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At least 91 records · Page 5

Interlayer engineering of Fe 3 GeTe 2 : From 3D superlattice to 2D monolayer

The discoveries of ferromagnetism down to the atomically thin limit in van der Waals (vdW) crystals by mechanical exfoliation have enriched the family of magnetic thin films [C. Gong et al., Nature 546 , 265–269 (2017) and B. Huang et al., Nature 546 , 270–273 (2017)]. However, compared to the study of traditional magnetic thin films by physical deposition methods, the toolbox of the vdW crystals based on mechanical exfoliation and transfer suffers from low yield and ambient corrosion problem and now is facing new challenges to study magnetism. For example, the formation of magnetic superlattice is difficult in vdW crystals, which limits the study of the interlayer interaction in vdW crystals [M. Gibertini, M. Koperski, A. F. Morpurgo, K. S. Novoselov, Nat. Nanotechnol. 14 , 408–419 (2019)]. Here, we report a strategy of interlayer engineering of the magnetic vdW crystal Fe 3 GeTe 2 (FGT) by intercalating quaternary ammonium cations into the vdW spacing. Both three-dimensional (3D) vdW superlattice and two-dimensional (2D) vdW monolayer can be formed by using this method based on the amount of intercalant. On the one hand, the FGT superlattice shows a strong 3D critical behavior with a decreased coercivity and increased domain wall size, attributed to the co-engineering of the anisotropy, exchange interaction, and electron doping by intercalation. On the other hand, the 2D vdW few layers obtained by over-intercalation are capped with organic molecules from the bulk crystal, which not only enhances the ferromagnetic transition temperature ( T C ), but also substantially protects the thin samples from degradation, thus allowing the preparation of large-scale FGT ink in ambient environment.

36 MATERIALS SCIENCE↗

Spin injection by spin–charge coupling in proximity induced magnetic graphene

Abstract Within the field of spintronics major efforts are directed towards developing applications for spin-based transport devices made fully out of two-dimensional materials. In this work we present an experimental realization of a spin-valve device where the generation of the spin signal is exclusively attributed to the spin-dependent conductivity of the magnetic graphene resulting from the proximity of an interlayer antiferromagnet, chromium sulfide bromide (CrSBr). We clearly demonstrate that the usage of the conventional air-sensitive 3D magnetic contacts can be fully avoided when graphene/CrSBr heterostructures are employed. Moreover, apart from providing exceptionally long spin relaxation length, the usage of graphene for both generation and transport of the spin allows to automatically avoid the conductivity mismatch between the source and the channel circuits that has to be considered when using conventional low-resistive contacts. Our results address a necessary step in the engineering of spintronic circuitry out of layered materials and precede further developments in the area of complex spin-logic devices. Moreover, we introduce a fabrication procedure where we designed and implemented a recipe for the preparation of electrodes via a damage-free technique that offers an immediate advantage in the fields of air-sensitive and delicate organic materials.

36 MATERIALS SCIENCE↗

Twisted bilayers of thin film magnetic topological insulators

Twisted bilayer graphene (TBG) near "magic angles" has emerged as a rich platform for strongly correlated states of two-dimensional (2D) Dirac semimetals. Here we show that twisted bilayers of thin film magnetic topological insulators (MTIs) with large in-plane magnetization can realize flat bands near 2D Dirac nodes. Using a simple model for thin films of MTIs, we derive a continuum model for two such MTIs, twisted by a small angle with respect to each other. When the magnetization is in plane, we show that interlayer tunneling terms act as effective SU (2) vector potentials, which are known to lead to flat bands in TBG. We show that by changing the in-plane magnetization, it is possible to tune the twisted bilayer MTI band dispersion to quadratic band touching or to flat bands, similar to the TBG. If realized, this system can be a highly tunable platform for strongly correlated phases of two-dimensional Dirac semimetals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Magnetic evolution induced by freezing of Ag + fluctuations in an intercalated transition metal dichalcogenide

Here, we present a comprehensive study on the magnetic evolution processes in AgCrSe 2 using both neutron scattering and theoretical calculations. Additionally, the development of magnetic short-range correlation with decoupled interlayer interactions is confirmed between 55 and 200 K. Significant magneto-crystalline anisotropy energy around 0.1 meV of Cr 3+ is identified that mainly contributes to the robust existence of the in-plane magnetic correlations in the magnetic short-order regime. Furthermore, the indirect superexchange interactions through Cr-Se-Ag-Se-Cr path between the adjacent CrSe 6 octahedral layers is also demonstrated. In combination with the mutual coupling among multiple degrees of freedom (spin, phonon, lattice, and dipole), we reveal the key role of the freezing of Ag + fluctuations in preventing interlayer exchange interactions from decoupling.

36 MATERIALS SCIENCE↗

Strong Zeeman splitting in orbital-hybridized valleytronic interfaces

We report stacked heterointerfaces of two-dimensional (2D) materials are well-suited to obtain novel electronic functionality at small length scales, because the intrinsic properties of both materials can be blended by interlayer coupling with remarkable effects on the electronic band structure. In particular, band degeneracy at the K and K' Brillouin zone valleys of 2D materials can be broken by symmetry reductions by applying an external magnetic field, with possible application in valleytronic devices. Nevertheless, this usually requires impractically large external magnetic fields > 100 T. An alternative and more practical route is provided via stacking a non-centrosymmetric layered material on a magnetic substrate to induce valley splitting through the magnetic proximity effect; however, the splitting magnitude can vary sharply between similar interfaces. In this work, first-principle calculations are used to calculate the valley splitting of eight low-strain interfaces with transition metal dichalcogenides stacked on 2D magnetic substrates. It is shown that the interlayer band hybridization plays a major role when the two layers’ bands are closely aligned in energy, with the resulting band repulsion and the total valley splitting being strongly dependent on the Hubbard U correction , showing up to an order of magnitude change. The WSe 2 /CrGeTe 3 interface in particular shows strong interlayer interactions, which can potentially lead to a significantly high valley splitting of 26 meV; however further experimental investigations will be needed to resolve uncertainties in the predicted valley splitting.

36 MATERIALS SCIENCE↗

Exchange bias in La 0.7 Sr 0.3 CrO 3 /La 0.7 Sr 0.3 MnO 3 /La 0.7 Sr 0.3 CrO 3 heterostructures

In the recent past, heterostructures of magnetic oxide thin films have attracted a great deal of research excitement due to very interesting physical properties such as antiferromagnetic interlayer coupling, tunable exchange-bias, interfacial driven magnetic properties and high mobility electron gas across the interfaces. In this work, we report on the comprehensive magnetic properties observed from the heterostructures of (2 unit cells) La 0.7 Sr 0.3 CrO 3 /(8 unit cells) La 0.7 Sr 0.3 MnO 3 /(2 unit cells) La 0.7 Sr 0.3 CrO 3 , which are epitaxially deposited on SrTiO 3 substrate by plasma-assisted oxide molecular beam epitaxy. Using SQUID magnetometer, the magnetic properties are studied when the magnetic field was applied both in plane and out of plane. The Curie temperature of this structure is found to be at 290 K. Most significantly, at 2 K, we observed a complete up/down shift (along magnetization axis) of hysteresis loop when the sample was cooled under a magnetic field of ± 5000 Oe in the in-plane configuration. We believe that the strong antiferromagnetic (super) exchange coupling of Mn-Cr across the two interfaces is responsible for the observed exchange bias. We will present and discuss our in-detailed experimental findings collected on this heterostructure as a function of temperature and magnetic field.

36 MATERIALS SCIENCE↗

Room temperature colossal superparamagnetic order in aminoferrocene–graphene molecular magnets

Intensive studies are published for graphene-based molecular magnets due to their remarkable electric, thermal, and mechanical properties. However, to date, most of all produced molecular magnets are ligand based and subject to challenges regarding the stability of the ligand(s). The lack of long-range coupling limits high operating temperature and leads to a short-range magnetic order. Herein, we introduce an aminoferrocene-based graphene system with room temperature superparamagnetic behavior in the long-range magnetic order that exhibits colossal magnetocrystalline anisotropy of 8 × 10 5 and 3 × 10 7 J/m 3 in aminoferrocene and graphene-based aminoferrocene, respectively. These values are comparable to and even two orders of magnitude larger than pure iron metal. Aminoferrocene [C 10 H 11 FeN] + is synthesized by an electrophilic substitution reaction. It was then reacted with graphene oxide that was prepared by the modified Hammers method. The phase structure and functionalization of surface groups were characterized and confirmed by XRD, FT-IR, and Raman spectroscopy. To model the behavior of the aminoferrocene between two sheets of hydroxylated graphene, we have used density functional theory by placing the aminoferrocene molecule between two highly ordered hydroxylated sheets and allowing the structure to relax. Here, the strong bowing of the isolated graphene sheets suggests that the charge transfer and resulting magnetization could be strongly influenced by pressure effects. In contrast to strategies based on ligands surface attachment, our present work that uses interlayer intercalated aminoferrocene opens routes for future molecular magnets as well as the design of qubit arrays and quantum systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

K 2 Co 2 TeO 6 : A layered magnet with a S = 1 2 Co 2 + honeycomb lattice

Recent observations of Kitaev interactions in d 7 electron configurations have generated research interest in Co 2+ based honeycomb magnets. Here, we report the synthesis of a K 2 Co 2 TeO 6 single crystal. X-ray diffraction and electron microscopy experiments show that K 2 Co 2 TeO 6 crystallizes in a $P$6 3 /$mcm$ space group with undistorted honeycomb layers of Co 2+ ions. Anisotropic magnetic and thermodynamic characterizations demonstrate an effective S = $\frac{1}{2}$ state of Co 2+ at low temperature, competing magnetic phases, and weak magnetic transitions that can be suppressed by applying fields. Moreover, the interlayer K disorder level is tunable by thermal treatments, and it affects the magnetic features obviously. In conclusion, our findings provide a new and promising platform for studying Kitaev physics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Distinct magneto-Raman signatures of spin-flip phase transitions in CrI 3

The discovery of 2-dimensional (2D) materials, such as CrI 3 , that retain magnetic ordering at monolayer thickness has resulted in a surge of both pure and applied research in 2D magnetism. Here, we report a magneto-Raman spectroscopy study on multilayered CrI 3 , focusing on two additional features in the spectra that appear below the magnetic ordering temperature and were previously assigned to high frequency magnons. Instead, we conclude these modes are actually zone-folded phonons. We observe a striking evolution of the Raman spectra with increasing magnetic field applied perpendicular to the atomic layers in which clear, sudden changes in intensities of the modes are attributed to the interlayer ordering changing from antiferromagnetic to ferromagnetic at a critical magnetic field. Our work highlights the sensitivity of the Raman modes to weak interlayer spin ordering in CrI 3 .

47 OTHER INSTRUMENTATION↗

Enhanced positive and negative exchange bias in FeF 2 /Ni with dusted interfaces

An enhanced exchange bias was found in FeF 2 /Ni interfaces by inserting dusting of Pd and Cu atoms. We have used an ultrathin wedge to investigate systematically the effect of a discontinuous nonmagnetic spacer between the antiferromagnetic and ferromagnetic layers. Negative and positive exchange biases are symmetric and maximized for less than two angstroms of the nonmagnetic layer. Moreover, the dusting reduces the field cooling threshold to switch between the negative and the positive exchange bias. This finding demonstrates that nonmagnetic dusted layers can improve the interfacial exchange energy density in antiferromagnetic/ferromagnetic heterostructures and modify the bulk antiferromagnetic domain structure. Other dusting materials such as Ag, Ti, V, and SiO 2 showed no enhancement in FeF 2 /Ni bilayers, which indicates the atomic sensitivity of this effect.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Widely Tunable Quantum Phase Transition from Moore-Read to Composite Fermi Liquid in Bilayer Graphene

Here, we develop a proposal to realize a widely tunable and clean quantum phase transition in bilayer graphene between two paradigmatic fractionalized phases of matter: the Moore-Read fractional quantum Hall state and the composite Fermi liquid metal. This transition can be realized at total fillings $\textit{ν}$ = ±3 + 1/2 and the critical point can be controllably accessed by tuning either the interlayer electric bias or the perpendicular magnetic field values over a wide range of parameters. We study the transition numerically within a model that contains all leading single particle corrections to the band structure of bilayer graphene and includes the fluctuations between the $\textit{n}$ = 0 and $\textit{n}$ = 1 cyclotron orbitals of its zeroth Landau level to delineate the most favorable region of parameters to experimentally access this unconventional critical point. We also find evidence for a new anisotropic gapless phase stabilized near the level crossing of $\textit{n}$ = 0/1 orbits.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Photo-induced non-collinear interlayer RKKY coupling in bulk Rashba semiconductors

Abstract The interplay between light-matter, spin-orbit, and magnetic interactions allows the investigation of light-induced magnetic phenomena that are otherwise absent without irradiation. We present our analysis of light-driven effects on the interlayer exchange coupling mediated by a bulk Rashba semiconductor in a magnetic multilayer. The collinear magnetic exchange coupling mediated by the photon-dressed spin-orbit coupled electrons of BiTeI develops light-induced oscillation periods and displays new decay power laws, both of which are enhanced with an increasing light-matter coupling. For magnetic layers with non-collinear magnetization, we find a non-collinear magnetic exchange coupling uniquely generated by light-driving of the multilayer. As the non-collinear magnetic exchange coupling mediated by the photon-dressed electrons of BiTeI is unique to the irradiated system and it is enhanced with increasing light-matter coupling, this effect offers a promising platform of investigation of light-driven effects on magnetic phenomena in spin-orbit coupled systems. In this platform, light properties, such as its intensity, can serve as external knobs for inducing non-collinear couplings of the interlayer exchange and for modulating the collinear couplings. Both of these effects signify the photo-generated modification in the spin textures of spin-orbit coupled electrons in BiTeI.

Physics↗

Spin Stripes and Superconductivity in Bilayer Nickelates

The bilayer nickelate La3Ni2O7 has recently emerged as a high-temperature superconductor with unusual spin stripe order in its ambient pressure phase. We propose a microscopic Hamiltonian that faithfully reflects the crystalline symmetry of this system, with the primary aim of addressing its unconventional magnetism at ambient pressure. Using state-of-the-art density matrix renormalization group calculations, we show that (π/2,π/2) spin stripe order arises in our model at sizable Hund's coupling JH from a hidden quasi-one-dimensionality and persists over a range of electron concentrations. In the more symmetric high-pressure regime, our model exhibits enhanced interlayer pairing tendencies when the interlayer antiferromagnetic coupling J⊥ becomes sufficiently large. Our results provide a microscopic origin of the diagonal spin stripes and identify Hund's coupling JH and interlayer coupling J⊥ as key ingredients governing magnetic order and pairing tendencies in La3Ni2O7.

Wang, Hao-Xin [The Chinese University of Hong Kong↗

Synthesis and anisotropic magnetism in quantum spin liquid candidates A YbSe 2 ( A = K and Rb)

The quantum spin liquid (QSL) state in rare-earth triangular lattices has attracted much attention recently due to its potential application in quantum computing and communication. Here, we report the single-crystal growth synthesis, crystal structure characterizations, and magnetic properties of AYbSe 2 (A = K and Rb) compounds. The x-ray diffraction analysis shows that AYbSe 2 (A = K and Rb) crystallizes in a trigonal space group, R-3m (No. 166) with Z = 3. AYbSe 2 possesses a two-dimensional (2D) Yb–Se–Yb layered structure formed by edged-shared YbSe 6 octahedra. The magnetic properties are highly anisotropic for both title compounds, and no long-range order is found down to 0.4 K, revealing the possible QSL ground state in these compounds. The isothermal magnetization exhibits a one-third magnetization plateau when the magnetic fields are applied in the ab-plane. Heat capacity is performed along both ab-plane and c axis and features the characteristic dome for triangular magnetic lattice compounds as a function of magnetic fields. Due to the change in the interlayer and intralayer distance of Yb 3+ , the dome shifts to low fields from KYbSe 2 to RbYbSe 2 . All these results indicate that the AYbSe 2 family presents unique frustrated magnetism close to the possible QSL and noncollinear spin states.

36 MATERIALS SCIENCE↗

Tuning magnetic order in the van der Waals metal $Fe_5GeTe_2$ by cobalt substitution

Fe 5 - x GeTe 2 is a van der Waals material with one of the highest reported bulk Curie temperatures, T C ≈ 310 K . Here, theoretical calculations and experiments are utilized to demonstrate that the magnetic ground state is highly sensitive to local atomic arrangements and the interlayer stacking. Cobalt substitution is found to be an effective way to manipulate the magnetic properties while also increasing the ordering temperature. In particular, cobalt substitution up to ≈ 30 % enhances T C and changes the magnetic anisotropy, while ≈ 50 % cobalt substitution yields an antiferromagnetic state. Single crystal x-ray diffraction evidences a structural change upon increasing the cobalt concentration, with a rhombohedral cell observed in the parent material and a primitive cell observed for ≈ 46 % cobalt content relative to iron. First-principles calculations demonstrate that it is a combination of high cobalt content and the concomitant change to primitive layer stacking that produces antiferromagnetic order. These results illustrate the sensitivity of magnetism in Fe 5 - x GeTe 2 to composition and structure, and emphasize the important role of local structural order-disorder and layer stacking in cleavable magnetic materials.

36 MATERIALS SCIENCE↗

Single crystal growth, chemical defects, magnetic and transport properties of antiferromagnetic topological insulators ( Ge 1 – δ – x Mn x ) 2 Bi 2 Te 5 ( x ≤ 0.47 , 0.11 ≤ δ ≤ 0.20 )

Magnetic topological insulators provide a platform for emergent phenomena arising from the interplay between magnetism and band topology. Here we report the single crystal growth, crystal structure, magnetic and transport properties, as well as the neutron scattering studies of topological insulator series (Ge 1–δ–x Mn x ) 2 ⁢Bi 2 ⁢Te 5 (x ≤ 0.47, 0.11 ≤ δ ≤ 0.20). Upon doping up to x = 0.47, the lattice parameter c decreases by 0.8%, while the lattice parameter a remains nearly unchanged. Significant Ge vacancies and Ge/Bi site mixing are revealed via elemental analysis as well as refinements of the neutron and x-ray diffraction data, resulting in holes dominating the charge transport. At x = 0.47, below 10.8 K, a bilayer A-type antiferromagnetic ordered state emerges, featuring an ordered moment of 3.0(3) μ B /Mn at 5 K, with the c axis as the easy axis. Magnetization data unveils a much stronger effective interlayer antiferromagnetic exchange interaction and a much smaller uniaxial anisotropy compared to MnBi 2 ⁢Te 4 . We attribute the former to the shorter nearest-neighbor Mn-Mn interlayer superexchange path and the latter to the smaller ligand-field splitting in (Ge 1–δ–x ⁢Mn x ) 2 ⁢Bi 2 ⁢Te 5 . Finally, our study demonstrates that this series of materials holds promise for the investigation of the layer Hall effect and quantum metric nonlinear Hall effect.

36 MATERIALS SCIENCE↗

Spin wave theory for the triaxial magnetic anisotropy 2D van der Waals antiferromagnet CrSBr

The magnetic properties of two-dimensional (2D) materials have been attracting increasing attention in recent years due to their unique behavior and possible applications in new devices. One material of great interest is the 2D van der Waals (vdW) crystal CrSBr, which exhibits antiferromagnetic (AF) order at low temperatures due to an interlayer AF exchange interaction. Here, we present a full quantum spin-wave theory for vdW crystals considering one interlayer and three intralayer exchange interactions, and triaxial magnetic anisotropy. The fits of the theoretical results to antiferromagnetic resonance measurements and inelastic neutron scattering data in CrSBr yield reliable values for the seven interaction parameters that can be used to calculate other properties of this interesting material.

2D materials↗

Synthesis, structure and canted antiferromagnetism of layered cobalt hydroxide sorbate

Layered hybrid organic–inorganic compounds of the transition metal hydroxides, in which part of the hydroxide ions are exchanged for organic ligands that act as spacers of the 2-dimensional inorganic layers, elicit new or enhanced properties. The interlayer ligands enable fine-tuning of the physicochemical properties of the metal hydroxide layers, including their magnetism. Specifically, within the Co(OH) 2 family of transition ion hydroxides, this approach has been leveraged to stabilize antiferromagnetic and ferrimagnetic ground states for pillared and layered complexes, respectively. Here, in this work, we further investigate the effects of changing dimensionality, local Co coordination, and interlayer spacing on the magnetic ground state of brucite-like β-Co(OH) layered complexes. We report the hydrothermal synthesis of a new crystalline material, Co(OH)(sorb), where the inorganic layers are spaced by monotopic, doubly unsaturated sorbate ligands (sorb = [C 6 H 7 O 2 ] – ). The material was structurally characterized using powder X-ray and neutron diffraction measurements and the crystal structure was solved ab initio from powder diffraction data and refined using the Rietveld method. The magnetic susceptibility and magnetization measurements reveal canted antiferromagnetic ordering with T N = 41.7 K. This report augments our understanding of tuning magnetism through dimensionality in layered complexes and represents a step forward in the design of new 2D layered hybrid compounds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗