Imaging domain reversal in an ultrathin van der Waals ferromagnet
David A. Broadway, Sam C. Scholten, Cheng Tan, Nikolai Dontschuk, Scott E. Lillie, Brett C. Johnson, Guolin Zheng, Zhenhai Wang, Artem R. Oganov, Shangjie Tian,… 展开作者
David A. Broadway, Sam C. Scholten, Cheng Tan, Nikolai Dontschuk, Scott E. Lillie, Brett C. Johnson, Guolin Zheng, Zhenhai Wang, Artem R. Oganov, Shangjie Tian, Chenghe Li, Hechang Lei, Lan Wang, Lloyd C. L. Hollenberg, Jean-Philippe Tetienne
The recent isolation of two-dimensional van der Waals magnetic materials has uncovered rich physics that often differs from the magnetic behaviour of their bulk counterparts. However, the microscopic details of fundamental processes such as the initial magnetization or domain reversal, which govern the magnetic hysteresis, remain largely unknown in the ultrathin limit. Here we employ a widefield nitrogen-vacancy (NV) microscope to directly image these processes in few-layer flakes of magnetic semiconductor vanadium triiodide (VI$_3$). We observe complete and abrupt switching of most flakes at fields $H_c\approx0.5-1$ T (at 5 K) independent of thickness down to two atomic layers, with no intermediate partially-reversed state. The coercive field decreases as the temperature approaches the Curie temperature ($T_c\approx50$ K), however, the switching remains abrupt. We then image the initial magnetization process, which reveals thickness-dependent domain wall depinning fields well below $H_c$. These results point to ultrathin VI$_3$ being a nucleation-type hard ferromagnet, where the coercive field is set by the anisotropy-limited domain wall nucleation field. This work illustrates the power of widefield NV microscopy to investigate magnetization processes in van der Waals ferromagnets, which could be used to elucidate the origin of the hard ferromagnetic properties of other materials and explore field- and current-driven domain wall dynamics.
We demonstrate near unity, broadband absorbing optoelectronic devices using sub-15 nm thick transition metal dichalcogenides (TMDCs) of molybdenum and tungsten as van der Waals semiconductor active layers. Specifically, we report that near-unity light absorption is possible in extremely thin (< 15 nm) Van der Waals semiconductor structures by coupling to strongly damped optical modes of semiconductor/metal heterostructures. We further fabricate Schottky junction devices using these highly absorbing heterostructures and characterize their optoelectronic performance. Our work addresses one of th…
We report experimental measurements for ultrathin (< 15 nm) van der Waals heterostructures exhibiting external quantum efficiencies exceeding 50%, and show that these structures can achieve experimental absorbance > 90%. By coupling electromagnetic simulations and experimental measurements, we show that pn WSe2/MoS2 heterojunctions with vertical carrier collection can have internal photocarrier collection efficiencies exceeding 70%.
We report broadband ferromagnetic resonance (FMR) measurements based on a coplanar waveguide (CPW) of ultrathin magnetic film structures that comprise in-plane/out-of-plane decoupled layers deposited on nonmagnetic buffer layers of various thickness or other buffer structures with a diverse sheet resistance. We show that the excitation of the fundamental mode can be substantially (up to 10 times) enhanced in the structures deposited on buffer layers with a low sheet resistance in comparison to the structures deposited on thin or weakly conducting buffer layers. The results are analyzed in term…
Two-dimensional (2D) magnetic van der Waals materials provide a powerful platform for studying fundamental physics of low-dimensional magnetism, engineering novel magnetic phases, and enabling ultrathin and highly tunable spintronic devices. To realize high quality and practical devices for such applications, there is a critical need for robust 2D magnets with ordering temperatures above room temperature that can be created via exfoliation. Here the study of exfoliated flakes of cobalt substituted Fe5GeTe2 (CFGT) exhibiting magnetism above room temperature is reported. Via quantum magnetic ima…
We report on the large-scale synthesis of highly oriented ultrathin MoO3 layers using a simple and low-cost atmospheric pressure by van der Waals epitaxy growth on muscovite mica substrates. By this method we are able to synthetize high quality centimeter-scale MoO3 crystals with thicknesses ranging from 1.4 nm (two layers) up to a few nanometers. The crystals can be easily transferred to an arbitrary substrate (such as SiO2) by a deterministic transfer method and extensively characterized to demonstrate the high quality of the resulting crystal. We also study the electronic band structure of …
Ferromagnetic behaviour has been observed experimentally for the first time in nanostructured Manganese. Ultrathin ($\sim$ 0.6 nm) Manganese nanosheets have been synthesized inside the two dimensional channels of sol-gel derived Na-4 mica. The magnetic properties of the confined system are measured within 2K-300K temperature range. The confined structure is found to show a ferromagnetic behaviour with a nonzero coercivity value. The coercivity value remains positive throughout the entire temperature range of measurement. The experimental variation of susceptibility as a function of temperature…
We present a new approach to infer the surface density of magnetic moments $I_s$ in ultrathin ferromagnetic films with perpendicular anisotropy. It relies on quantitative stray field measurements with an atomic-size magnetometer based on the nitrogen-vacancy center in diamond. The method is applied to microstructures patterned in a 1-nm-thick film of CoFeB. We report measurements of $I_s$ with a few percent uncertainty and a spatial resolution in the range of $(100$ nm)$^2$, an improvement by several orders of magnitude over existing methods. As an example of application, we measure the modifi…
We analyze the electric current and magnetic field driven domain wall motion in perpendicularly magnetized ultrathin ferromagnetic films in the presence of interfacial Dzyaloshinskii-Moriya interaction and both out-of-plane and in-plane uniaxial anisotropies. We obtain exact analytical Walker-type solutions in the form of one-dimensional domain walls moving with constant velocity due to both spin-transfer torques and out-of-plane magnetic field. These solutions are embedded into a larger family of propagating solutions found numerically. Within the considered model, we find the dependencies of…
Ultrathin ferromagnets with frustrated exchange and the Dzyaloshinskii-Moriya interaction can support topological solitons such as skyrmions and antiskyrmions, which are metastable and can be considered particle-antiparticle counterparts. When spin-orbit torques are applied, the motion of an isolated antiskyrmion driven beyond its Walker limit can generate skyrmion-antiskyrmion pairs. Here, we use atomistic spin dynamics simulations to shed light on the scattering processes involved in this pair generation. Under certain conditions a proliferation of these particles and antiparticles can appea…
We report the growth of high quality Bi$_{2-x}$Sb$_x$Te$_{3-y}$Se$_y$ ultrathin nanoplates (BSTS-NPs) on an electrically insulating fluorophlogopite mica substrate using a catalyst-free vapor solid method. Under an optimized pressure and suitable Ar gas flow rate, we control the thickness, the size and the composition of BSTS-NPs. Raman spectra showing systematic change indicate that the thicknesses and compositions of BSTS-NPs are indeed accurately controlled. Electrical transport demonstrates that a robust Dirac cone carrier transport in BSTS-NPs. Since BSTS-NPs provide superior dominant sur…
Metamaterials and metasurfaces operating in the visible and near-infrared (NIR) offer a promising route towards next-generation photodetectors and devices for solar energy harvesting. While numerous metamaterials and metasurfaces using metals and semiconductors have been demonstrated, semimetals-based metasurfaces in the vis-NIR range are notably missing. Here, we experimentally demonstrate a broadband metasurface superabsorber based on large area, semimetallic, van der Waals PtSe2 thin films in agreement with electromagnetic simulations. Our results show that PtSe2 is an ultrathin and scalabl…
Ultrathin and flat optical lenses are essential for modern optical imaging, spectroscopy, and energy harvesting. Dielectric metasurfaces comprising nanoscale quasi-periodic resonator arrays are promising for such applications, as they can tailor the phase, amplitude, and polarization of light at subwavelength resolution, enabling multi-functional optical elements. To achieve 2πphase coverage, however, most dielectric metalenses need a thickness comparable to the wavelength, requiring fabrication of high-aspect-ratio scattering elements. Here, we report ultrathin dielectric metalenses made of v…
We present a detailed study of the ground-state magnetic structure of ultrathin Fe films on the surface of fcc Ir(001). We use the spin-cluster expansion technique in combination with the relativistic disordered local moment scheme to obtain parameters of spin models and then determine the favored magnetic structure of the system by means of a mean field approach and atomistic spin dynamics simulations. For the case of a single monolayer of Fe we find that layer relaxations very strongly influence the ground-state spin configurations, whereas Dzyaloshinskii-Moriya (DM) interactions and biquadr…
Transition metal ferromagnetic films with perpendicular magnetic anisotropy (PMA) have ferromagnetic resonance (FMR) linewidths that are one order of magnitude larger than soft magnetic materials, such as pure iron (Fe) and permalloy (NiFe) thin films. A broadband FMR setup has been used to investigate the origin of the enhanced linewidth in Ni$|$Co multilayer films with PMA. The FMR linewidth depends linearly on frequency for perpendicular applied fields and increases significantly when the magnetization is rotated into the film plane. Irradiation of the film with Helium ions decreases the PM…
Charge transfer plays a key role at the interfaces of heterostructures, which can affect electronic structures and ultimately the physical properties of the materials. However, charge transfer is difficult to manipulate externally once the interface formed. Here, we report electrically tunable charge transfer in Fe3GeTe2/Cr2Ge2Te6/Fe3GeTe2 all-magnetic van der Waals heterostructures, which can be exploited to selectively modify the magnetic properties of the top or bottom Fe3GeTe2 electrodes. The directional charge transfer from metallic Fe3GeTe2 to semiconducting Cr2Ge2Te6 remarkably modifies…
The dynamics of domain walls in ultrathin ferromagnetic strips with perpendicular magnetic anisotropy is studied from both numerical and analytical micromagnetics. The influence of the interfacial Dzyaloshinskii-Moriya interaction associated to a bi-layer strip arrangement has been considered, giving rise to the formation of Dzyaloshinskii domain walls. Such walls possess under equilibrium conditions an inner magnetization structure defined by a certain orientation angle that make them to be considered as intermediate configurations between Bloch and Néel walls. Two different dynamics are cons…
We have synthesized unique colloidal nanoplatelets of the ferromagnetic two-dimensional (2D) van der Waals material CrI3 and have characterized these nanoplatelets structurally, magnetically, and by magnetic circular dichroism spectroscopy. The isolated CrI3 nanoplatelets have lateral dimensions of ~25 nm and ensemble thicknesses of only ~4 nm, corresponding to just a few CrI3 monolayers. Magnetic and magneto-optical measurements demonstrate robust 2D ferromagnetic ordering in these nanoplatelets with Curie temperatures similar to those observed in bulk CrI3, despite the strong spatial confine…
Following the recent isolation of monolayer CrI3, there has been a surge of new two-dimensional van der Waals magnetic materials, whose incorporation in van der Waals heterostructures offers a new platform for spintronics, proximity magnetism, and quantum spin liquids. A primary question in this burgeoning field is how exfoliating crystals to the few-layer limit influences their magnetism. Studies on CrI3 have shown a different magnetic ground state for ultrathin exfoliated films but the origin is not yet understood. Here, we use electron tunneling through few-layer crystals of the layered ant…
Due to the chemical inertness of 2D hexagonal-Boron Nitride (h-BN), few atomic-layer h-BN is often used to encapsulate air-sensitive 2D crystals such as Black Phosphorus (BP). However, the effects of h-BN on Schottky barrier height, doping and contact resistance are not well known. Here, we investigate these effects by fabricating h-BN encapsulated BP transistors with cobalt (Co) contacts. In sharp contrast to directly Co contacted p-type BP devices, we observe strong n-type conduction upon insertion of the h-BN at the Co/BP interface. First principles calculations show that this difference ar…
Ferromagnetism in two-dimensional materials presents a promising platform for the development of ultrathin spintronic devices with advanced functionalities. Recently discovered ferromagnetic van der Waals crystals such as CrI$_{3}$, readily isolated two-dimensional crystals, are highly tunable through external fields or structural modifications. However, there remains a challenge because of material instability under air exposure. Here, we report the observation of an air stable and layer dependent ferromagnetic (FM) van der Waals crystal, CrPS$_{4}$, using magneto-optic Kerr effect microscopy…
The integration of magnetic material with semiconductors has been fertile ground for fundamental science as well as of great practical interest toward the seamless integration of information processing and storage. Here we create van der Waals heterostructures formed by an ultrathin ferromagnetic semiconductor CrI3 and a monolayer of WSe2. We observe unprecedented control of the spin and valley pseudospin in WSe2, where we detect a large magnetic exchange field of nearly 13 T and rapid switching of the WSe2 valley splitting and polarization via flipping of the CrI3 magnetization. The WSe2 phot…
The discovery of ferromagnetism in two-dimensional (2D) monolayers has stimulated growing research interest in both spintronics and material science. However, these 2D ferromagnetic layers are mainly prepared through an incompatible approach for large-scale fabrication and integration, and moreover, a fundamental question whether the observed ferromagnetism actually correlates with the 2D crystalline order has not been explored. Here, we choose a typical 2D ferromagnetic material, Fe3GeTe2, to address these two issues by investigating its ferromagnetism in an amorphous state. We have fabricate…
Magnomechanical Coupling in Suspended 2D van der Waals Ferromagnets
Kavli Institute of Nanoscience, Delft University of Technology（代尔夫特理工大学卡弗里纳米科学研究所）；Department of Precision and Microsystems Engineering, Delft University of Technology（代尔夫特理工大学精密与微系统工程系）
Ultrathin black phosphorus, or phosphorene, is the second known elementary two-dimensional material that can be exfoliated from a bulk van der Waals crystal. Unlike graphene it is a semiconductor with a sizeable band gap and its excellent electronic properties make it attractive for applications in transistor, logic, and optoelectronic devices. However, it is also the first widely investigated two dimensional electronic material to undergo degradation upon exposure to ambient air. Therefore a passivation method is required to study the intrinsic material properties, understand how oxidation af…
We demonstrate that kinetics play an important role in the epitaxial growth of Fe$_3$GeTe$_2$ (FGT) van der Waals (vdW) ferromagnetic films by molecular beam epitaxy. By varying the deposition rate, we control the formation or suppression of an initial tellurium-deficient non-van der Waals phase (Fe$_3$Ge$_2$) prior to realizing epitaxial growth of the vdW FGT phase. Using cross-sectional scanning transmission electron microscopy and scanning tunneling microscopy, we optimize the FGT films to have atomically smooth surfaces and abrupt interfaces with the Ge(111) substrate. The magnetic propert…
Emergent color centers with accessible spins hosted by van der Waals materials have attracted substantial interest in recent years due to their significant potential for implementing transformative quantum sensing technologies. Hexagonal boron nitride (hBN) is naturally relevant in this context due to its remarkable ease of integration into devices consisting of low-dimensional materials. Taking advantage of boron vacancy spin defects in hBN, we report nanoscale quantum imaging of low-dimensional ferromagnetism sustained in Fe3GeTe2/hBN van der Waals heterostructures. Exploiting spin relaxomet…
The intersection of topology and magnetism represents a new playground to discover novel quantum phenomena and device concepts. In this work, we show that a van der Waals compound MnSb$_{1.8}$Bi$_{0.2}$Te$_4$ exhibits a ferromagnetic ground state with a Curie temperature of 26 K, in contrast to the antiferromagnetic order previously found for other members of the Mn(Sb, Bi)$_2$Te$_4$ family. We employ magneto-transport, bulk magnetization and neutron scattering studies to illustrate the magnetic and electrical properties of MnSb$_{1.8}$Bi$_{0.2}$Te$_4$ and report on the observation of an unusu…
The renormalization group equations describing a finite 2DXY system with fourfold anisotropy are solved in two steps, in order to study the magnetic transition to paramagnetism in an ultrathin film. First, the equations are linearized near the critical coupling $K=J/k_BT=2/π$. An exact solution of the linearized equations confirms that a finite-size Kosterlitz-Thouless (KT) transition occurs in the presence of weak fourfold anisotropy, and that an Ising transition occurs for strong anisotropy. The behaviour of a given system is determined by the product of an anisotropy parameter and the logar…
We perform ultrafast pump-probe measurements on a nanometer-thick crystalline Bi-doped yttrium iron garnet film with perpendicular magnetic anisotropy. Tuning the photon energy of the pump laser pulses above and below the material's bandgap, we trigger ultrafast optical and spin dynamics via both one- and two-photon absorption. Contrary to the common scenario, the optically-induced heating of the system induces an increase up to 20% of the ferromagnetic resonance frequency. We explain this unexpected result in terms of a photo-induced modification of the magnetic anisotropy, i.e. of the effect…
Topologically protected magnetic structures provide a robust platform for low power consumption devices for computation and data storage. Examples of these structures are skyrmions, chiral domain walls, and spin spirals. Here we use scanning electron microscopy with polarization analysis to unveil the presence of chiral counterclockwise Néel spin spirals at the surface of a bulk van der Waals ferromagnet Fe$_3$GeTe$_2$ (FGT), at zero magnetic field. These Néel spin spirals survive up to FGT's Curie temperature $T_\mathrm{C}= 220 \mathrm{~K}$, with little change in the periodicity $p=300 \mathr…
Anomalous Nernst effect, a result of charge current driven by temperature gradient, provides a probe of the topological nature of materials due to its sensitivity to the Berry curvature near the Fermi level. Fe3GeTe2, one important member of the recently discovered two-dimensional van der Waals magnetic materials, offers a unique platform for anomalous Nernst effect because of its metallic and topological nature. Here, we report the observation of large anomalous Nernst effect in Fe3GeTe2. The anomalous Hall angle and anomalous Nernst angle are about 0.07 and 0.09 respectively, far larger than…
The recent observation of current-induced domain wall (DW) motion with large velocity in ultrathin magnetic wires has opened new opportunities for spintronic devices. However, there is still no consensus on the underlying mechanisms of DW motion. Key to this debate is the DW structure, which can be of Bloch or Néel type, and dramatically affects the efficiency of the different proposed mechanisms. To date, most experiments aiming to address this question have relied on deducing the DW structure and chirality from its motion under additional in-plane applied fields, which is indirect and involv…
We present the complete zero temperature phase diagram of a model for ultrathin films with perpendicular anisotropy. The whole parameter space of relevant coupling constants is studied in first order anisotropy approximation. Because the ground state is known to be formed by perpendicular stripes separated by Bloch walls, a standard variational approach is used, complemented with specially designed Monte Carlo simulations. We can distinguish four regimes according to the different nature of striped domains: a high anisotropy Ising regime with sharp domain walls, a saturated stripe regime with …
We theoretically investigate the exchange interaction between magnetic impurities in ultrathin Bi$_2$Se$_3$ topological insulator films by taking into account the low-energy states produced by the impurities. We find that the locally induced impurity resonances strongly influence the exchange interaction between magnetic moments. In particular, we find a non-collinear alignment being more favorable than the collinear ferromagnetic alignment preferred when impurity states are ignored and only the pristine topological insulator band structure is considered. Moreover, we show that by applying of …
The valley-polarized quantum anomalous Hall effect (VQAHE) attracts intensive interest since it uniquely combines valleytronics and spintronics with nontrivial band topology. Here, based on first-principles calculations and Wannier-function-based tight-binding (WFTB) model, we reveal that valley-based Hall effects and especially the VQAHE induced by external magnetic fields can occur in two-dimensional (2D) ferromagnetic van der Waals heterostructures (vdWHs). The results show that considerable valley-splitting derived from the Zeeman exchange energy drives these vdWHs generating the valley an…
Layered ferromagnets with high coercivity have special applications in nanoscale memory elements in electronic circuits, such as data storage. Therefore, searching for new hard ferromagnets and effectively tuning or enhancing the coercivity are the hottest topics in layered magnets today. Here, we report a strain tunability of perpendicular magnetic anisotropy in van der Waals (vdW) ferromagnets VI3 using magnetic circular dichroism measurements. For an unstrained flake, the M-H curve shows a rectangular-shaped hysteresis loop with perpendicular magnetic anisotropy and a large coercivity (up t…
We present theoretical studies of the influence of spin orbit coupling on the spin wave excitations of the Fe monolayer and bilayer on the W(110) surface. The Dzyaloshinskii-Moriya interaction is active in such films, by virtue of the absence of reflection symmetry in the plane of the film. When the magnetization is in plane, this leads to a linear term in the spin wave dispersion relation for propagation across the magnetization. The dispersion relation thus assumes a form similar to that of an energy band of an electron trapped on a semiconductor surfaces with Rashba coupling active. We also…
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.
Planar spin transport in disordered ultrathin magnetic bilayers comprising a ferromagnet and a normal metal (typically used for spin pumping, spin Seebeck and spin-orbit torque experiments) is investigated theoretically. Using a tight-binding model that treats extrinsic spin Hall effect, spin swapping and spin relaxation on equal footing, we show that the nature of spin-orbit coupled transport dramatically depends on ratio between the layers thickness $d$ and the mean free path $λ$. While spin Hall effect dominates in the diffusive limit ($d\ggλ$), spin swapping dominates in Knudsen regime ($d…
We study existence and properties of one-dimensional edge domain walls in ultrathin ferromagnetic films with uniaxial in-plane magnetic anisotropy. In these materials, the magnetization vector is constrained to lie entirely in the film plane, with the preferred directions dictated by the magnetocrystalline easy axis. We consider magnetization profiles in the vicinity of a straight film edge oriented at an arbitrary angle with respect to the easy axis. To minimize the micromagnetic energy, these profiles form transition layers in which the magnetization vector rotates away from the direction of…
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…
The emergence of a topological superconducting state in van der Waals heterostructures provides a new platform for exploring novel strategies to control topological superconductors. In particular, impurities in van der Waals heterostructures, generically featuring a moire pattern, can potentially lead to the unique interplay between atomic and moire length scales, a feature absent in generic topological superconductors. Here we address the impact of non-magnetic impurities on a topological moire superconductor, both in the weak and strong regime, considering both periodic arrays and single imp…
Recent advances in nanofabrication make it possible to produce multilayer nanostructures composed of ultrathin film materials with thickness down to a few monolayers of atoms and lateral extent of several tens of nanometers. At these scales, ferromagnetic materials begin to exhibit unusual properties, such as perpendicular magnetocrystalline anisotropy and antisymmetric exchange, also referred to as Dzyaloshinskii-Moriya interaction (DMI), because of the increased importance of interfacial effects. The presence of surface DMI has been demonstrated to fundamentally alter the structure of domain…
Optimal skyrmion stability in antisymmetric ultrathin ferromagnetic bilayers
Université de Toulouse, CNRS, CEMES（图卢兹大学，法国国家科学研究中心，电子与分子材料中心）；School of Mathematics, University of Bristol（布里斯托尔大学数学学院）；Dipartimento di Matematica, Università di Pisa（比萨大学数学系）
We characterize skyrmions in ultrathin ferromagnetic films as local minimizers of a reduced micromagnetic energy appropriate for quasi two-dimensional materials with perpendicular magnetic anisotropy and interfacial Dzyaloshinskii-Moriya interaction. The minimization is carried out in a suitable class of two-dimensional magnetization configurations that prevents the energy from going to negative infinity, while not imposing any restrictions on the spatial scale of the configuration. We first demonstrate existence of minimizers for an explicit range of the model parameters when the energy is do…
