It is known that ab initio molecular dynamics (AIMD) simulations of liquid water, based on the generalized gradient approximation (GGA) to density functional theory (DFT), yield structural and diffusive properties in reasonable agreement with experiment only if artificially high temperatures are used in the simulations. The equilibrium density, at normal conditions, of DFT water has been recently shown by Schmidt et al. [J. Phys. chem. B, 113, 11959 (2009)] to be underestimated by different GGA functionals for exchange and correlation, and corrected by the addition of interatomic pair potentials to describe van derWaals (vdW) interactions. In this contribution we present a DFTAIMD study of liquid water using several GGA functionals as well as the van der Waals density functional (vdW-DF) of Dion et al. [Phys. Rev. Lett. 92, 246401(2004)]. As expected, we find that the density of water is grossly underestimated by GGA functionals. When a vdW-DF is used, the density improves drastically and the experimental diffusivity is reproduced without the need of thermal corrections. We analyze the origin of the density differences between all the functionals. We show that the vdW-DF increases the population of non-H-bonded interstitial sites, at distances between the first and second coordination shells. However, it excessively weakens the H-bond network, collapsing the second coordination shell. This structural problem is partially associated to the choice of GGA exchange in the vdW-DF. We show that a different choice for the exchange functional is enough to achieve an overall improvement both in structure and diffusivity.
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 recent non-local correlation functional of Vydrov and van Voorhis[J. Chem. Phys. 133, 244103 (2010)] is investigated and two new versions of the functional are suggested as being appropriate for describing van der Waals interactions in solids. A refitting of the original functional is demonstrated to result in very accurate interlayer binding energies for weakly bonded layered solids. A VV10 functional based on the generalized gradient approximation by Armiento and Mattsson[Phys. Rev. B 72, 085108 (2005)], while performing slightly worse for interlayer binding is highly successful in descr…
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 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…
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.
Van der Waals density functional: Self-consistent potential and the nature of the van der Waals bond
我们导出了对应于非定域范德华密度泛函的交换关联势[M。迪翁，H。Rydberg，E. Schroder，D. C. Langreth，和B. I. Lundqvist，《物理评论快报》92，246401（2004）]。我们使用这种潜在的自洽计算的基态属性的一些范德华络合物以及晶体硅。对于后者，很少或没有范德华相互作用的预期，我们发现，结果主要是由半局部交换和相关性在标准的广义梯度近似（GGA），与完全非局部项几乎没有影响。另一方面，我们的研究结果表明，范德瓦尔斯复合物的自洽在平衡分离的影响不大。这一发现验证了以前的计算与相同的功能，治疗完全非本地项作为一个后GGA扰动。我们的结果与波函数计算的比较表明，我们的方法的实用性。交换相关势也使我们能够计算赫尔曼-费曼力，从而提供了有效的几何弛豫方法，并释放了依赖于自洽电荷分布的其他标准技术的潜在用途。范德瓦尔斯键的性质进行了讨论的自洽键电荷。
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…
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 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.
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.
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 …
Copper indium thiophosphate, CuInP2S6, has attracted much attention in recent years due to its van der Waals layered structure and robust ferroelectricity at room temperature. In this review, we aim to give an overview of the various properties of CuInP2S6, covering structural, ferroelectric, dielectric, piezoelectric and transport properties, as well as its potential applications. We also highlight the remaining questions and possible research directions related to this fascinating material and other compounds of the same family.
We theoretically address grazing incidence fast atom diffraction (GIFAD) for H atoms impinging on a LiF(001) surface. Our model combines a description of the H-LiF(001) interaction obtained from Density Functional Theory calculations with a semi-quantum treatment of the dynamics. We analyze simulated diffraction patterns in terms of the incidence channel, the impact energy associated with the motion normal to the surface, and the relevance of Van der Waals (VdW) interactions. We then contrast our simulations with experimental patterns for different incidence conditions. Our most important find…
Among the van der Waals heterostructures, graphene/h-BN heterostructure is an appropriate candidate for 2D nanoelectronic devices. In this paper, using non-equilibrium molecular dynamics simulation approach, heat transport in bilayer graphene/h-BN and graphene/h-BN van der Waals heterostructure (i.e. h-BN flakes periodically inserted on the top and bottom of a graphene layer) are explored. The results show that by increasing the length of the system, the thermal conductivity of bilayer graphene/h-BN increases. Furthermore, it was revealed that heat transport in graphene/h-BN heterostructure en…
In controlled X-ray irradiation experiments, the formation of trap states in the prototypical van der Waals bonded semiconductor Rubrene is studied quantitatively for doses up to 82 Gy (Gy = J/kg). About 100 electronic trap states, located around 0.3 eV above the valence band, are created by each absorbed 8 keV photon which is 2-3 orders of magnitude more than 1 MeV protons produce. Thermal annealing is shown to reduce these traps. Local structural disorder, which has also been induced by other means in different studies, is thus identified as a common origin of trap states in van der Waals bo…
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.
With the example of hexagonal boron nitride, we demonstrate how the character of electron-hole (e-h) pairs in van der Waals bound low-dimensional systems is driven by layer stacking. Four types of excitons appear, with either a two- or three-dimensional spatial extension. Electron and hole distributions are either overlapping or exhibit a charge-transfer nature. We discuss under which structural and symmetry conditions they appear and they are either dark or bright. This analysis provides the key elements to identify, predict, and possibly tailor the character of e-h pairs in van der Waals mat…
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…
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.
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 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…
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…
The van de Waals interaction between two graphene sheets is studied at finite temperatures. Graphene's thermal length $(ξ_T = \hbar v / k_B T)$ controls the force versus distance $(z)$ as a crossover from the zero temperature results for $z\ll ξ_T$, to a linear-in-temperature, universal regime for $z\gg ξ_T$. The large separation regime is shown to be a consequence of the classical behavior of graphene's plasmons at finite temperature. Retardation effects are largely irrelevant, both in the zero and finite temperature regimes. Thermal effects should be noticeable in the van de Waals interactio…
A van der Waals coupled Weyl semimetal material NbIrTe4 is investigated by combining scanning tunneling microscopy/spectroscopy and first principles calculations. We observe a sharp peak in the tunneling conductance near the zero bias energy, and its origin is ascribed to a van Hove singularity associated with a Lifshitz transition of the topologically none trivial Fermi arc states. Furthermore, tunneling spectroscopy measurements show a surprisingly large signature of electron boson coupling, which presumably represents anomalously enhanced electron phonon coupling through the enhanced charge…
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. …
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…
Van der Waals heterostructures have recently garnered interest for application in high-performance photovoltaic materials. Consequently, understanding the basic electronic characteristics of these heterostructures is important for their utilisation in optoelectronic devices. The electronic structures and bond relaxation of two-dimensional (2D) Sb/transition metal disulfides (TMDs, MoSe2, and MoTe2) van der Waals heterostructures were systematically studied using the bond-charge (BC) correlation and hybrid density functional theory. We found that the Sb/MoSe2 and Sb/MoTe2 heterostructures had i…
Pristine van der Waals (vdW) interfaces between two-dimensional (2D) and other materials are core to emerging optical and electronic devices. Their direct fabrication is, however, challenged as the vdW forces are weak and cannot be tuned to accommodate integration of arbitrary layers without solvents, sacrificial-layers or high-temperatures, steps that can introduce damage. To address these limitations, we introduce a single-step 2D material-to-device integration approach in which forces promoting transfer are decoupled from the vdW forces at the interface of interest. We use this adhesive mat…
We present a phenomenological theory for coupled spin-charge dynamics in magnetic van der Waals heterostructures. The system studied consists of a layered antiferromagnet inserted into a capacitive vdW heterostructure. It has been recently demonstrated that charge doping in such layered antiferromagnets can modulate the strength, and even the sign, of exchange coupling between the layer magnetizations. This provides a mechanism for electrically generating magnetization dynamics. The central result we predict here is that the magnetization dynamics reciprocally results in inducing charge dynami…
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…
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%.
