We develop a computational database, web-apps, and machine-learning (ML) models to accelerate the design and discovery of two-dimensional (2D)-heterostructures. Using density functional theory (DFT) based lattice-parameters and electronic band-energies for 674 non-metallic exfoliable 2D-materials, we generate 226,779 possible heterostructures. We classify these heterostructures into type-I, II and III systems according to Andersons rule, which is based on the relative band-alignments of the non-interacting monolayers. We find that type-II is the most common and the type-III the least common heterostructure type. We subsequently analyze the chemical trends for each heterostructure type in terms of the periodic table of constituent elements. The band alignment data can be also used for identifying photocatalysts and high-work function 2D-metals for contacts. We validate our results by comparing them to experimental data as well as hybrid-functional predictions. Additionally, we carry out DFT calculations of a few selected systems (MoS2/WSe2, MoS2/h-BN, MoSe2/CrI3), to compare the band-alignment description with the predictions from Andersons rule. We develop web-apps to enable users to virtually create combinations of 2D materials and predict their properties. Additionally, we use ML tools to predict band-alignment information for 2D materials. The web-apps, tools and associated data will be distributed through JARVIS-Heterostructure website (https://jarvis.nist.gov/jarvish/). Our analysis, results and the developed web-apps can be applied to the screening and design applications, such as finding novel photocatalysts, photodetectors, and high-work function (WF) 2D-metal contacts.
The unique physics found in moiré superlattices of twisted or lattice-mismatched atomic layers hold great promise for future quantum technologies. However, twisted configurations are typically thermodynamically unfavorable, making the accurate twist angle control in direct growth implausible. While rotationally aligned moiré superlattices based on lattice-mismatched layers such as WSe2/WS2 can be synthesized, they lack the critical tunability of the moiré period and the moiré formation mechanisms are not well-understood. Here, we report the scalable, thermodynamically driven van der Waals epit…
Artificially engineered 2D materials offer unique physical properties for thermal management, surpassing naturally occurring materials. Here, using van der Waals epitaxy, we demonstrate the ability to engineer extremely insulating ultra-thin thermal metamaterials based on crystalline lattice-mismatched Bi2Se3/MoSe2 superlattices and graphene/PdSe2 heterostructures with exceptional thermal resistances (70-202 m^2K/GW) and ultralow cross-plane thermal conductivities (0.01-0.07 Wm^-1K^-1) at room temperature, comparable to those of amorphous materials. Experimental data obtained using frequency-d…
Nanobelts, nanoribbons and other quasi-one-dimensional nanostructures formed from layered, so-called, van der Waals semiconductors have garnered much attention due to their high-performance, tunable optoelectronic properties. For layered alloys made from the gallium monochalcogenides GaS, GaSe, and GaTe, near-continuous tuning of the energy bandgap across the full composition range has been achieved in GaSe1-xSx and GaSe1-xTex alloys. Gold-catalyzed vapor-liquid-solid (VLS) growth of these alloys yields predominantly nanobelts, nanoribbons and other nanostructures for which the fast crystal gr…
Moiré lattices which consist of parallel but staggered periodic lattices have been extensively explored due to their salient physical properties, such as van Hove singularities[1, 2], commensurable incommensurable transitions[3], non-Abelian gauge potentials[4], fractional quantum Hall effects[5-7], van der Waals interfaces[8, 9] and unconventional superconductivity[10, 11]. However, there are limited demonstrations of such concepts for classical wave systems. Here, we realized gauge fields in one-dimensional Moiré phononic lattices consisting of two superimposed periodic patterns which mismat…
Remote epitaxy on monolayer graphene is promising for synthesis of highly lattice mismatched materials, exfoliation of free-standing membranes, and re-use of expensive substrates. However, clear experimental evidence of a remote mechanism remains elusive. In many cases, due to contaminants at the transferred graphene/substrate interface, alternative mechanisms such as pinhole-seeded lateral epitaxy or van der Waals epitaxy can explain the resulting exfoliatable single-crystalline films. Here, we find that growth of the Heusler compound GdPtSb on clean graphene on sapphire substrates produces a…
Flexo-Strain Engineering of Phonons and Ferrons in Thin Films of Van der Waals Ferrielectrics
Institute of Physics, National Academy of Sciences of Ukraine（乌克兰国家科学院物理研究所）；Frantsevich Institute for Problems in Materials Science, National Academy of Sciences of Ukraine（乌克兰国家科学院弗拉采维奇材料科学问题研究所）；Department of Materials Science and Engineering, University of Wisconsin-Madison（威斯康星大学麦迪逊分校材料科学与工程系）；V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine（乌克兰国家科学院V.拉什卡廖夫半导体物理研究所）；Department of Microelectronics, Igor Sikorsky Kyiv Polytechnic Institute（伊戈尔·西科尔斯基基辅理工学院微电子系）；Institute of Solid-State Physics and Chemistry, Uzhhorod University（乌日霍罗德大学固体物理与化学研究所）；Department of Materials Science and Engineering, Pennsylvania State University（宾夕法尼亚州立大学材料科学与工程系）
Directionally Locked Heteroepitaxy with a Structurally Modulated van der Waals Material
Princeton University（普林斯顿大学）；Princeton Materials Institute（普林斯顿材料研究所）；Donostia International Physics Center（圣塞巴斯蒂安国际物理中心）；University of the Basque Country (UPV/EHU)（巴斯克大学）；Boston College（波士顿学院）；The Hong Kong University of Science and Technology（香港科技大学）；Indian Institute of Technology Guwahati（印度理工学院古瓦哈提分校）；National Institute for Materials Science（日本国立材料研究所）；Centro de Física de Materiales (CSIC-UPV/EHU)（材料物理中心）；Université de Sherbrooke（舍布鲁克大学）
Presently a lot of efforts are devoted to the investigation of new two-dimensional magnetic materials, which are considered as promising for the realization of the future electronics and spintronics devices. However, the utilization of these materials in different junctions requires complicated processing that in many cases leads to unwanted parasitic effects influencing the performance of the junctions. Here, we propose the new elegant approach for the realization of the "one-material"-based magnetic tunnel junction. The several layers of 2D van der Waals MnPX3 (X: S, Se), which is insulating…
We present vibrational properties of Franckeite, which is a naturally occurring van der Waals heterostructure consisting of two different semiconducting layers. Franckeite is a complex layered crystal composed of alternating SnS$_2$ like pseudohexagonal and PbS-like pseudotetragonal layers stacked on top of each other, providing a unique platform to study vibrational properties and thermal transport across layers with mass density and phonon mismatches. By using micro-Raman spectroscopy and first-principles Raman simulations, we found that the PbS-like pseudotetragonal structure is mostly comp…
Retrieving optical parameters of emerging van der Waals flakes
ICFO-Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology（ICFO-光子科学研究所，巴塞罗那科学技术研究院）；Department of Electrical Engineering, Ferdowsi University of Mashhad（马什哈德费尔多西大学电气工程系）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（国家材料科学研究所电子与光学材料研究中心）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（国家材料科学研究所材料纳米架构研究中心）
Moiré superlattices from stacks of van der Waals materials offer an exciting arena in the fields of condensed matter physics and materials science. Typically, these moiré superlattices consist of materials with identical or similar structures, and the long moiré period arises from a small twist angle or lattice mismatch. In this article, we discuss that long moiré period appears in a new moiré system by stacking two dissimilar van der Waals layers with large lattice mismatch, resulting in couplings between moiré bands from remote valleys in the momentum space. In this system, the first layer i…
Bandgap engineering and quantum confinement in semiconductor heterostructures provide the means to fine-tune material response to electromagnetic fields and light in a wide range of the spectrum. Nonetheless, forming semiconductor heterostructures on lattice-mismatched substrates has been a challenge for several decades, leading to restrictions for device integration and the lack of efficient devices in important wavelength bands. Here, we show that the van der Waals epitaxy of two-dimensional (2D) GaSe and InSe heterostructures occur on substrates with substantially different lattice paramete…
Spectrally Programmable Spin-Polarized Photocurrents in WSe$_2$-NiPS$_3$ Magnetic van der Waals Heterostructures
Bar-Ilan University（巴伊兰大学）；Technical University of Darmstadt（达姆施塔特工业大学）；Technische Universität Dresden（德累斯顿工业大学）；Center for Advanced Systems Understanding, CASUS, HZDR（先进系统理解中心，CASUS，HZDR）；Yonsei University（延世大学）
Van der Waals (vdW) tunnel junctions are attractive due to their atomically sharp interface, gate tunablity, and robustness against lattice mismatch between the successive layers. However, the negative differential resistance (NDR) demonstrated in this class of tunnel diodes often exhibits noisy behaviour with low peak current density, and lacks robustness and repeatability, limiting their practical circuit applications. Here we propose a strategy of using a 1L-WS$_2$ as an optimum tunnel barrier sandwiched in a broken gap tunnel junction of highly doped black phosphorus (BP) and SnSe$_2$. We …
When two-dimensional van der Waals materials are stacked to build heterostructures, moiré patterns emerge from twisted interfaces or from mismatch in lattice constant of individual layers. Relaxation of the atomic positions is a direct, generic consequence of the moiré pattern, with many implications for the physical properties. Moiré driven atomic relaxation may be naively thought to be restricted to the interfacial layers and thus irrelevant for multi-layered heterostructures. However, we provide experimental evidence for the importance of the three dimensional nature of the relaxation in tw…
Designer three-dimensional electronic bands in asymmetric transition metal dichalcogenide heterostructures
Monash University（蒙纳士大学）；University of Manchester（曼彻斯特大学）；Syarif Hidayatullah State Islamic University Jakarta（雅加达希达亚图拉国立伊斯兰大学）；Flinders University（弗林德斯大学）；Tohoku University（东北大学）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；Pennsylvania State University（宾夕法尼亚州立大学）
Three-Dimensional Non-Foliated Fractional Quantum Hall Phases with Irrational Anyons in Twisted van der Waals Multilayers
Pohang University of Science and Technology（浦项科技大学）；Daegu Gyeongbuk Institute of Science and Technology (DGIST)（大邱庆北科学技术院）；Korea Advanced Institute of Science and Technology（韩国科学技术院）；Institute for Basic Science（基础科学研究院）
Combining various two-dimensional materials into novel van der Waals (vdW) heterostructures has been shown to lead to new emergent quantum systems. A novel heterostructure composed of a vdW topological insulator (TI) such as Bi$_{2}$Se$_{3}$ with a quantum spin liquid (QSL) such as $α$-RuCl$_{3}$ is of great interest for the potential for the chiral Dirac electrons in the TI surface states to interact strongly with the fractionalized fermionic spin excitations in the QSL. We report the heteroepitaxial growth of Bi$_{2}$Se$_{3}$ thin films on $α$-RuCl$_{3}$ as well as the characterization of th…
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。
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…
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…
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.
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.
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…
Efficient calculation of van der Waals dispersion coefficients with time-dependent density functional theory in real time: application to polycyclic aromatic hydrocarbons
