Chromium triiodide, CrI$_3$, is emerging as a promising magnetic two-dimensional semiconductor where spins are ferromagnetically aligned within a single layer. Potential applications in spintronics arise from an antiferromagnetic ordering between adjacent layers that gives rise to spin filtering and a large magnetoresistance in tunnelling devices. This key feature appears only in thin multilayers and it is not inherited from bulk crystals, where instead neighbouring layers share the same ferromagnetic spin orientation. This discrepancy between bulk and thin samples is unexpected, as magnetic ordering between layers arises from exchange interactions that are local in nature and should not depend strongly on thickness. Here we solve this controversy and show through polarization resolved Raman spectroscopy that thin multilayers do not undergo a structural phase transition typical of bulk crystals. As a consequence, a different stacking pattern is present in thin and bulk samples at the temperatures at which magnetism sets in and, according to previous first-principles simulations, this results in a different interlayer magnetic ordering. Our experimental findings provide evidence for the strong interplay between stacking order and magnetism in CrI$_3$, opening interesting perspectives to design the magnetic state of van der Waals multilayers.
Stacking order can significantly influence the physical properties of two-dimensional (2D) van der Waals materials. The recent isolation of atomically thin magnetic materials opens the door for control and design of magnetism via stacking order. Here we apply hydrostatic pressure up to 2 GPa to modify the stacking order in a prototype van der Waals magnetic insulator CrI3. We observe an irreversible interlayer antiferromagnetic (AF) to ferromagnetic (FM) transition in atomically thin CrI3 by magnetic circular dichroism and electron tunneling measurements. The effect is accompanied by a monocli…
Using polarization-resolved Raman spectroscopy, we investigate layer number, temperature, and magnetic field dependence of Raman spectra in one- to four-layer $\mathrm{CrI_{3}}$. Layer-number-dependent Raman spectra show that in the paramagnetic phase a doubly degenerated $E_{g}$ mode of monolayer $\mathrm{CrI_{3}}$ splits into one $A_{g}$ and one $B_{g}$ mode in N-layer (N > 1) $\mathrm{CrI_{3}}$ due to the monoclinic stacking. Their energy separation increases in thicker samples until an eventual saturation. Temperature-dependent measurements further show that the split modes tend to merge u…
Two-dimensional (2D) magnetic materials have attracted much recent interest with unique properties emerging at the few-layer limit. Beyond the reported impacts on the static magnetic properties, the effects of reducing the dimensionality on the magnetization dynamics are also of fundamental interest and importance for 2D device development. In this report, we investigate the spin dynamics in atomically-thin antiferromagnetic FePS3 of varying layer numbers using ultrafast pump-probe spectroscopy. Following the absorption of an optical pump pulse, the time evolution of the antiferromagnetic orde…
As a 2D ferromagnetic semiconductor with magnetic ordering, atomically thin chromium triiodide is the latest addition to the family of two-dimensional (2D) materials. However, realistic exploration of CrI3-based devices and heterostructures is challenging, due to its extreme instability under ambient conditions. Here we present Raman characterization of CrI3, and demonstrate that the main degradation pathway of CrI3 is the photocatalytic substitution of iodine by water. While simple encapsulation by Al2O3, PMMA and hexagonal BN (hBN) only leads to modest reduction in degradation rate, minimizi…
We address the interplay between stacking and interlayer exchange for ferromagnetically ordered CrI$_3$, both for bilayers and bulk. Whereas bulk CrI$_3$ is ferromagnetic, both magneto-optical and transport experiments show that interlayer exchange for CrI$_3$ bilayers is antiferromagnetic. Bulk CrI$_3$ is known to assume two crystal structures, rhombohedral and monoclinic, that differ mostly in the stacking between monolayers. Below 210-220 Kelvin, bulk CrI$_3$ orders in a rhombohedral phase. Our density functional theory calculations show a very strong dependence of interlayer exchange and s…
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…
Exfoliated chromium triiodide (CrI$_3$) is a layered van der Waals (vdW) magnetic insulator that consists of ferromagnetic layers coupled through antiferromagnetic interlayer exchange. The resulting permutations of magnetic configurations combined with the underlying crystal symmetry produces tunable magneto-optical phenomena that is unique to the two-dimensional (2D) limit. Here, we report the direct observation of 2D magnons through magneto-Raman spectroscopy with optical selection rules that are strictly determined by the honeycomb lattice and magnetic states of atomically thin CrI$_3$. In …
The magnetic state of atomically thin semiconducting layered antiferromagnets such as CrI$_3$ and CrCl$_3$ can be probed by forming tunnel barriers and measuring their resistance as a function of magnetic field ($H$) and temperature ($T$). This is possible because the tunneling magnetoresistance originates from a spin-filtering effect sensitive to the relative orientation of the magnetization in different layers, i.e., to the magnetic state of the multilayers. For systems in which antiferromagnetism occurs within an individual layer, however, no spin-filtering occurs: it is unclear whether thi…
Recently, Kayyalha et al. (2019 Phys. Rev. Lett. 122 047003) reported on anomalous enhancement of the self-field critical currents, Ic(sf,T), at low temperatures in Nb/BiSbTeSe2-nanoribbon/Nb Josephson junctions. The enhancement was attributed to the low-energy Andreev bound states arising from winding of the electronic wave function around the circumference of the topological insulator BiSbTeSe2 nanoribbon. In this paper, we show that identical enhancement in Ic(sf,T) and in the upper critical field, Bc2(T), at approximately same reduced temperatures, were reported by several research groups …
Van der Waals (vdW) heterostructures synthesized through the chemical vapor deposition (CVD) method allow creation and tuning of intriguing electronic and optical properties of two- dimensional (2D) materials, the knowledge of which is critical for a wide range of potential applications. Here we report our scanning tunneling microscopy/spectroscopy (STM/STS) study of as-grown MoS2 monolayer and WS2/MoS2 heterobilayer on SiO2. The heterobilayer appears smoother than the MoS2 monolayer, with root mean square (RMS) roughness of 0.230 +- 0.021 nm in the former and 0.329 +- 0.033 nm in the latter. …
The ability of spin-orbit interactions to convert charge current into spin current, most often in the bulk of heavy metal thin films, has been the hallmark of spintronics in the last decade. In this study, we demonstrate how the insertion of light metal element interface profoundly affects both the nature of spin-orbit torque and its efficiency in terms of damping-like ($H_{\text{DL}}$) and field-like ($H_{\text{FL}}$) effective fields in ultrathin Co ferromagnet. Indeed, we measure unexpectedly large $H_{\text{FL}}$/$H_{\text{DL}}$ ratio ($\sim$2.5) upon inserting a 1.4 nm thin Al layer in Pt…
Ionic transport in nano- to sub-nano-scale pores is highly dependent on translocation barriers and potential wells. These features in the free-energy landscape are primarily the result of ion dehydration and electrostatic interactions. For pores in atomically thin membranes, such as graphene, other factors come into play. Ion dynamics both inside and outside the geometric volume of the pore can be critical in determining the transport properties of the channel due to several commensurate length scales, such as the effective membrane thickness, radii of the first and the second hydration layers…
One account of two-dimensional (2D) structural transformations in 2D ferroelectrics predicts an evolution from a structure with Pnm2$_1$ symmetry into a structure with square P4/nmm symmetry and is consistent with experimental evidence, while another argues for a transformation into a structure with rectangular Pnmm symmetry. An analysis of the assumptions made in these models is provided here, and six fundamental results concerning these transformations are contributed as follows: (i) Softened phonon modes produce rotational modes in these materials. (ii) The transformation to a structure wit…
Resolving the momentum degree of freedom of excitons - electron-hole pairs bound by the Coulomb attraction in a photoexcited semiconductor, has remained a largely elusive goal for decades. In atomically thin semiconductors, such a capability could probe the momentum forbidden dark excitons, which critically impact proposed opto-electronic technologies, but are not directly accessible via optical techniques. Here, we probe the momentum-state of excitons in a WSe2 monolayer by photoemitting their constituent electrons, and resolving them in time, momentum and energy. We obtain a direct visual of…
Atomically thin semiconductors have dimensions that are commensurate with critical feature sizes of future optoelectronic devices defined using electron/ion beam lithography. Robustness of their emergent optical and valleytronic properties is essential for typical exposure doses used during fabrication. Here, we explore how focused helium ion bombardment affects the intrinsic vibrational, luminescence and valleytronic properties of atomically thin MoS$_{2}$. By probing the disorder dependent vibrational response we deduce the interdefect distance by applying a phonon confinement model. We show…
Magnetic proximity effects are crucial ingredients for engineering spintronic, superconducting, and topological phenomena in heterostructures. Such effects are highly sensitive to the interfacial electronic properties, such as electron wave function overlap and band alignment. The recent emergence of van der Waals (vdW) magnets enables the possibility of tuning proximity effects via designing heterostructures with atomically clean interfaces. In particular, atomically thin CrI3 exhibits layered antiferromagnetism, where adjacent ferromagnetic monolayers are antiferromagnetically coupled. Explo…
Current-induced domain wall (DW) motion has drawn great attention in the last decades as the key operational principle of emerging magnetic memory devices. As the major driving force of the current-induced DW motion, the spin-orbit torque (SOT) on chiral DWs has been proposed and extensively studied nowadays. However, we demonstrate here that there exists another driving force, which is larger than the SOT in ultra-thin Co films. Moreover, the direction of the present force is found to be opposite to the prediction of the spin-transfer torque (STT), resulting in the DW motion along the current…
In nano-device applications using 2D van der Waals materials, a heat dissipation through nano-scale interfaces can be a critical issue for optimizing device performances. By using a time-domain thermoreflectance measurement technique, we examine a cross-plane thermal transport through mono-layered (n=1) and bi-layered (n=2) WSe2 flakes which are sandwiched by top metal layers of Al, Au, and Ti and the bottom Al2O3 substrate. In these nanoscale structures with hetero- and homo-junctions, we observe that the thermal boundary resistance (TBR) is significantly enhanced as the number of WSe2 layers…
Interlayer coupling between twisted graphenes through atomically-precise barriers
The University of Hong Kong（香港大学）；State Key Laboratory of Optical Quantum Materials, The University of Hong Kong（香港大学光学量子材料国家重点实验室）；National Graphene Institute, University of Manchester（曼彻斯特大学国家石墨烯研究所）；Department of Physics and Astronomy, University of Manchester（曼彻斯特大学物理与天文学系）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（物质材料研究机构电子与光学材料研究中心）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（物质材料研究机构材料纳米结构研究中心）
Recent research in two-dimensional (2D) materials has boosted a renovated interest in the p-n junction, one of the oldest electrical components which can be used in electronics and optoelectronics. 2D materials offer remarkable flexibility to design novel p-n junction device architectures, not possible with conventional bulk semiconductors. In this Review we thoroughly describe the different 2D p-n junction geometries studied so far, focusing on vertical (out-of-plane) and lateral (in-plane) 2D junctions and on mixed-dimensional junctions. We discuss the assembly methods developed to fabricate…
Atomically-thin transition metal dichalcogenide crystals (TMDCs) hold great promise for future semiconductor optoelectronics due to their unique electronic and optical properties. In particular, electron-hole pairs (excitons) in TMDCs are stable at room temperature and interact strongly with light. When TMDCs are embedded in an optical microcavity, the excitons can hybridise with cavity photons to form exciton polaritons (polaritons herein), which display both ultrafast velocities and strong interactions. The ability to manipulate and trap polaritons on a microchip is critical for future appli…
This article provides an overview, primarily from an experimental perspective, of recent progress and future prospects in using helium to realize a range of quantum materials of generic interest, by "top-down" and "bottom-up" nanotechnology. We can grow model systems to realise new quantum states of matter, and explore key issues in condensed matter physics. In the language of cold atomic gases, two dimensional and confined 3He and 4He provide "quantum simulators", with the potential to uncover new emergent quantum states. These include: strictly 2D Fermi system with Mott-Hubbard transition; i…
The morphology and dimension of the conductive filament formed in a memristive device are strongly influenced by the thickness of its switching medium layer. Aggressive scaling of this active layer thickness is critical towards reducing the operating current, voltage and energy consumption in filamentary type memristors. Previously, the thickness of this filament layer has been limited to above a few nanometers due to processing constraints, making it challenging to further suppress the on-state current and the switching voltage. Here, we study the formation of conductive filaments in a materi…
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…
Two-dimensional semiconductors are structurally ideal channel materials for the ultimate atomic electronics after silicon era. A long-standing puzzle is the low carrier mobility (μ) in them as compared with corresponding bulk structures, which constitutes the main hurdle for realizing high-performance devices. To address this issue, we perform combined experimental and theoretical study on atomically thin MoS2 field effect transistors with varying the number of MoS2 layers (NLs). Experimentally, an intimate relation is observed with a 10-fold degradation in μ for extremely thinned monolayer ch…
The ability to exfoliate layered materials down to the single layer limit has opened the opportunity to understand how a gradual reduction in dimensionality affects the properties of bulk materials. Here we use this top-down approach to address the problem of superconductivity in the two-dimensional limit. The transport properties of electronic devices based on 2H tantalum disulfide flakes of different thicknesses are presented. We observe that superconductivity persists down to the thinnest layer investigated (3.5 nm), and interestingly, we find a pronounced enhancement in the critical temper…
Mott transition has been realized in atomically thin monolayer (ML) of two dimensional semiconductors (WS$_2$) via optically excited carriers above a critical carrier density through many body interactions. The above nonlinear optical transition occurs when excited electron hole pairs in ML WS2 continuum heavily interact with each other followed by transformation into a collective electron hole plasma phase (EHP), by losing their identity as individual quasiparticles. This is manifested by the alluring red-shift-blue-shift crossover (RBC) phenomena of the excitonic peaks in the emission spectr…
The recent discovery of ferromagnetic single-layer CrI3 creates ample opportunities for studying fundamental properties of atomically-thin magnets. By using first-principles calculations and model analysis, we show that a lateral strain and/or charge doping can have unexpected effects on the magnetic properties of CrI3. In particular, strain tunes the magnetic order and anisotropy: (1) a compressive strain leads to a phase transition from a ferromagnetic insulator to an antiferromagnetic insulator, while (2) a tensile strain can flip the magnetic orientation from off-plane to in-plane. Interes…
We present a probe-type scanning tunneling microscope (STM) with atomic resolution that is designed to be directly inserted and work in a harsh vibrational cryogen-free superconducting magnet system. When a commercial variable temperature insert (VTI) is installed in the magnet and the STM is in turn housed in the VTI, a lowest temperature of 1.6 K can be achieved, where the STM still operates well. We have tested it in an 8 T superconducting magnet cooled with the pulse-tube cryocooler (PTC) and obtained atomically revolved graphite and NiSe2 images as well as the scanning tunneling spectrum …
When thinned down to the atomic scale, many layered van der Waals materials exhibit an interesting evolution of their electronic properties, whose main aspects can be accounted for by changes in the single-particle band structure. Phenomena driven by interactions are also observed, but identifying experimentally systematic trends in their thickness dependence is challenging. Here, we explore the evolution of gate-induced superconductivity in exfoliated MoS2 multilayers ranging from bulk-like to individual monolayers. We observe a clear transition for all the thicknesses down to the ultimate at…
Ion channels play a key role in regulating cell behavior and in electrical signaling. In these settings, polar and charged functional groups -- as well as protein response -- compensate for dehydration in an ion-dependent way, giving rise to the ion selective transport critical to the operation of cells. Dehydration, though, yields ion-dependent free-energy barriers and thus is predicted to give rise to selectivity by itself. However, these barriers are typically so large that they will suppress the ion currents to undetectable levels. Here, we establish that graphene displays a measurable deh…
Contactless cavity sensing of superfluid stiffness in atomically thin 4Hb-TaS$_2$
University of California, Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；Kavli Energy NanoScience Institute at the University of California, Berkeley and the Lawrence Berkeley National Laboratory（加州大学伯克利分校与劳伦斯伯克利国家实验室卡弗里纳米科学能源研究所）；University of Florida（佛罗里达大学）
The magnetic properties in two-dimensional van der Waals materials depend sensitively on structure. CrI3, as an example, has been recently demonstrated to exhibit distinct magnetic properties depending on the layer thickness and stacking order. Bulk CrI3 is ferromagnetic (FM) with a Curie temperature of 61 K and a rhombohedral layer stacking, while few-layer CrI3 has a layered antiferromagnetic (AFM) phase with a lower ordering temperature of 45 K and a monoclinic stacking. In this work, we use cryogenic magnetic force microscopy to investigate CrI3 flakes in the intermediate thickness range (…
We report ab initio calculations of the spin splitting of the uppermost valence band (UVB) and the lowermost conduction band (LCB) in bulk and atomically thin GaS, GaSe, GaTe, and InSe. These layered monochalcogenides appear in four major polytypes depending on the stacking order, except for the monoclinic GaTe. Bulk and few-layer $ε$- and $γ$-type, and odd-number $β$-type GaS, GaSe, and InSe crystals are noncentrosymmetric. The spin splittings of the UVB and the LCB near the $Γ$-point in the Brillouin zone are finite, but still smaller than those in a zinc-blende semiconductor such as GaAs. O…
MoS2 monolayers exhibit excellent light absorption and large thermoelectric power, which are, however, accompanied with very strong exciton binding energy - resulting in complex photoresponse characteristics. We study the electrical response to scanning photo-excitation on MoS2 monolayer (1L) and bilayer (2L) devices, and also on monolayer/bilayer (1L/2L) planar heterojunction and monolayer/few-layer/multi-layer (1L/FL/ML) planar double heterojunction devices to unveil the intrinsic mechanisms responsible for photocurrent generation in these materials and junctions. Strong photoresponse modula…
Exploring new parameter regimes to realize and control novel phases of matter has been a main theme in modern condensed matter physics research. The recent discovery of 2D magnetism in nearly freestanding monolayer atomic crystals has already led to observations of a number of novel magnetic phenomena absent in bulk counterparts. Such intricate interplays between magnetism and crystalline structures provide ample opportunities for exploring quantum phase transitions in this new 2D parameter regime. Here, using magnetic field and temperature dependent circularly polarized Raman spectroscopy of …
The recent discovery of ferromagnetism in 2D van der Waals (vdw) crystals has generated widespread interest, owing to their potential for fundamental and applied research. Advancing the understanding and applications of vdw magnets requires methods to quantitatively probe their magnetic properties on the nanoscale. Here, we report the study of atomically thin crystals of the vdw magnet CrI$_3$ down to individual monolayers using scanning single-spin magnetometry, and demonstrate quantitative, nanoscale imaging of magnetisation, localised defects and magnetic domains. We determine the magnetisa…
The recent discovery of magnetism in atomically thin layers of van der Waals crystals has created great opportunities for exploring light-matter interactions and magneto-optical phenomena in the two-dimensional limit. Optical and magneto-optical experiments have provided insights into these topics, revealing strong magnetic circular dichroism and giant Kerr signals in atomically thin ferromagnetic insulators. However, the nature of the giant magneto-optical responses and their microscopic mechanism remain unclear. Here, by performing first-principles GW and Bethe-Salpeter equation calculations…
The physical properties of epitaxial films can fundamentally differ from those of bulk single crystals even above the critical thickness. By a combination of non-resonant x-ray magnetic scattering, neutron diffraction and vector-mapped x-ray magnetic linear dichroism photoemission electron microscopy, we show that epitaxial (111)-BiFeO3 films support sub-micron antiferromagnetic domains, which are magneto-elastically coupled to a coherent crystallographic monoclinic twin structure. This unique texture, which is absent in bulk single crystals, should enable control of magnetism in BiFeO3 film d…
