Van der Waals materials composed of stacks of individual atomic layers have attracted considerable attention due to their exotic electronic properties that can be altered by, for example, manipulating the twist angle of bilayer materials or the stacking sequence of trilayer materials. To fully understand and control the unique properties of these few-layer materials, a technique that can provide information about their local in-plane structural deformations, twist direction, and out-of-plane structure is needed. In principle, interference in overlap regions of Bragg disks originating from separate layers of a material encodes three-dimensional information about the relative positions of atoms in the corresponding layers. Here, we describe an interferometric four-dimensional scanning transmission electron microscopy technique that utilizes this phenomenon to extract precise structural information from few-layer materials with nm-scale resolution. We demonstrate how this technique enables measurement of local pm-scale in-plane lattice distortions as well as twist direction and average interlayer spacings in bilayer and trilayer graphene, and therefore provides a means to better understand the interplay between electronic properties and precise structural arrangements of few-layer 2D materials.
Interlayer exchange couplings were examined for Co2FeAl0.5Si0.5(CFAS)/Cr/CFAS trilayered films grown on MgO (001) single crystal and thermally oxidized Si substrates. The films were (001) epitaxial on MgO and (110) textured polycrystalline on SiO2. Strong exchange couplings were observed for the films with the 1.5 nm thick Cr spacer layer. A 90 degree coupling is dominant in the (001) epitaxial film. In contrast, an antiparallel coupling exists in the polycrystalline one. The relationship of interlayer couplings with the structure is discussed.
The manipulation of the antiferromagnetic interlayer coupling in the epitaxial Fe/Cr/Fe(001) trilayer system by moderate 5 keV He ion beam irradiation has been investigated experimentally. It is shown that even for irradiation with very low fluences (10^14 ions/cm^2) a drastic change in strength of the coupling appears. For thin Cr-spacers (below 0.6 - 0.7 nm) the coupling strength decreases with fluence, becoming ferromagnetic for fluences above (2x10^14 ions/cm^2). The effect is connected with the creation of magnetic bridges in the layered system due to atomic exchange events caused by the …
When the thickness of metal film approaches the nanoscale, itinerant carriers resonate between its boundaries and form quantum well states (QWSs), which are crucial to account for the film electrical, transport and magnetic properties. Besides the classic origin of particle-in-a-box, the QWSs are also susceptible to the crystal structures that affect the quantum resonance. Here we investigate the QWSs and the magnetic interlayer exchange coupling (IEC) in the Fe/Ag/Fe (001) trilayer from first-principles calculations. We find that the carriers at the Brillouin-zone center (belly) and edge (nec…
We describe a systematic study of the exchange coupling between a magnetically hard metallic ferromagnet (MnAs) and a magnetically soft ferromagnetic semiconductor (GaMnAs) in bilayer and trilayer heterostructures. An exchange spring model of MnAs/GaMnAs bilayers accounts for the variation of the exchange bias field with layer thickness and composition. We also present evidence for hole-mediated interlayer exchange coupling in MnAs/p-GaAs/\GaMnAs trilayers and study the dependence of the exchange bias field on the thickness of the spacer layer.
Manipulating electronic interlayer coupling in layered van der Waals (vdW) materials is essential for designing opto-electronic devices. Here, we control vibrational and electronic interlayer coupling in bi- and trilayer 2H-MoS$_2$ using large external electric fields in a micro-capacitor device. The electric field lifts Raman selection rules and activates phonon modes in excellent agreement with ab-initio calculations. Through polarization resolved photoluminescence spectroscopy in the same device, we observe a strongly tunable valley dichroism with maximum circular polarization degree of $\s…
Light-induced interlayer spacing dynamics via orbital phonon coupling
Gwangju Institute of Science and Technology (GIST)（光州科学技术院）；Max Planck Institute for the Structure and Dynamics of Matter（马克斯·普朗克物质结构与动力学研究所）；Universidad del País Vasco UPV/EHU（巴斯克大学）；The Flatiron Institute（平顶山研究所）
Vertically stacked van der Waals heterostructures constitute a promising platform for providing tailored band alignment with enhanced excitonic systems. Here we report observations of neutral and charged interlayer excitons in trilayer WSe2-MoSe2-WSe2 van der Waals heterostructures and their dynamics. The addition of a WSe2 layer in the trilayer leads to significantly higher photoluminescence quantum yields and tunable spectral resonance compared to its bilayer heterostructures at cryogenic temperatures. The observed enhancement in the photoluminescence quantum yield is due to significantly la…
Magnetic proximity effect between topological insulator (TI) and ferromagnetic insulator (FMI) is considered to have great potential in spintronics. However, a complete determination of interfacial magnetic structure has been highly challenging. We theoretically investigate the interlayer exchange coupling of two FMIs separated by a TI thin film, and show that the particular electronic states of the TI contributing to the proximity effect can be directly identified through the coupling behavior between two FMIs, together with a tunability of coupling constant. Such FMI/TI/FMI structure not onl…
Correlated interlayer quantum Hall state in large-angle twisted trilayer graphene
Daegu Gyeongbuk Institute of Science and Technology (DGIST)（大邱庆北科学技术院）；Ulsan National Institute of Science and Technology（蔚山科学技术院）；University of Seoul（首尔大学）；Pohang University of Science and Technology（浦项科技大学）；National Institute for Materials Science（物质材料研究机构）；Korea Advanced Institute of Science and Technology（韩国科学技术院）；Institute for Basic Science（基础科学研究所）
Two-dimensional (2D) layered transition metal dichalcogenides (TMDs) have recently attracted tremendous interest as potential valleytronic and nano-electronic materials, in addition to being well-known as excellent lubricants in the bulk. The interlayer van der Waals (vdW) coupling and low frequency phonon modes, and how they evolve with the number of layers, are important for both the mechanical and electrical properties of 2D TMDs. Here we uncover the ultra-low frequency interlayer breathing and shear modes in few-layer MoS2 and WSe2, prototypical layered TMDs, using both Raman spectroscopy …
From monolayers composed of different atoms, we can build structures with spontaneous vertical polarization by conveniently stacking multiple layers. We have studied, using first-principles methods and based on modern polarization theory, a system composed of three layers of hexagonal Boron-Nitride(h-BN) in all possible stackings. We obtain for each of the configurations how charge transfers between the layers and how it impacts on the polarization of the system. In addition, we studied a system of three layers, one of them rotated, and we found that not only did the magnitude of the polarizat…
We present a detailed numerical simulation study of the effects caused by the magnetodipolar interaction between ferromagnetic (FM) layers of a trilayer magnetic nanoelement on its magnetization dynamics. As an example we use a Co/Cu/Ni80Fe20 element with a square lateral shape where the magnetization of FM layers forms a closed Landau-like domain pattern. First we show that when the thickness of the non-magnetic (NM) spacer is in the technology relevant region h ~ 10 nm, magnetodipolar interaction between 90o Neel domain walls in FM layers qualitatively changes the equilibrium magnetization s…
The phonon dispersions of monolayer and few-layer graphene (AB bilayer, ABA and ABC trilayers) are investigated using the density-functional perturbation theory (DFPT). Compared with the monolayer, the optical phonon $E_{2g}$ mode at $Γ$ splits into two and three doubly degenerate branches for bilayer and trilayer graphene, respectively, due to the weak interlayer coupling. These modes are of various symmetry and exhibit different sensitivity to either Raman or infrared (IR) measurements (or both). The splitting is found to be 5 cm$^{-1}$ for bilayer and 2 to 5 cm$^{-1}$ for trilayer graphene.…
The spin-orbit torque, a torque induced by a charge current flowing through the heavy-metal conducting layer with strong spin-orbit interactions, provides an efficient way to control the magnetization direction in heavy-metal/ferromagnet nanostructures, required for applications in the emergent magnetic technologies like random access memories, high-frequency nano oscillators, or bio-inspired neuromorphic computations. We study the interface properties, magnetization dynamics, magnetostatic features and spin-orbit interactions within the multilayer system Ti(2)/Co(1)/Pt(0-4)/Co(1)/MgO(2)/Ti(2)…
Spin transport and magnetic proximity effect in CoFeB/normal metal/Pt trilayers
Rheinland-Pfälzische Technische Universität Kaiserslautern-Landau（莱茵兰-普法尔茨技术大学凯泽斯劳滕-兰道校区）；Instituto de Micro y Nanotecnología, IMN-CNM, CSIC（微型与纳米技术研究所，IMN-CNM，西班牙国家科学研究委员会）；Aristotle University of Thessaloniki（塞萨洛尼基亚里士多德大学）；Johannes Gutenberg University Mainz（美因茨约翰内斯古腾堡大学）
We demonstrate that surface relaxation, which is insignificant in trilayer graphene, starts to manifest in Bernal-stacked tetralayer graphene. Bernal-stacked few-layer graphene has been investigated by analyzing its Landau level spectra through quantum capacitance measurements. We find that in trilayer graphene, the interlayer interaction parameters were similar to that of graphite. However, in tetralayer graphene, the hopping parameters between the bulk and surface bilayers are quite different. This shows a direct evidence for the surface relaxation phenomena. In spite of the fact that the Va…
Experimental and theoretical studies of manganese deposition on graphene/Ni(111) shows that a thin ferromagnetic Ni3Mn layer, which is protected by the graphene overlayer, is formed upon Mn intercalation. The electronic bands of graphene are affected by Ni3Mn interlayer formation through a slight reduction of n-type doping compared to graphene/Ni(111) and a suppression of the interface states characteristic of graphene/Ni(111). Our DFT-based theoretical analysis of interface geometric, electronic, and magnetic structure gives strong support to our interpretation of the experimental scanning tu…
For epitaxial trilayers of the magnetic rare-earth metals Gd and Tb, exchange coupled through a non-magnetic Y spacer layer, element-specific hysteresis loops were recorded by the x-ray magneto-optical Kerr effect at the rare-earth $M_5$ thresholds. This allowed us to quantitatively determine the strength of interlayer exchange coupling (IEC). In addition to the expected oscillatory behavior as a function of spacer-layer thickness $d_Y$, a temperature-induced sign reversal of IEC was observed for constant $d_Y$, arising from magnetization-dependent electron reflectivities at the magnetic inter…
This work reports on the magnetic interlayer coupling between two amorphous CoFeB layers, separated by a thin Ru spacer. We observe an antiferromagnetic coupling which oscillates as a function of the Ru thickness x, with the second antiferromagnetic maximum found for x=1.0 to 1.1 nm. We have studied the switching of a CoFeB/Ru/CoFeB trilayer for a Ru thickness of 1.1 nm and found that the coercivity depends on the net magnetic moment, i.e. the thickness difference of the two CoFeB layers. The antiferromagnetic coupling is almost independent on the annealing temperatures up to 300 degree C whil…
We report on the influence of stray fields for both low and high magnetic fields applied parallel to trilayers consisting of a low-T Nb interlayer and two outer Ni Fe layers having in-plane anisotropy. At low magnetic fields these trilayers exhibit a pronounced magnetoresistance effect. Its dynamic transport behavior is presented through detailed I-V characteristics. More importantly, the detailed evolution of the longitudinal and transverse magnetic components of the trilayers is presented from close to well below T . These data clearly show that below T and for low magnetic fields the transp…
Remote Moiré Modulation of Decoupled Dirac Subsystems in Twisted Trilayer Graphene
Daegu Gyeongbuk Institute of Science and Technology (DGIST)（大邱庆北科学技术院）；National Institute for Materials Science（国立材料研究所）；Korea Advanced Institute of Science and Technology（韩国科学技术院）；Institute for Basic Science（基础科学研究院）
Electronic structures and their Landau quantizations in twisted graphene bilayer and trilayer are investigated using scanning tunnelling microscopy and spectroscopy. In the twisted trilayer, the top graphene layer and second layer are AB (Bernal) stacking and there is a stacking misorientation between the second layer and third layer. Both the twisted bilayer and trilayer exhibit two pronounced low-energy van Hove singularities (VHSs) in their spectra. Below the VHSs, the observed Landau level quantization in the twisted bilayer is identical to that of massless Dirac fermion in graphene monola…
Spin current generated by spin Hall effect in the heavy metal would diffuse up and down to adjacent ferromagnetic layers and exert torque on their magnetization, called spin-orbit torque. Antiferromagnetically coupled trilayers, namely the so-called synthetic antiferromagnets (SAF), are usually employed to serve as the pinned layer of spintronic devices based on spin valves and magnetic tunnel junctions to reduce the stray field and/or increase the pinning field. Here we investigate the spin-orbit torque in MgO/CoFeB/Ta/CoFeB/MgO perpendicularly magnetized multilayer with interlayer antiferrom…
The ABC-stacked N-layer-graphene family of two-dimensional electron systems is described at low energies by two remarkably flat bands with Bloch states that have strongly momentum-dependent phase differences between carbon pi-orbital amplitudes on different layers, and large associated momentum space Berry phases. These properties are most easily understood using a simplified model with only nearest-neighbor inter-layer hopping which leads to gapless semiconductor electronic structure, with p^N dispersion in both conduction and valence bands. We report on a study of the electronic band structu…
Due to the absence of interlayer coupling and inversion symmetry, transition metal dichalcogenide (MX$_2$) semiconductor monolayers exhibit novel properties that are distinctly different from their bulk crystals such as direct optical band gaps, large band spin splittings, spin-valley coupling, piezoelectric and nonlinear optical responses, and thus have promising applications in, e.g., opto-electronic and spintronic devices. Here we have performed a systematic first-principles study of the second-order nonlinear optical properties of MX$_2$ (M = Mo, W; X = S, Se) monolayers and trilayers with…
We show that the coupling between two ferromagnetic layers separated by a nonmagnetic spacer can be used to control the depinning of domain walls and induce unidirectional domain wall propagation. We investigated CoFeB/Ti/CoFeB trilayers where the easy axis of the magnetization of the top CoFeB layer is out-of-plane and that of the bottom layer is in-plane. Using Magneto-optic Kerr effect microscopy, we find that the depinning of a domain wall in the perpendicularly magnetized CoFeB layer is influenced by the orientation of the magnetization of the in-plane layer, which gives rise to a field-d…
Recent advances on the stabilization and manipulation of chiral magnetization configurations in systems consisting in alternating atomic layers of ferromagnetic and non-magnetic materials hold promise of innovation in spintronics technology. The low dimensionality of the systems promotes spin orbit driven interfacial effects like antisymmetric Dzyaloshinskii-Moriya interactions (DMI) and surface magnetic anisotropy, whose relative strengths may be tuned to achieve stable nanometer sized magnetic objects with fixed chirality. While in most of the cases this is obtained by engineering complex mu…
The effect of the number of stacking layers and the type of stacking on the electronic and optical properties of bilayer and trilayer black phosphorus are investigated by using first principles calcula- tions within the framework of density functional theory. We find that inclusion of many body effects (i.e., electron-electron and electron-hole interactions) modifies strongly both the electronic and opti- cal properties of black phosphorus. While trilayer black phosphorus with a particular stacking type is found to be a metal by using semilocal functionals, it is predicted to have an electroni…
We report on the transport and magnetic properties of hybrid trilayers and bilayers that consist of low spin-polarized Ni80Fe20 exhibiting in-plane but no uniaxial anisotropy and low-Tc Nb. We reveal a magnetoresistance effect that is pronounced. In our trilayers the magnetoresistance exhibits an increase of two orders of magnitude when the superconducting state is reached: from the conventional normal-state values 0.6 % it goes up to 1000 % for temperatures below Tc. In contrast, in the bilayers the effect is only minor since from 3% in the normal state increases only to 70 % for temperatures…
It is of fundamental importance but challenging to simultaneously identify atomic and magnetic configurations of two-dimensional van der Waals materials. In this work, we show that the nonreciprocal second-harmonic generation (SHG) can be a powerful tool to answer this challenge. Despite the preserved lattice inversion symmetry, the interlayer antiferromagnetic order and spin-orbit coupling generate enhanced SHG in PT-symmetric bilayer chromium triiodide (CrI3). Importantly, the in-plane polarization-resolved SHG is sensitive to subtly different interlayer structures that cannot be told by lin…
The physical properties of two-dimensional van der Waals (2D vdW) crystals depend sensitively on the interlayer coupling, which is intimately connected to the stacking arrangement and the interlayer spacing. For example, simply changing the twist angle between graphene layers can induce a variety of correlated electronic phases, which can be controlled further in a continuous manner by applying hydrostatic pressure to decrease the interlayer spacing. In the recently discovered 2D magnets, theory suggests that the interlayer exchange coupling strongly depends on layer separation, while the stac…
Transition metal dichalcogenides (TMDs) constitute a versatile platform for atomically thin optoelectronics devices and spin-valley memory applications. In monolayers optical absorption is strong, but the transition energy is not tunable as the neutral exciton has essentially no out-of-plane electric dipole. In contrast, interlayer exciton transitions in heterobilayers are widely tunable in applied electric fields, but their coupling to light is considerably reduced. Here, we show tuning over 120 meV of interlayer excitons with high oscillator strength in bilayer MoS2. These shifts are due to …
Chern-Selective multi-valley Flat Bands in Twisted Mono-Bilayer and Mono-Trilayer MoTe$_2$
Beijing National Laboratory for Condensed Matter Physics and Institute of physics, Chinese academy of sciences（中国科学院物理研究所）；University of Chinese academy of sciences（中国科学院大学）；Center for Computational Quantum Physics, Flatiron Institute（平顿研究所计算量子物理中心）；Department of Physics, Princeton University（普林斯顿大学物理系）；Laboratoire de Physique de l’Ecole normale supérieure, ENS, Université PSL, CNRS, Sorbonne Université, Université Paris-Diderot, Sorbonne Paris Cité（巴黎高等师范学院物理实验室）
We clarify the role of quantum-well states in magnetic trilayer systems from majority carrier in the ferromagnetic and all carriers in the antiferromagnetic configurations. In addition to numerical and analytic calculations, heuristic pictures are provided to explain effects of a capping layer and side-layer modulation in recent experiments. This immediately offers answers to two unexplained subtle findings in experiments and band-structure calculations, individually. Furthermore, it allows a more flexible tuning of or even turning off the interlayer exchange coupling.
The intertwined ferroelectricity and band topology will enable the non-volatile control of the topological states, which is of importance for nanoelectrics with low energy costing and high response speed. Nonetheless, the principle to design the novel system is unclear and the feasible approach to achieve the coexistence of two parameter orders is absent. Here, we propose a general paradigm to design 2D ferroelectric topological insulators by sliding topological multilayers on the basis of first-principles calculations. Taking trilayer Bi2Te3 as a model system, we show that in the van der Waal…
Sliding of two-dimensional materials is critical for their application as solid lubricants for space, and also relevant for strain engineering and device fabrication. Dopants such as Ni surprisingly improve lubrication in MoS$_2$, despite formation of interlayer bonds by intercalated Ni, and the mechanism has remained unclear. While sliding on the atomistic level has been theoretically investigated in pristine 2D materials, there has been little work on doped forms, especially for the complicated case of intercalation. We use density functional theory to study sliding of Ni-doped MoS$_2$, cons…
