The study of non-s-wave unconventional superconductivities in strongly correlated electron systems has been a central issue in condensed matter physics for more than 30 years. In such unconventional superconductivities, d-wave Cooper pairing with antiparallel spins has been often observed in various quasi-two-dimensional (quasi-2D) bulk systems. Interestingly, many theories predicted that the triangular lattice causes the d-wave pairing to be unstable and may lead to more exotic pairing such as parallel spin (spin-triplet) pairing. Here we focus on a bulk organic triangular-lattice system in which superconductivity emerges near a nonmagnetic Mott insulating phase. We demonstrate, by using low-power nuclear magnetic resonance (NMR) measurements, that the spin susceptibility of the superconducting state retains the normal state value even deep in the superconducting state. This result indicates the possibility that the material exhibits spin-triplet superconductivity. Our finding will bring insights also into understanding the 2D materials with triangular moiré superlattices that are considered also to show unconventional superconductivities near Mott-like insulating states.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Nonequilibrium optical response of a one-dimensional Mott insulator

We define, compute, and analyze the nonequilibrium differential optical conductivity of the one-dimensional extended Hubbard model at half-filling after applying a pump pulse, using the time-dependent density matrix renormalization group method. The melting of the Mott insulator is accompanied by a suppression of the local magnetic moment and ensuing photogeneration of doublon-holon pairs. The differential optical conductivity reveals (i) mid-gap states related to parity-forbidden optical states and (ii) strong renormalization and hybridization of the excitonic resonance and the absorption band, yielding a Fano resonance. We offer evidence and interpret such a resonance as a signature of nonequilibrium optical excitations resembling excitonic strings, (bi)excitons, and unbound doublon-holon pairs, depending on the magnitude of the intersite Coulomb repulsion. We discuss our results in the context of pump and probe spectroscopy experiments on organic Mott insulators.

1-dimensional systems↗

DOE OSTI2022

Doping-driven resistive collapse of the Mott insulator in a minimal model for VO 2

Here we study the resistive collapse of the Mott insulator state in the dimer Hubbard model. This minimal model has been used to describe the physics of VO 2 , and should be relevant to other strongly correlated materials. It incorporates the physics of correlated dimers and the explicit competition between on-site Coulomb repulsion and magnetic exchange interactions. Our results unveil that between the Mott insulator at half filling and the Fermi liquid metal at high doping there is an intermediate bad metallic phase with exotic features such as a pseudogap, orbital selectivity, and a first-order metal-metal transition. The model is solved within dynamical mean field theory by means of quantum Monte Carlo, which provides the numerically exact solution of the model in the limit of large lattice dimensionality. This model can be considered as a minimal one that captures exotic phenomena associated to the physics of a doped Mott insulator, shading light on their basic physical mechanism.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Interaction between magnetic moments and itinerant carriers in $d^0$ ferromagnetic SiC

Elucidating the interaction between magnetic moments and itinerant carriers is an important step to spintronic applications. In this work, we investigate magnetic and transport properties in d0 ferromagnetic SiC single crystals prepared by postimplantation pulsed laser annealing. Magnetic moments are contributed by the p states of carbon atoms, but their magnetic circular dichroism is different from that in semi-insulating SiC samples. The anomalous Hall effect and negative magnetoresistance indicate the influence of d 0 spin order on free carriers. The ferromagnetism is relatively weak in N-implanted SiC compared with that in Al-implanted SiC after annealing. The results suggest that d 0 magnetic moments and itinerant carriers can interact with each other, which will facilitate the development of SiC spintronic devices with d 0 ferromagnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Implementation of a drive cylinder for low collisional experiments on magnetic reconnection

For most laboratory plasma experiments, Coulomb collisions between the particle species are sufficiently frequent that the particle distribution functions are relaxed to a near-Maxwellian form. This hampers the applicability of such experiments to phenomena observed in tenuous and near-collisionless space plasma. The Terrestrial Reconnection EXperiment (TREX) at the Wisconsin Plasma Physics Laboratory aims to study collisionless reconnection for parameters relevant to the Earth’s magnetosphere. To reduce the role of collisional effects, a reconnection Drive Cylinder has been developed, which increases both the effective system size of the TREX configuration and the rate at which reconnection can be driven. These two effects now permit TREX to reach a kinetic reconnection regime where collisional effects are minimized. The Drive Cylinder is comprised of 12 single loop drive-coils connected in parallel to a 10 kV capacitor bank. Insulated sheets of aluminum are applied to smooth the magnetic fields and enhance the drive efficiency. Following is a description of the technical details and performance of the Drive Cylinder.

Instruments & Instrumentation↗

DOE OSTI2019

Spin Seebeck effect in insulating SrFeO 3–δ films

In SrFeO 3–δ , noncollinear antiferromagnetic spin textures have led to the observation of the topological Hall effect and may give rise to novel magnetic excitations. Here, we measured the spin Seebeck effect in epitaxial, oxygen reduced SrFeO 3–δ films, which are nonferromagnetic and insulating at low temperatures. Here, we detected a spin Seebeck signal below 300K and the signal is enhanced below approximate to 100K, near the ordering temperature of incommensurate antiferromagnetism found in bulk single crystals of SrFeO 3–δ . The spin Seebeck signal increases in magnitude and develops a nonlinear dependence on the magnetic field at lower temperatures. Control experiments were used to verify that the measured signal arises from a spin current and to rule out magnetic proximity effects. Our work shows a detectable spin Seebeck signal in nonferromagnetic insulator SrFeO 3–δ .

36 MATERIALS SCIENCE↗

DOE OSTI2025

Local aging effects in PuB 4 : Growing inhomogeneity and slow dynamics of local field fluctuations probed by 239 Pu NMR

Plutonium-based correlated electron materials host exotic physical phenomena ranging from unconventional heavy-fermion superconductivity to topological Kondo insulating states. Self-irradiation damage can influence many properties of such radioactive materials. Structural disorder effects due to α radiation have been frequently studied using techniques such as transport, thermodynamics, and x-ray diffraction. Here, in this study, we use 239 Pu nuclear magnetic resonance (NMR) to study the long-term influence of self-damage on the lattice and local electronic structures in a single crystal of the candidate topological insulator plutonium tetraboride (PuB 4 ). We first characterize the anisotropy of the 239 Pu resonance and confirm the local axial-site symmetry inferred from previous polycrystalline measurements. Aging effects are then evaluated over the time frame of six years. We find that, though the static 239 Pu NMR spectra show a slight modulation in their shape, their field-rotation pattern reveals no change in 239 Pu local site symmetry over time, suggesting that aging has a surprisingly small impact on the spatial distribution of the static hyperfine field. Further, ligand-site 11 B NMR finds little time-dependent change in the size of electric field gradient around 11 B sites. By contrast, aging has a prominent impact on the 239 Pu NMR relaxation processes and signal intensity. Specifically, aging-induced damage manifests itself as an increase in the spin-lattice relaxation time 𝑇 1 , an increased distribution of 𝑇 1 , and a signal intensity that decreases linearly by 20% per year. An effective spin-spin relaxation time 𝑇 2,eff in the aged sample shortens drastically towards lower temperature, suggesting growth of slow fluctuations of the hyperfine field that are linked to radiation-damage-induced inhomogeneity. Our NMR study sheds light on the interplay of radiation damage and local magnetic interactions in correlated insulators.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

Doping Induced Magnetic and Electronic Phase Transitions in the Ferrimagnetic Half-Metallic Mn 4 Al 11 Compound

The future of spintronics and semiconductor applications demands materials with tailored electronic and magnetic properties. Here, this study uses density functional theory to investigate the electronic structure of the half-metallic compound Mn 4 Al 11 under uniaxial strain and in its Ge-substituted derivatives. Strain analysis shows that although the half-metallic band gap collapses under strain beyond −2%, the ferrimagnetic character remains stable. Ge substitution at six inequivalent Al sites in Mn 4 Al 11 results in varying degrees of metallicity and magnetic properties. Substitution at Al═ (000) induces a metal-to-insulator transition with an indirect semiconducting gap of 0.14 eV. Bonding and hybridization analyses reveal that local Mn–Al interactions due to Ge substitution significantly modify the local electronic structure, causing both electronic and magnetic phase transitions. This work highlights the effectiveness of substitutional doping in tuning half-metallicity and magnetic properties in inorganic solids, enabling the design of materials for future technological applications.

alloys↗

DOE OSTI2023

Metal–insulator transition in composition-tuned nickel oxide films

Abstract Thin films of the solid solution Nd 1 − x La x NiO 3 are grown in order to study the expected 0 K phase transitions at a specific composition. We experimentally map out the structural, electronic and magnetic properties as a function of x and a discontinuous, possibly first order, insulator–metal transition is observed at low temperature when x = 0.2. Raman spectroscopy and scanning transmission electron microscopy show that this is not associated with a correspondingly discontinuous global structural change. On the other hand, results from density functional theory (DFT) and combined DFT and dynamical mean field theory calculations produce a 0 K first order transition at around this composition. We further estimate the temperature-dependence of the transition from thermodynamic considerations and find that a discontinuous insulator–metal transition can be reproduced theoretically and implies a narrow insulator–metal phase coexistence with x . Finally, muon spin rotation ( µ SR) measurements suggest that there are non-static magnetic moments in the system that may be understood in the context of the first order nature of the 0 K transition and its associated phase coexistence regime.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Atomic-Scale Modulation of Synthetic Magnetic Order in Oxide Superlattices

We report atomic-scale precision control of magnetic interactions facilitates a synthetic spin order useful for spintronics, including advanced memory and quantum logic devices. Conventional modulation of synthetic spin order has been limited to metallic heterostructures that exploit Ruderman–Kittel–Kasuya–Yosida interaction through a nonmagnetic metallic spacer; however, they face issues arising from Joule heating and/or electric breakdown. The practical realization and observation of a synthetic spin order across a nonmagnetic insulating spacer will lead to the development of spin-related devices with a completely different concept. Herein, the atomic-scale modulation of the synthetic spiral spin order in oxide superlattices composed of ferromagnetic metal and nonmagnetic insulator layers is reported. The atomically controlled superlattice exhibits an oscillatory magnetic behavior, representing the existence of a spiral spin structure. Depth-sensitive polarized neutron reflectometry evidences modulated spiral spin structures as a function of the nonmagnetic insulator layer thickness. Atomic-scale customization of the spin state can move the field one step further to actual spintronic applications.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2021

Competing magnetic states in transition metal dichalcogenide moiré materials

Small-twist-angle transition metal dichalcogenide (TMD) heterobilayers develop isolated flat moiré bands that are approximately described by triangular lattice generalized Hubbard models. In this paper we explore the metallic and insulating states that appear under different control conditions at a density of one electron per moiré period and the transitions between them. By combining fully self-consistent Hartree-Fock theory calculations with strong-coupling expansions around the atomic limit, we identify four different magnetic states and one nonmagnetic state near the model phase diagram’s metal-insulator phase transition line. Here, ferromagnetic insulating states, stabilized by nonlocal direct exchange interactions, are surprisingly prominent.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2014

High-pressure synthesis, crystal structure and magnetic properties of double perovskite oxide Ba{sub 2}CuOsO{sub 6}

A new compositional double perovskite oxide Ba{sub 2}CuOsO{sub 6} was synthesized under high-pressure (6 GPa) and high-temperature (1500 °C) conditions. The polycrystalline Ba{sub 2}CuOsO{sub 6} was characterized by synchrotron X-ray diffraction, thermogravimetric analysis, and magnetic susceptibility, isothermal magnetization, and specific heat measurements. The oxide crystallizes in a double-perovskite structure with an I4/m space group, in which Os(VI) and Cu(II) are ordered in the perovskite B-site. Ba{sub 2}CuOsO{sub 6} is electrically insulating with an activation energy of 0.813(2) eV and shows antiferromagnetic-like characteristics at temperatures of ∼55 K and ∼70 K. The results of the first-principle calculation suggested that the spin–orbit interaction of Os(VI) plays a substantial role in the insulating state. The Jahn–Teller distortion of CuO{sub 6} octahedra influences the magnetic characteristics with regard to possible two-dimensional magnetic correlations. - Graphical abstract: A new compositional double perovskite oxide Ba{sub 2}CuOsO{sub 6} synthesized by a high-pressure (6 GPa) and high-temperature (1500 °C) method. - Highlights: • A new compositional double perovskite oxide Ba{sub 2}CuOsO{sub 6} was synthesized. • Ba{sub 2}CuOsO{sub 6} is electrically insulating and antiferromagnetic below ∼70 K. • The Jahn–Teller distortion of CuO{sub 6} has relevance to possible magnetic anisotropy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Microscopic subsurface characterization of layered magnetic materials using magnetic resonance force microscopy

This project resulted in the following accomplishments: 1) The invention of scanned probe ferromagnetic resonance microscopy. Upon implementation and refinement this approach was used to measure static and dynamic magnetic resonance properties of ferromagnets with an unprecedented combination of spectral and spatial resolution. 2) Demonstration and study of spin pumping in a pristine ferromagnet across a boundary defined entirely by a magnetic field gradient, and so free of materials discontinuities. 3) First demonstrated highly efficient dynamic spin injection from Y 3 Fe 5 O 12 (YIG) into NiO, an antiferromagnetic (AF) insulator and robust spin propagation in AF NiO over distances up to 100-nm thickness; both spin injection and spin transport are mediated by the AF spin correlations. 4) Demonstration of exceptionally high efficiency conversion of spin current to charge current achieved in spin pumping from the dynamic magnetization of a ferromagnetic insulator into a variety of adjacent metal films. 5) Seminal study of the nature of spin-orbit coupling in d-electron metals that revealed the dominant sensitivity of the d-orbital moment to the d-electron count and revealing the important roles of both d-electron configuration and atomic number in the physics of the spin Hall effect. 6) Demonstration of observation of FMR by means of optically-detected NV diamond relaxometry that provided a highly sensitive, spatially resolved FMR detection method and revealed spin pumping across 100-nm length scales by means of dipolar coupling. 7) Using magnetic field localization, developed for FMR imaging, demonstrated a novel approach to discretizing spin wave modes to improve the characteristics of auto-oscillators driven by pure spin currents produced by the spin Hall effect. 8) We demonstrated large spin pumping signals from propagating high wavevector spinwaves in thin film YIG find that the spin pumping efficiency was insensitive to wavevector thus emphasizing the promise of thin YIG films for spinwave-based spintronics by allowing for predictable down-scaling of device dimensions and enabling a broad range of operational frequencies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Ferromagnetic superexchange in insulating Cr 2 MoO 6 by controlling orbital hybridization

We report the magnetic and electronic structures of the newly synthesized inverse-trirutile compound Cr 2 MoO 6 . Despite the same crystal symmetry and similar bond-lengths and bond-angles to Cr 2 TeO 6 , Cr 2 MoO 6 possesses a magnetic structure of the Cr 2 MoO 6 type, different from that seen in Cr 2 TeO 6 . Ab-initio electronic structure calculations show that the sign and strength of the Cr-O-Cr exchange coupling is strongly influenced by the hybridization between Mo 4d and O 2p orbitals. This result further substantiates our recently proposed mechanism for tuning the exchange interaction between two magnetic atoms by modifying the electronic states of the non-magnetic atoms in the exchange path through orbital hybridization. This approach is fundamentally different from the conventional methods of controlling the exchange interaction by either carrier injection or through structural distortions.

36 MATERIALS SCIENCE↗