The combination of metallicity and ferroelectricity breaks traditional boundaries, paving new avenues for innovative electronic materials and devices. This breakthrough is particularly notable, as metallicity and ferroelectricity have traditionally been considered mutually exclusive physical properties. In this work, starting with non-polar metallic single layers, we propose a general scheme for designing 2D ferroelectric metals (FEMs) based on van der Waals interaction. By first-principles calculations, we further substantiate the feasibility of the design scheme in real materials such as FeSe and H-MnTe2. Notably, this scheme unveils unique metallic ferroelectricity, characterized by reversing polarization through interlayer sliding. Furthermore, the combination of inherent magnetism with sliding ferroelectricity leads to multiferroicity. The investigated design scheme and observed phenomena have broad applicability across 2D materials. Our results not only pave the way for research in 2D FEMs but also offer promising prospects for foundational studies of coupled physical phenomena in 2D lattices.
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.
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.
2D intercorrelated ferroelectrics, exhibiting a coupled in-plane and out-of-plane ferroelectricity, is a fundamental phenomenon in the field of condensed-mater physics. The current research is based on the paradigm of bi-directional inversion asymmetry in single-layers, which restricts 2D intercorrelated ferroelectrics to extremely few systems. Herein, we propose a new scheme for achieving 2D intercorrelated ferroelectrics using van der Waals (vdW) interaction, and apply this scheme to a vast family of 2D vdW materials. Using first-principles, we demonstrate that 2D vdW multilayers-for example…
We show how van der Waals (vdW) forces outcompete covalent and ionic forces to control ferroelectric ordering in CuInP2S6 nanoflakes as well as in CuInP2S6 and CuBiP2Se6 crystals. While the self-assembly of these 2D layered materials is clearly controlled by vdW effects, this result indicates that the internal layer structure is also similarly controlled. Using up to 14 first-principles computational methods, we predict that the bilayers of both materials should be antiferroelectric. However, antiferroelectric nanoflakes and bulk materials are shown to embody two fundamentally different types …
Coexistence of ferromagnetism and ferroelectricity in the van der Waals multiferroic CuIn0.2V0.8P2S6
D crystal consortium, Materials Research Institute, Pennsylvania State University（宾夕法尼亚州立大学材料研究所）；Department of Physics, Pennsylvania State University（宾夕法尼亚州立大学物理系）；Department of Electrical and Computer Engineering and Quantum Technology Center, University of Maryland（马里兰大学电气与计算机工程系及量子技术中心）；Department of Chemistry, Michigan State University（密歇根州立大学化学系）；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）
Van der Waals (vdW) layered materials have rather weaker interlayer bonding than the intra-layer bonding, therefore the exfoliation along the stacking direction enables the achievement of monolayer or few layers vdW materials with emerging novel physical properties and functionalities. The ferroelectricity in vdW materials recently attracts renewed interest for the potential use in high-density storage devices. As the thickness going thinner, the competition between the surface energy, depolarization field and interfacial chemical bonds may give rise to the modification of ferroelectricity and…
The interest in ferroelectric van der Waals crystals arises from the potential to realize ultrathin ferroic systems owing to the reduced surface energy of these materials and the layered structure that allows for exfoliation. Here, we quantitatively unravel giant negative electrostriction of van der Waals layered copper indium thiophosphate (CIPS), which exhibits an electrostrictive coefficient Q33 as high as -3.2 m4/C2 and a resulting bulk piezoelectric coefficient d33 up to -85 pm/V. As a result, the electromechanical response of CIPS is comparable in magnitude to established perovskite ferr…
The van der Waals layered material CuInP2S6 features interesting functional behavior, including the existence of four uniaxial polarization states, polarization reversal against the electric field through Cu ion migration, a negative-capacitance regime, and reversible extraction of Cu ions. At the heart of these characteristics lies the high mobility of Cu ions, which also determines the spontaneous polarization. Therefore, Cu migration across the lattice results in unusual ferroelectric behavior. Here, we demonstrate how the interplay of polar and ionic properties provides a path to ionically…
Quantum spin Hall insulators (QSHI) have been proposed to power a number of applications, many of which rely on the possibility to switch on and off the non-trivial topology. Typically this control is achieved through strain or external electric fields, which require energy consumption to be maintained. On the contrary, a non-volatile mechanism would be highly beneficial and could be realized through ferroelectricity if opposite polarization states are associated with different topological phases. While this is not possible in a single ferroelectric material where the two polarization states a…
Layered indium selenides ($In_{2}Se_{3}$) have recently been discovered to host robust out-of-plane and in-plane ferroelectricity in the $α$ and $β$' phases, respectively. In this work, we utilise angle-resolved photoelectron spectroscopy to directly measure the electronic bandstructure of $β'-In_{2}Se_{3}$, and compare to hybrid density functional theory (DFT) calculations. In agreement with DFT, we find the band structure is highly two-dimensional, with negligible dispersion along the c-axis. Due to n-type doping we are able to observe the conduction band minima, and directly measure the min…
A ferroelectric junction transistor memory made from switchable van der Waals p-n heterojunctions
Zhejiang University（浙江大学）；King Abdullah University of Science and Technology（阿卜杜拉国王科技大学）；Wenzhou University（温州大学）；Chinese Academy of Sciences（中国科学院）；South China Normal University（华南师范大学）；Xidian University（西安电子科技大学）
Ferroelectric van der Waals heterostructures provide a natural platform to design a variety of electrically controllable devices. In this work, we demonstrate that AB bilayer graphene encapsulated in MoTe$_2$ acts as a valley valve that displays a switchable built-in topological gap, leading to ferroelectrically driven topological channels. Using a combination of ab initio calculations and low energy models, we show that the ferroelectric order of MoTe$_2$ allows the control of the gap opening in bilayer graphene and leads to topological channels between different ferroelectric domains. Moreov…
Ferroelecticity, one of the keys to realize nonvolatile memories owing to the remanent electric polarization, has been an emerging phenomenon in the two-dimensional (2D) limit. Yet the demonstrations of van der Waals (vdW) memories using 2D ferroelectric materials as an ingredient are very limited. Especially, gate-tunable ferroelectric vdW memristive device, which holds promises in future neuromorphic applications, remains challenging. Here, we show a prototype gate-programmable memory by vertically assembling graphite, CuInP2S6, and MoS2 layers into a metal-ferroelectric-semiconductor archit…
Layer-polarized anomalous Hall effect (LP-AHE), derived from the coupling between Berry curvature and layer degree of freedom, is of importance for both fundamental physics and device applications. Nonetheless, the current research paradigm is rooted in topological systems, rendering such phenomenon rather scarce. Here, through model analysis, we propose an alternative, but general mechanism to realize the LP-AHE in valleytronic van der Waals bilayers by interlayer sliding. The interaction between the out-of-plane ferroelectricity and A-type antiferromagnetism gives rise to the layer-locked Be…
Many-body description of two-dimensional van der Waals ferroelectric $α-$In$_2$Se$_3$
National Laboratory of the Rockies（落基山国家实验室）；Department of Physics, University at Buffalo, State University of New York（纽约州立大学布法罗分校物理系）；Department of Physics, King’s College London（伦敦国王学院物理系）；Eastern Institute for Advanced Study, Eastern Institute of Technology（东部理工学院前沿研究院）；Department of Physics and Astronomy, University of Nebraska-Lincoln（内布拉斯加大学林肯分校物理与天文学系）
Magnetic skyrmions are chiral nanoscale spin textures which are usually induced by Dzyaloshinskii-Moriya interaction (DMI). Recently, magnetic skyrmions have been observed in two-dimensional (2D) van der Waals (vdW) ferromagnetic materials, such as Fe$_{3}$GeTe$_{2}$. The electric control of skyrmions is important for their potential application in low-power memory technologies. Here, we predict that DMI and magnetic skyrmions in a Fe$_{3}$GeTe$_{2}$ monolayer can be controlled by ferroelectric polarization of an adjacent 2D vdW ferroelectric In$_{2}$Se$_{3}$. Based on density functional theor…
Multiferroic materials are potential to be applied in novel magnetoelectric devices, for example, high-density non-volatile storage. Last decades, research on multiferroic materials was focused on three-dimensional (3D) materials. However, 3D materials suffer from the dangling bonds and quantum tunneling in the nano-scale thin films. Two-dimensional (2D) materials might provide an elegant solution to these problems, and thus are highly on demand. Using first-principles calculations, we predict ferromagnetism and driven ferroelectricity in the monolayer and even a few-layers of CuCrP2S6. Althou…
The discoveries of magnetism and ferroelectricity in 2D van der Waals (vdW) materials have brought important functionalities to the 2D materials family, and may trigger a revolution in next generation nanoelectronics and spintronics. In this perspective article, we briefly review the recent progress in the field of 2D ferroelectrics, focusing on the mechanisms that drive spontaneous polarizations in 2D systems, unique properties brought about by the reduced lattice dimensionality, and promising applications of 2D ferroelectrics. At the end, we provide an outlook for challenges that need to be …
Ferroelectric tuning of the valley polarized metal-semiconductor transition in Mn2P2S3Se3/Sc2CO2 van der Waals heterostructures and application to nonlinear Hall effect devices
Room-Temperature Noncolinear Ferroelectricity in van der Waals WO$_2$Cl$_2$ with a Wide Bandgap
Key Laboratory of Quantum Materials and Devices of Ministry of Education, School of Physics, Southeast University（东南大学物理学院量子材料与器件教育部重点实验室）；School of Advanced Materials and Nanotechnology, Xidian University（西安电子科技大学先进材料与纳米技术学院）；Jiangsu Key Laboratory of Advanced Laser Materials and Devices, School of Physics and Electronic Engineering, Jiangsu Normal University（江苏师范大学物理与电子工程学院江苏省先进激光材料与器件重点实验室）；Information Materials and Intelligent Sensing Laboratory of Anhui Province, Institutes of Physical Science and Information Technology, Anhui University（安徽大学物质科学与信息技术研究院安徽省信息材料与智能感知实验室）；College of Science, Hebei University of Science and Technology（河北科技大学理学院）；Quantum Innovation Centre (Q. InC), Agency for Science, Technology and Research (A*STAR)（新加坡科技研究局量子创新中心）；Chaotic Matter Science Research Center, Department of Materials, Metallurgy and Chemistry & Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry, Jiangxi University of Science and Technology（江西理工大学材料冶金化学系混沌物质科学研究中心江西省功能分子材料化学重点实验室）
Realizing a state of matter in two dimensions has repeatedly proven a novel route of discovering new physical phenomena. Van der Waals (vdW) materials have been at the center of these now extensive research activities. They offer a natural way of producing a monolayer of matter simply by mechanical exfoliation. This work demonstrates that the possible multiferroic state with coexisting antiferromagnetic and ferroelectric orders possibly persists down to the bilayer flake of NiI$_{2}$. By exploiting the optical second-harmonic generation technique, both magnitude and direction of the ferroelect…
Following the recent demonstration that van der Waals forces control the ferroelectric ordering of layers within nanoflakes and bulk samples of CuBiP2Se6 and CuInP2S6, it is demonstrated that they also control the internal geometrical structure of isolated monolayers of these materials. This internal structure involves large displacements of the copper atoms, either normal to the layer plane or else within the plane, that change its ligation environment. In both cases, the van der Waals dispersion force out-competes traditional bonding effects to control structure. However, we find that the as…
Composition-Driven Tunable Optical and Electrical Properties in Van der Waals Ferroelectric NbOI2-xClx Alloys
Dalian University of Technology（大连理工大学）；Dalian University of Technology and Belarusian State University Joint Institute, Dalian University of Technology（大连理工大学与白俄罗斯国立大学联合研究院）；Belarusian State University（白俄罗斯国立大学）；Belarusian National Technical University（白俄罗斯国立技术大学）
Efficient high-harmonic generation in van der Waals ferroelectric NbOI$_2$ crystals
International Center for Quantum Materials, School of Physics, Peking University（北京大学物理学院量子材料国际中心）；School of Science, Nanjing University of Posts and Telecommunications（南京邮电大学理学院）；Institute of Ultrafast Optical Physics, Department of Applied Physics, Nanjing University of Science and Technology（南京理工大学应用物理系超快光学研究所）；Beijing Academy of Quantum Information Sciences（北京量子信息科学研究院）
Multiferroic materials with coupled ferroelectric and ferromagnetic properties are important for multifunctional devices due to their potential ability of controlling magnetism via electric field, and vice versa. The recent discoveries of two-dimensional ferromagnetic and ferroelectric materials have ignited tremendous research interest and aroused hope to search for two-dimensional multiferroics. However, intrinsic two-dimensional multiferroic materials and, particularly, those with strong magnetoelectric couplings are still rare to date. In this paper, using first-principles simulations, we …
