The electronic properties of van der Waals (vdW) structures can be substantially modified by the moire superlattice potential, which strongly depends on the twist angle among the compounds. In twisted bilayer graphene (TBG), two low-energy Van Hove singularities (VHSs) move closer with decreasing twist angles and finally become highly non-dispersive flat bands at the magic angle (~ 1.1 degree). When the Fermi level lies within the flat bands of the TBG near the magic angle, Coulomb interaction is supposed to exceed the kinetic energy of the electrons, which can drive the system into various strongly correlated phases. Moreover, the strongly correlated states of flat bands are also realized in other graphene-based vdW structures with an interlayer twist. In this article, we mainly review the recent experimental advances on the strongly correlated physics of the magic-angle TBG (MATBG) and the small-angle twisted multilayer graphene. Lastly we will give out a perspective of this field.
Recent research showed that the rotational degree of freedom in stacking 2D materials yields great changes in the electronic properties. Here we focus on an often overlooked question: are twisted geometries stable and what defines their rotational energy landscape? Our simulations show how epitaxy theory breaks down in these systems and we explain the observed behaviour in terms of an interplay between flexural phonons and the interlayer coupling, governed by Moiré superlattice. Our argument applied to the well-studied MoS$_2$/Graphene system rationalize experimental results and could serve as…
Moiré structures in small-angle-twisted bilayers of two-dimensional semiconductors with a broken-symmetry interface form arrays of ferroelectric domains with periodically alternating out-of-plane polarization. Here, we propose a network theory for the tunability of such FE domain structure by applying an electric field perpendicular to the 2D crystal. Using multiscale analysis, we derive a fully parametrized string-theory-like description of the domain wall network and show that it undergoes a qualitative change, after the arcs of partial dislocation like domain walls merge (near the network n…
The properties of van der Waals (vdW) heterostructures are drastically altered by a tunable moiré superlattice arising from periodic variations of atomic alignment between the layers. Exciton diffusion represents an important channel of energy transport in semiconducting transition metal dichalcogenides (TMDs). While early studies performed on TMD heterobilayers have suggested that carriers and excitons exhibit long diffusion lengths, a rich variety of scenarios can exist. In a moiré crystal with a large supercell size and deep potential, interlayer excitons may be completely localized. As the…
We demonstrate that the concept of moiré flat bands can be generalized to achieve electronic band engineering in all three spatial dimensions. For many two dimensional van der Waals materials, twisting two adjacent layers with respect to each other leads to flat electronic bands in the two corresponding spatial directions -- a notion sometimes referred to as twistronics as it enables a wealth of physical phenomena. Within this two dimensional plane, large moiré patterns of nanometer size form. The basic concept we propose here is to stack multiple twisted layers on top of each other in a prede…
In van der Waals (vdW) heterostructures formed by stacking two monolayers of transition metal dichalcogenides, multiple exciton resonances with highly tunable properties are formed and subject to both vertical and lateral confinement. We investigate how a unique control knob, the twist angle between the two monolayers, can be used to control the exciton dynamics. We observe that the interlayer exciton lifetimes in $\text{MoSe}_{\text{2}}$/$\text{WSe}_{\text{2}}$ twisted bilayers (TBLs) change by one order of magnitude when the twist angle is varied from 1$^\circ$ to 3.5$^\circ$. Using a low-en…
Magnetic van der Waals (vdW) materials have been heavily pursued for fundamental physics as well as for device design. Despite the rapid advances, so far magnetic vdW materials are mainly insulating or semiconducting, and none of them possesses a high electronic mobility - a property that is rare in layered vdW materials in general. The realization of a magnetic high-mobility vdW material would open the possibility for novel magnetic twistronic or spintronic devices. Here we report very high carrier mobility in the layered vdW antiferromagnet GdTe3. The electron mobility is beyond 60,000 cm2 V…
The weak antilocalization (WAL) effect is known as a quantum correction to the classical conductivity, which never appeared in two-dimensional magnets. In this work, we reported the observation of a WAL effect in the van der Waals ferromagnet Fe5-xGeTe2 with a Curie temperature Tc ~ 270 K, which can even reach as high as ~ 120 K. The WAL effect could be well described by the Hikami-Larkin-Nagaoka and Maekawa-Fukuyama theories in the presence of strong spin-orbit coupling (SOC). Moreover, A crossover from a peak to dip behavior around 60 K in both the magnetoresistance and magnetoconductance wa…
We reveal by first-principles calculations that the interlayer binding in a twisted MoS2/MoTe2 heterobilayer decreases with increasing twist angle, due to the increase of the interlayer overlapping degree, a geometric quantity describing well the interlayer steric effect. The binding energy is found to be a Gaussian-like function of twist angle. The resistance to rotation, an analogue to the interlayer sliding barrier, can also be defined accordingly. In sharp contrast to the case of MoS2 homobilayer, here the energy band gap reduces with increasing twist angle. We find a remarkable interlayer…
There has been a huge increase of interests in two-dimensional van der Waals materials over the past ten years or so with the conspicuous absence of one particular class of materials: magnetic van der Waals systems. In this Viewpoint, we point it out and illustrate how we might be able to benefit from exploring these so-far neglected materials.
In recent years, noncollinear topological textures have long gained increasing research attentions for their high values of both fundamental researches and potential applications. The recent discovery of intrinsic orders in magnetic and polar two-dimensional van der Waals materials provides a new ideal platform for the investigation of noncollinear topological textures. Here, we review the theoretical and experimental progresses on noncollinear topological textures in two-dimensional van der Waals materials in very recent years. During these years, magnetic skyrmions of both Bloch and Néel typ…
We examined what interactions control the sign and strength of the interlayer coupling in van der Waals ferromagnets such as Fe3-xGeTe2, Cr2Ge2Te6, CrI3 and VI3, to find that high-spin orbital interaction across the van der Waals gaps are a key to understanding their ferromagnetism. Interlayer ferromagnetic coupling in Fe3-xGeTe2 Cr2Ge2Te6, and CrI3 is governed by the high-spin two-orbital two-electron destabilization, but that in VI3 by the high-spin four-orbital two-electron stabilization. These interactions explain a number of seemingly puzzling observations in van der Waals fer-romagnets.
The recent emergence of 2D van der Waals magnets down to atomic layer thickness provides an exciting platform for exploring quantum magnetism and spintronics applications. The van der Waals nature stabilizes the long-range ferromagnetic order as a result of magnetic anisotropy. Furthermore, giant tunneling magnetoresistance and electrical control of magnetism have been reported. However, the potential of 2D van der Waals magnets for magnonics, magnon-based spintronics, has not been explored yet. Here, we report the experimental observation of long-distance magnon transport in quasi-twodimensio…
The van der Waals heterostructures are a fertile frontier for discovering emergent phenomena in condensed matter systems. They are constructed by stacking elements of a large library of two-dimensional materials, which couple together through van der Waals interactions. However, the number of possible combinations within this library is staggering, and fully exploring their potential is a daunting task. Here we introduce van der Waals metamaterials to rapidly prototype and screen their quantum counterparts. These layered metamaterials are designed to reshape the flow of ultrasound to mimic ele…
Van der Waals-Casimir dispersion interactions between two apposed graphene layers, a graphene layer and a substrate, and in a multilamellar graphene system are analyzed within the framework of the Lifshitz theory. This formulation hinges on a known form of the dielectric response function of an undoped or doped graphene sheet, assumed to be of a random phase approximation form. In the geometry of two apposed layers the separation dependence of the van der Waals-Casimir interaction for both types of graphene sheets is determined and compared with some well known limiting cases. In a multilamell…
The emergence of graphene and two-dimensional van der Walls materials renewed interest to investigation of the low-frequency noise in the low-dimensional systems. The layered van der Waals materials offers unique opportunities for studying the low-frequency noise owing to the properties controlled by the thickness of these materials, and tunable carrier concentration. In this review, we describe unusual low-frequency noise phenomena in quasi-2D and quasi-1D van der Waals materials. We also demonstrate that the low-frequency noise spectroscopy is a powerful tool for investigation of the electro…
Here, we propose quantum spin Hall-like phononic states in van der Waals bilayer systems with antiferromagnetic ordering. Antiferromagnetic ordering in bilayer systems with small interlayer interaction makes the total Chern number zero, where the Chern numbers for each layer are opposite to each other. In bilayer CrI3 where antiferromagnetic ordering has been experimentally demonstrated, we show that the quantum spin Hall-like states appear with spatially separated chiral edge modes.
Research on graphene and other two-dimensional atomic crystals is intense and likely to remain one of the hottest topics in condensed matter physics and materials science for many years. Looking beyond this field, isolated atomic planes can also be reassembled into designer heterostructures made layer by layer in a precisely chosen sequence. The first - already remarkably complex - such heterostructures (referred to as 'van der Waals') have recently been fabricated and investigated revealing unusual properties and new phenomena. Here we review this emerging research area and attempt to identif…
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…
The exfoliation of two naturally occurring van der Waals minerals, graphite and molybdenite, arouse an unprecedented level of interest by the scientific community and shaped a whole new field of research: 2D materials research. Several years later, the family of van der Waals materials that can be exfoliated to isolate 2D materials keeps growing, but most of them are synthetic. Interestingly, in nature plenty of naturally occurring van der Waals minerals can be found with a wide range of chemical compositions and crystal structures whose properties are mostly unexplored so far. This Perspectiv…
The van der Waals interactions between two parallel graphitic nanowiggles (GNWs) are calculated using the coupled dipole method (CDM). The CDM is an efficient and accurate approach to determine such interactions explicitly by taking into account the discrete atomic structure. Our findings show that the van der Waals forces vary from attraction to repulsion as nanoribbons move along their lengths with respect to each other. This feature leads to a number of stable and unstable positions of the system during the movement process. These positions can be tuned by changing the length of GNW. Moreov…
We propose a tubal van der Waals heterostructure by rolling up the graphene and MoS2 atomic layers into a tubal form. We illustrate that the interlayer space for the tubal van der Waals heterostructure can be varied in a specific range, which is determined by the competition between the interlayer van der Waals force and the mechanical properties of the atomic layers. The variability of the interlayer space can be utilized to efficiently tune mechanical properties of the tubal van der Waals heterostructure. More specifically, we demonstrate that the Poisson's ratio of the tubal van der Waals h…
We show that the usual sum of $R^{-6}$ contributions from elements separated by distance $R$ can give \emph{qualitatively} wrong results for the electromagnetically non-retarded van der Waals interaction between non-overlapping bodies. This occurs for anisotropic nanostructures that have a zero electronic energy gap, such as nanowires, conducting nanotubes, and nano-layered systems including metals and graphene planes. In all these cases our analytic microscopic calculations give an interaction falling off with a power of separation different from the conventional value. We discuss implication…
The new-found two-dimensional antiferromagnetic GdTe$_3$ is attractive owing to its highest carrier mobility among all known layered magnetic materials, as well as its potential application for novel magnetic twistronic and spintronic devices. Here, we have used high-resolution angle-resolved photoemission spectroscopy to investigate its Fermi surface topology and low-lying electronic band structure. The Fermi surface is partially gapped by charge density wave below the transition temperature, the residual part reconstructs making GdTe$_3$ metallic. The high carrier mobility can be attributed …
We derive the exchange-correlation potential corresponding to the nonlocal van der Waals density functional [M. Dion, H. Rydberg, E. Schroder, D. C. Langreth, and B. I. Lundqvist, Phys. Rev. Lett. 92, 246401 (2004)]. We use this potential for a self-consistent calculation of the ground state properties of a number of van der Waals complexes as well as crystalline silicon. For the latter, where little or no van der Waals interaction is expected, we find that the results are mostly determined by semilocal exchange and correlation as in standard generalized gradient approximations (GGA), with the…
A new implementation is proposed for including van der Waals interactions in Density Functional Theory using the Maximally-Localized Wannier functions. With respect to the previous DFT/vdW-WF method, the present DFT/vdW-WF2 approach, which is based on the simpler London expression and takes into account the intrafragment overlap of the localized Wannier functions, leads to a considerable improvement in the evaluation of the $C_6$ van der Waals coefficients, as shown by the application to a set of selected dimers. Preliminary results on Ar on graphite and Ne on the Cu(111) metal surface suggest…
A literature survey of experimentally measured mobility values for the two-dimensional materials MoS2, MoSe2, MoTe2, WS2, WSe2, and black phosphorous carried out during 2015.
The application of new materials in nanotechnology opens new perspectives and enables ground-breaking innovations. Two-dimensional van der Waals materials and more specific, 2D chalcogenides are a promising class of new materials awaiting their usage in the semiconductor industry. However, the integration of van der Waals materials relying on industry-compatible manufacturing processes is still a major challenge. This is currently restricting the application of these new materials to the research laboratories environment only. The large-area and single-crystalline growth of van der Waals mater…
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%.
Although sheets of layered van der Waals solids offer great opportunities to custom-design nanomaterial properties, their weak interlayer adhesion challenges structural stability against mechanical deformation. Here, bending-induced delamination of multilayer sheets is investigated by molecular dynamics simulations, using graphene as an archetypal van der Waals solid. Simulations show that delamination of a graphene sheet occurs when its radius of curvature decreases roughly below $R_c=5.3\text{nm}\times (\text{number of layers})^{3/2}$ and that, as a rule, one-third of the layers get delamina…
Heat conduction mechanisms in superlattices could be different across different types of interfaces. Van der Waals superlattices are structures physically assembled through weak van der Waals interactions by design, and may host properties beyond the traditional limits of lattice matching and processing compatibility, offering new types of interfaces. In this work, natural van der Waals (SnS)1.17(NbS2)n superlattices are synthesized, and their thermal conductivities are measured by time-domain thermoreflectance as a function of interface density. Our results show that heat conduction of (SnS)1…
Adhesion is a key issue for researchers of various fields, it is therefore of uppermost importance to understand the parameters that are involved. Commonly, only surface parameters are employed to determine the adhesive forces between materials. Yet, van der Waals forces act not only between atoms in the vicinity of the surface, but also between atoms in the bulk material. In this review, we describe the principles of van der Waals interactions and outline experimental and theoretical studies investigating the influence of the subsurface material on adhesion. In addition, we present a collecti…
We establish a general equivalence between van der Waals interaction energies within the formalism of the non-local van der Waals functional of the density functional theory and within the formalism of the field approach based on the secular determinants of the electromagnetic field modes. We then compare the two methods explicitly in the case of a planparallel geometry with a continuously varying dielectric response function and show that their respective numerical implementations are not equivalent. This allows us to discuss the merits of the two approaches and possible advantages of either …
We propose a practical approach to spin-polarized systems within the van der Waals density functional (vdW-DF). The method was applied to a gas phase oxygen molecule and a parallel (H-type) pair of oxygen molecules. It was found that vdW-DF improves the equilibrium distance and binding energy. In particular, one type of vdW-DF can describe such systems reasonably well. The van der Waals interaction has been confirmed to have an energy comparable to the magnetic one, while emerging at a distance rather longer than the latter.
We used the binding energy-bond-charge model to study the atomic bonding and electrical properties of the two-dimensional graphene/BN van der Waals heterostructure. We manipulated its atomic bonding and electrical properties by manufacturing defects. We discovered that this process yielded a band structure with a flat band, i.e., a horizontal band structure without dispersion at the Fermi level. Thus, our research is significant because it is the first report on this flat band of defect graphene/BN van der Waals heterostructures.
A simple and computationally efficient scheme to calculate approximate imaginary-frequency dependent polarizability, hence asymptotic van der Waals coefficient, within density functional theory is proposed. The dynamical dipolar polarizabilities of atoms and molecules are calculated starting from the Thomas-Fermi-von Weizsäcker (TFvW) approximation for the independent-electron kinetic energy functional. The van der Waals coefficients for a number of closed-shell ions and a few molecules are hence calculated and compared with available values obtained by fully first-principles calculations. The…
Using the density functional theory calculations, we studied the ferroelectric, electrical and optical properties of series of bias-controllable endohedral fullerenes (TM@C28, TM= Ti-Ni). The important finding is that Cr@C28 has a large electric dipole moment and an appropriate bandgap (~1.2eV) as building blocks for ferroelectric-photovoltaic materials. By sandwiching Cr@C28 molecules between two van der Waals layers, e.g., graphene or transition metal dichalcogenides, the heterostructures may have exotic ferroelectric and photovoltaic properties with high tunability and performance.
Ubiquitous Van der Waals interactions between atoms and molecules are important for many molecular and solid structures. These systems are often studied from first principles using the Density Functional Theory (DFT). However, the commonly used DFT functionals fail to capture the essence of Van der Waals effects. Many attempts to correct for this problem have been proposed, which are not completely satisfactory because they are either very complex and computationally expensive or have a basic semiempirical character. We here describe a novel approach, based on the use of the Maximally-Localize…
Detailed experimental data for physisorption potential-energy curves of H2 on low-indexed faces of Cu challenge theory. Recently, density-functional theory has been developed to also account for nonlocal correlation effects, including van der Waals forces. We show that one functional, denoted vdW-DF2, gives a potential-energy curve promisingly close to the experiment-derived physisorptionenergy curve. The comparison also gives indications for further improvements of the functionals.
The aim of this study is to clarify the physics which governs the transition from epsilon phase to zeta phase of solid oxygen observed experimentally at 96 GPa using density functional theory (DFT). The transition was predicted at 40 GPa with PBE functional. Then the Hubbard correction was added to enhance the localization of p-orbital of oxygen. The epsilon-zeta transition pressure was significantly improved to 70 GPa. Finally, we included the non-local van der Waals correction. The transition pressure slightly increases to 80 GPa. These results demonstrate that the contribution from Hubbard …
We present fully ab-initio calculations of van der Waals coefficients for two different situations: i) the interaction between hydrogenated silicon clusters; and ii) the interactions between these nanostructures and a non metallic surface (a silicon or a silicon carbide surface). The methods used are very efficient, and allow the calculation of systems containing hundreds of atoms. The results obtained are further analyzed and understood with the help of simple models. These models can be of interest for molecular dynamics simulations of silicon nanostructures on surfaces, where they can give …
We study the dependence of the heat transfer and the van der Waals friction between two semi-infinite solids on the dielectric properties of the bodies. We show that the heat transfer and van der Waals friction at short separation between the solids may increase by many orders of magnitude when the surfaces are covered by adsorbates, or can support low-frequency surface plasmons. In this case the heat transfer and van der Waals friction are determined by resonant photon tunneling between adsorbate vibrational modes, or surface plasmon modes. The enhancement of the van der Waals friction is esp…
We study the mutual interactions of simple, parallel polymers and nanotubes, and develop a scheme to include the van der Waals interactions in the framework of density functional theory (DFT) for these molecules at intermediate to long-range separations. We primarily focus on the polymers polyethylene, isotactic polypropylene, and isotactic polyvinylchloride, but our approach applies more generally to all simple polymers and nanotubes. From first-principle DFT calculations we extract the electron density of the polymers and their static electric response. We derive explicit expressions for the…
We apply a range of density-functional-theory-based methods capable of describing van der Waals interactions to weakly bonded layered solids in order to investigate their accuracy for extended systems. The methods under investigation are the local density approximation, semi-empirical force fields, non-local van der Waals density functionals and the random-phase approximation. We investigate the equilibrium geometries, elastic constants and the binding energies of a large and diverse set of compounds and arrive at conclusions about the reliability of the different methods. The study also point…
The transition of van der Waals to Casimir forces between macroscopic gold surfaces is investigated by Atomic Force Microscopy in the plane-sphere geometry. It was found that the transition appears to take place at separations about 10 % the plasma wavelength for evaporated gold surfaces, which compares to theoretical predictions by incorporation of experimental optical data and roughness corrections. Moreover, the force data allow estimation of the Hamaker constant AH in the van der Waals regime, which is in good agreement with the Lifshitz theory predictions (even if roughness corrections ar…
The cohesive energy, equilibrium lattice constant, and bulk modulus of noble metals are computed by different van der Waals-corrected Density Functional Theory methods, including vdW-DF, vdW-DF2, vdW-DF-cx, rVV10 and PBE-D. Two specifically-designed methods are also developed in order to effectively include dynamical screening effects: the DFT/vdW-WF2p method, based on the generation of Maximally Localized Wannier Functions, and the RPAp scheme (in two variants), based on a single-oscillator model of the localized electron response. Comparison with results obtained without explicit inclusion o…
The Lifshitz-type formulas describing the free energy and the force of the van der Waals interaction between an atom (molecule) and a single-wall carbon nanotube are obtained. The single-wall nanotube is considered as a cylindrical sheet carrying a two-dimensional free electron gas with appropriate boundary conditions on the electromagnetic field. The obtained formulas are used to calculate the van der Waals free energy and force between a hydrogen atom (molecule) and single-wall carbon nanotubes of different radia. Comparison studies of the van der Waals interaction of hydrogen atoms with sin…
We study the van der Waals friction between two flat metal surfaces in relative motion. For good conductors we find that normal relative motion gives a much larger friction than for parallel relative motion. The friction may increase by many order of magnitude when the surfaces are covered by adsorbates, or can support low-frequency surface plasmons. In this case the friction is determined by resonant photon tunneling between adsorbate vibrational modes, or surface plasmon modes.
The van der Waals friction between two semi-infinite solids, and between a small neutral particle and semi-infinite solid is reconsidered on the basis of thermal quantum field theory in the Matsubara formulation. The calculation of the friction to linear order in the sliding velocity is reduced to the finding of the equilibrium Green functions. Thus this approach cab be extended for bodsies with complex geometry. The friction calculated in this approach agrees with the friction calculated using a dynamical modification of the Lifshitz theory, which is based on the fluctuation-dissipation there…
Van der Waals magnets have emerged as a fertile ground for the exploration of highly tunable spin physics and spin-related technology. Two-dimensional (2D) magnons in van der Waals magnets are collective excitation of spins under strong confinement. Although considerable progress has been made in understanding 2D magnons, a crucial magnon device called the van der Waals magnon valve, in which the magnon signal can be completely and repeatedly turned on and off electrically, has yet to be realized. Here we demonstrate such magnon valves based on van der Waals antiferromagnetic insulator MnPS3. …
