Multiferroic tunnel junctions (MFTJs) have aroused significant interest due to their functional properties useful for non-volatile memory devices. So far, however, all the existing MFTJs have been based on perovskite-oxide heterostructures limited by a relatively high resistance-area (RA) product unfavorable for practical applications. Here, using first-principles calculations, we explore spin-dependent transport properties of van der Waals (vdW) MFTJs which consist of two-dimensional (2D) ferromagnetic FenGeTe2 (n = 3, 4, 5) electrodes and 2D ferroelectric In2Se3 barrier layers. We demonstrate that such FemGeTe2/In2Se3/FenGeTe2 (m, n = 3, 4, 5) MFTJs exhibit multiple non-volatile resistance states associated with different polarization orientation of the ferroelectric In2Se3 layer and magnetization alignment of the two ferromagnetic FenGeTe2 layers. We find a remarkably low RA product which makes the proposed vdW MFTJs superior to the conventional MFTJs in terms of their promise for non-volatile memory applications.
Switchable Magnetoelectric Transport in Graphene via a Van der Waals Multiferroic
Institute for Solid State Physics, The University of Tokyo（东京大学固体物质研究所）；Department of Physics, Institute of Science Tokyo（东京科学大学物理系）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（国家材料研究所电子与光学材料研究中心）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（国家材料研究所材料纳米结构研究中心）；Center for Emergent Matter Science, RIKEN（理化学研究所新兴物质科学中心）；Quantum-Phase Electronics Center and Department of Applied Physics, The University of Tokyo（东京大学量子相电子中心及应用物理系）
In multiferroic oxides with a transverse helical magnetic order, the magnetization exchange coupling is sinusoidally space-dependent. We theoretically investigate the spin-dependent electron grating effect in normal-metal/helical-multiferroic/ferromagnettic heterojunctions. The spin wave vector of the spiral can be added or subtracted from the electron spacial wave vector inducing spin-conserved and spin-flipped diffracted transmission and reflection. The predicted grating effect can be controlled by magnetization exchange coupling strength, the helicity spatial period, and the magnetization o…
Multiferroic materials with coupled ferroelectric and ferromagnetic properties are important for multifunctional devices due to their potential ability of controlling magnetism via electric field, and vice versa. The recent discoveries of two-dimensional ferromagnetic and ferroelectric materials have ignited tremendous research interest and aroused hope to search for two-dimensional multiferroics. However, intrinsic two-dimensional multiferroic materials and, particularly, those with strong magnetoelectric couplings are still rare to date. In this paper, using first-principles simulations, we …
Multiferroic materials have garnered wide interest for their exceptional static and dynamical magnetoelectric properties. In particular, type-II multiferroics exhibit an inversion-symmetry-breaking magnetic order which directly induces a ferroelectric polarization through various mechanisms, such as the spin-current or the inverse Dzyaloshinskii-Moriya effect. This intrinsic coupling between the magnetic and dipolar order parameters results in record-strength magnetoelectric effects. Two dimensional materials possessing such intrinsic multiferroic properties have been long sought for harnessin…
We theoretically investigate the angular and spin dependent transport in normal-metal/helical-multiferroic/ferromagnetic heterojunctions. We find a tunneling anisotropic magnetoresistance (TAMR) effect due to the spiral magnetic order in the tunnel junction and to an effective spin-orbit coupling induced by the topology of the localized magnetic moments in the multiferroic spacer. The predicted TAMR effect is efficiently controllable by an external electric field due to the magnetoelectric coupling.
Multiferroic van der Waals (vdW) heterostrucutres offers an exciting route towards novel nanoelectronics and spintronics device technology. Here we investigate the electronic and transport properties of multiferroic vdW heterostructure composed of ferromagnetic FeCl$_2$ monolayer and ferroelectric Sc$_2$CO$_2$ monolayer using first-principles density functional theory and quantum transport simulations. We show that FeCl$_2$/Sc$_2$CO$_2$ heterostructure can be reversibly switched from semiconducting to half-metallic behavior by electrically modulating the ferroelectric polarization states of Sc…
Thermoelectric transport across normal-metal/helical-multiferroic/ferromagnetic heterojunctions is theoretically investigated. We find a anisotropic charge and spin thermopower with a $C_{2v}$ symmetry. The angular dependence on the magnetization orientation of the ferromagnetic layer is substantiated by a phenomenological theory based on the symmetry of the effective spin-orbit interaction induced by the topology of the spiral magnetic order in the multiferroic barrier.
We develop a theory for interlayer tunneling in van der Waals heterostructures driven under a strong electromagnetic field, using graphene/{\it h}-BN/graphene as a paradigmatic example. Our theory predicts that strong anti-resonances appear at bias voltage values equal to an integer multiple of the light frequency. These features are found to originate from photon-assisted resonant tunneling transitions between Floquet sidebands of different graphene layers, and are unique to two-band systems due to the interplay of both intraband and interband tunneling transitions. Our results point to the p…
We investigate the micromechanical exfoliation and van der Waals (vdW) assembly of ferromagnetic layered dichalcogenide Fe0.25TaS2. The vdW interlayer coupling at the Fe-intercalated plane of Fe0.25TaS2 allows exfoliation of flakes. A vdW junction between the cleaved crystal surfaces is constructed by dry transfer method. We observe tunnel magnetoresistance in the resulting junction under an external magnetic field applied perpendicular to the plane, demonstrating spin-polarized tunneling between the ferromagnetic layered material through the vdW junction.
We report the fabrication of perpendicular ferromagnetic electrodes for tunneling devices consist of van der Waals heterostructure. We found MgO/Co/Pt films on Hexagonal BN shows perpendicular magnetic anisotropy (PMA) with the easy axis perpendicular to the substrate. Vacuum annealing enhances the perpendicular anisotropy. The easy axis along the perpendicular direction persists up to room temperature with the Pt layer thickness ranges from 1.5 to 5 nm. We employed the PMA electrodes to construct tunneling devices on graphene and monolayer WSe2, where spin injection characteristics and field …
We predict a new mechanism of surface plasmon amplification in graphene-insulator-graphene van der Waals heterostructures. The amplification occurs upon the stimulated interlayer electron tunneling accompanied by the emission of a coherent plasmon. The quantum-mechanical calculations of the non-local high-frequency tunnel conductivity show that a relative smallness of the tunneling exponent can be compensated by a strong resonance due to the enhanced tunneling between electron states with collinear momenta in the neighboring graphene layers. With the optimal selection of the barrier layer, the…
The understanding of and control over light emission from quantum tunneling has challenged researchers for more than four decades due to the intricate interplay of electrical and optical properties in atomic scale volumes. Here we introduce a device architecture that allows for the disentanglement of electronic and photonic pathways - van der Waals quantum tunneling devices. The electronic properties are defined by a stack of two-dimensional atomic crystals whereas the optical properties are controlled via an external photonic architecture. In van der Waals heterostructure made of gold, hexago…
The growing family of two-dimensional (2D) materials that are now available can be used to assemble van der Waals heterostructures with a wide range of properties. Of particular interest are tunnelling heterostructures, which have been used to study the electronic states both in the tunnelling barrier and in the emitter and collector contacts. Recently, 2D ferromagnets have been studied theoretically and experimentally. Here we investigate electron tunnelling through a thin (2-6 layers) ferromagnetic CrBr3 barrier. For devices with non-magnetic barriers, conservation of momentum can be relaxed…
Layered van der Waals materials have risen as powerful platforms to artificially engineer correlated states of matter. Here we show the emergence of a multiferroic order in a twisted dichalcogenide bilayer superlattice at quarter-filling. We show that the competition between Coulomb interactions leads to the simultaneous emergence of ferrimagnetic and ferroelectric orders. We derive the magnetoelectric coupling for this system, which leads to a direct strong coupling between the charge and spin orders. We show that, due to intrinsic spin-orbit coupling effects, the electronic structure shows a…
In transition metal dichalcogenides, defects have been found to play an important role, affecting doping, spin-valley relaxation dynamics, and assisting in proximity effects of spin-orbit coupling. Here, we study localized states in $\mathrm{WS}_2$ and how they affect tunneling through van der Waals heterostructures of h-BN/graphene/$\mathrm{WS}_2$/metal. The obtained conductance maps as a function of bias and gate voltage reveal single-electron transistor behavior (Coulomb blockade) with a rich set of transport features including excited states and negative differential resistance regimes. Ap…
Magnetic multilayer devices that exploit magnetoresistance are the backbone of magnetic sensing and data storage technologies. Here we report novel multiple-spin-filter magnetic tunnel junctions (sf-MTJs) based on van der Waals (vdW) heterostructures in which atomically thin chromium triiodide (CrI3) acts as a spin-filter tunnel barrier sandwiched between graphene contacts. We demonstrate tunneling magnetoresistance which is drastically enhanced with increasing CrI3 layer thickness, reaching a record 19,000% for magnetic multilayer structures using four-layer sf-MTJs at low temperatures. These…
Despite a rich choice of two-dimensional materials, which exists these days, heterostructures, both vertical (van der Waals) and in-plane, offer an unprecedented control over the properties and functionalities of the resulted structures. Thus, planar heterostructures allow p-n junctions between different two-dimensional semiconductors and graphene nanoribbons with well-defined edges; and vertical heterostructures resulted in the observation of superconductivity in purely carbon-based systems and realisation of vertical tunnelling transistors. Here we demonstrate simultaneous use of in-plane an…
We study the electron and spin transport in a van der Waals system formed by one layer with strong spin-orbit coupling and a second layer without spin-orbit coupling, in the regime when the interlayer tunneling is random. We find that in the layer without intrinsic spin-orbit coupling spin-charge coupled transport can be induced by two distinct mechanisms. First, the gapless diffusion modes of the two isolated layers hybridize in the presence of tunneling, which constitutes a source of spin-charge coupled transport in the second layer. Second, the random tunneling introduces spin-orbit couplin…
Effect of spin-dependent tunneling and intervalley scattering in magnetic-semiconductor van der Waals heterostructures on exciton and trion polarization
Van der Waal's heterostrucutures allow for novel devices such as two-dimensional-to-two-dimensional tunnel devices, exemplified by interlayer tunnel FETs. These devices employ channel/tunnel-barrier/channel geometries. However, during layer-by-layer exfoliation of these multi-layer materials, rotational misalignment is the norm and may substantially affect device characteristics. In this work, by using density functional theory methods, we consider a reduction in tunneling due to weakened coupling across the rotationally misaligned interface between the channel layers and the tunnel barrier. A…
Strongly bound excitons and many-body interactions between them determine light-matter interactions in van der Waals (vdW) heterostructures of 2D semiconductors. Unlike fundamental particles, quasiparticles in condensed matter, such as excitons, can be tailored to alter their interactions and realize emergent quantum phases. Here, using a WS$_2$/WSe$_2$/WS$_2$ heterotrilayer, we create a quantum superposition of oppositely oriented dipolar excitons - a quadrupolar exciton - wherein an electron is layer-hybridized in WS$_2$ layers while the hole localizes in WSe$_2$. In contrast to dipolar exci…
Formation of moiré superlattices is common in Van der Waals heterostructures as a result of the mismatch between lattice constants and misalignment of crystallographic directions of the constituent two-dimensional crystals. We discuss theoretically electron transport in a Van der Waals tunnelling transistor in which one of the electrodes is made of two crystals forming a moiré superlattice at their interface. By investigating structures containing either the aligned graphene/hexagonal boron nitride heterostructure or twisted bilayer graphene, we show that negative differential resistance is po…
The control of elastic and inelastic electron tunneling relies on materials with well defined interfaces. Van der Waals materials made of two-dimensional constituents form an ideal platform for such studies. Signatures of acoustic phonons and defect states have been observed in current-to-voltage ($I-V$) measurements. These features can be explained by direct electron-phonon or electron-defect interactions. Here, we use a novel tunneling process that involves excitons in transition metal dichalcogenides (TMDs). We study tunnel junctions consisting of graphene and gold electrodes separated by h…
Controlling magnetism by purely electrical means is a key challenge to better information technology1. A variety of material systems, including ferromagnetic (FM) metals2,3,4, FM semiconductors5, multiferroics6,7,8 and magnetoelectric (ME) materials9,10, have been explored for the electric-field control of magnetism. The recent discovery of two-dimensional (2D) van der Waals magnets11,12 has opened a new door for the electrical control of magnetism at the nanometre scale through a van der Waals heterostructure device platform13. Here we demonstrate the control of magnetism in bilayer CrI3, an …
In a recent article, A. Chen et al. claimed that they have switched (rotated by ~90 degrees) the magnetization of the soft layer of a magnetic tunnel junction (MTJ) in a non-volatile way with volatile strain by exploiting dipole interaction with the hard layer. I show that dipole interaction cannot cause this effect and the authors' explanation cannot be correct. An alternate explanation is offered.
Ferromagnetic van der Waals (vdW) materials are in demand for spintronic devices with all-two-dimensional-materials heterostructures. Here, we demonstrate mechanical exfoliation of magnetic-atom-intercalated transition metal dichalcogenide Cr1/3TaS2 from its bulk crystal; previously such intercalated materials were thought difficult to exfoliate. Magnetotransport in exfoliated tens-of-nanometres-thick flakes revealed ferromagnetic ordering below its Curie temperature TC ~ 110 K as well as strong in-plane magnetic anisotropy; these are identical to its bulk properties. Further, van der Waals he…
We have investigated the tunneling transport of mono- and few-layers of MnPS3 by using conductive atomic force microscopy. Due to the band alignment of indium tin oxide/MnPS3/Pt-Ir tip junction, the key features of both Schottky junction and Fowler-Nordheim tunneling (FNT) were observed for all the samples with varying thickness. Using the FNT model and assuming the effective electron mass (0.5 me) of MnPS3, we estimate the tunneling barrier height to be 1.31 eV and the dielectric breakdown strength as 5.41 MV/cm.
Atomically thin chromium triiodide (CrI3) has recently been identified as a layered antiferromagnetic insulator, in which adjacent ferromagnetic monolayers are antiferromagnetically coupled. This unusual magnetic structure naturally comprises a series of anti-aligned spin filters which can be utilized to make spin-filter magnetic tunnel junctions with very large tunneling magnetoresistance (TMR). Here we report voltage control of TMR formed by four-layer CrI3 sandwiched by monolayer graphene contacts in a dual-gated structure. By varying the gate voltages at fixed magnetic field, the device ca…
A heat-assisted multiferroic solid-state memory design is proposed and analysed, based on a PbNbZrSnTiO3 antiferroelectric substrate and Ni81Fe19 magnetic free layer. Information is stored as magnetisation direction in the free layer of a magnetic tunnel junction element. The bit writing process is contactless and relies on triggering thermally activated magnetisation switching of the free layer towards a strain-induced anisotropy easy axis. A stress is generated using the antiferroelectric substrate by voltage-induced antiferroelectric to ferroelectric phase change, and this is transmitted to…
As a result of sinusoidal spatial modulation, helimagnet induces spin-dependent diffracted transmission. In this work, we propose a general scattering matrix treatment to the transport properties in helimagnets with arbitrary helical structures. Multiferroic properties can be considered by taking electric polarization and magnetic helix together into account. A monolayer magnetic helix can be treated as a $δ$-barrier by diffraction theory. The conductance and shot noise properties of the normal metal/helimagnet/normal metal toy model are investigated. It is found that the shot noise is suppres…
We report on experimental investigations of an electrically driven WSe2 based light-emitting van der Waals heterostructure. We observe a threshold voltage for electroluminescence significantly lower than the corresponding single particle band gap of monolayer WSe2. This observation can be interpreted by considering the Coulomb interaction and a tunneling process involving excitons, well beyond the picture of independent charge carriers. An applied magnetic field reveals pronounced magneto-oscillations in the electroluminescence of the free exciton emission intensity with a 1/B-periodicity. Thi…
The magnetic tunnel junction (MTJ) is a backbone device for spintronics. Realizing next generation energy efficient MTJs will require operating mechanisms beyond the standard means of applying magnetic fields or large electrical currents. Here, we demonstrate a new concept for programmable MTJ operation via strain control of the magnetic states of CrSBr, a layered antiferromagnetic semiconductor used as the tunnel barrier. Switching the CrSBr from antiferromagnetic to ferromagnetic order generates a giant tunneling magnetoresistance ratio without external magnetic field at temperatures up to ~…
Interest in van der Waals materials often stems from a desire to miniaturise existing technologies by exploiting their intrinsic layered structure to create near atomically-thin components that do not suffer from surface defects. One appealing property is easily-switchable yet robust magnetic order, a quality only sparsely demonstrated in the case of in-plane anisotropy. In this work, we use widefield nitrogen-vacancy (NV) center magnetic imaging to measure the properties of individual flakes of CuCrP$_2$S$_6$, a multiferroic van der Waals magnet known to exhibit weak easy-plane anisotropy in …
We have performed device-based tunnelling spectroscopy of NbSe$_2$ in the vortex state with a magnetic field applied both parallel and perpendicular to the $a-b$ plane. Our devices consist of layered semiconductors placed on top of exfoliated NbSe$_2$ using the van der Waals transfer technique. At zero field, the spectrum exhibits a hard gap, and the quasiparticle peak is split into low and high energy features. The two features, associated with the effective two-band nature of superconductivity in NbSe$_2$, exhibit markedly distinct responses to the application of magnetic field, suggesting a…
Control over the electronic spectrum at low energy is at the heart of the functioning of modern advanced electronics: high electron mobility transistors, semiconductor and Capasso terahertz lasers, and many others. Most of those devices rely on the meticulous engineering of the size quantization of electrons in quantum wells. This avenue, however, hasn't been explored in the case of 2D materials. Here we transfer this concept onto the van der Waals heterostructures which utilize few-layers films of InSe as quantum wells. The precise control over the energy of the subbands and their uniformity …
Thin van der Waals (vdW) layered magnetic materials disclose the possibility to realize vdW heterostructures with new functionalities. Here we report on the realization and investigation of tunneling spin valves based on van der Waals heterostructures consisting of an atomically thin hBN layer acting as tunnel barrier and two exfoliated Fe3GeTe2 crystals acting as ferromagnetic electrodes. Low-temperature anomalous Hall effect measurements show that thin Fe3GeTe2 crystals are metallic ferromagnets with an easy axis perpendicular to the layers, and a very sharp magnetization switching at magnet…
Magnetic insulators are a key resource for next-generation spintronic and topological devices. The family of layered metal halides promises ultrathin insulating multiferroics, spin liquids, and ferromagnets, but new characterization methods are required to unlock their potential. Here, we report tunneling through the layered magnetic insulator CrI3 as a function of temperature and applied magnetic field. We electrically detect the magnetic ground state and inter-layer coupling and observe a field-induced metamagnetic transition. The metamagnetic transition results in magnetoresistances of 95%,…
Van der Waals (vdW) tunnel junctions are attractive due to their atomically sharp interface, gate tunablity, and robustness against lattice mismatch between the successive layers. However, the negative differential resistance (NDR) demonstrated in this class of tunnel diodes often exhibits noisy behaviour with low peak current density, and lacks robustness and repeatability, limiting their practical circuit applications. Here we propose a strategy of using a 1L-WS$_2$ as an optimum tunnel barrier sandwiched in a broken gap tunnel junction of highly doped black phosphorus (BP) and SnSe$_2$. We …
