Light-matter interaction is one of the key routes to understanding and manipulating geometric and electronic behaviors of materials, especially two-dimensional materials which are optically accessible owing to their high surface to volume ratio. In the current work we focus on the recently discovered two-dimensional sliding ferroelectric materials, in which the out-of-plane electric polarization can be switched with a small horizontal translation in one layer. Combining symmetry analysis and first-principles calculations, we predict that light illumination could inject non-equilibrium magnetic moments into the sliding ferroelectrics. Such magnetic moment is composed of both spin and orbital degrees of freedom contributions. We use $\mathrm{ZrI}_2$, $\mathrm{WTe}_2$, and $\mathrm{MoS}_2$ bilayer ferroelectrics to illustrate our theory. Under intermediate light illumination, one can yield non-equilibrium magnetic moments on the order of $0.1-1$ $μ_B$ in these systems, which also depends on the polarization nature of incident light. Furthermore, we show that such photo-injected magnetism changes its sign when the sliding dipole moment switches. This photo-magnetization can be detected by magneto-optical methods (such as Kerr or Faraday effect), which serves as an indicator of sliding ferroelectricity. Hence, one can use an all-optical pump and probe setup to measure and detect the subtle sliding ferroelectric phase.
Very recently, ferroelectric polarization in staggered bilayer hexagonal boron nitride (BBN) and its novel sliding inversion mechanism was reported experimentally (Science 2021, 372, 1458; 2021, 372, 1462), which paves a new way to realize van der Waals (vdW) ferroelectric devices with new functionalities. Here, we develop vdW sliding ferroelectric tunnel junctions (FTJs) using the sliding ferroelectric BBN unit as ultrathin barriers and explore their transport properties with different ferroelectric states and metal contacts via the first principles. It is found that the electrode/BBN contact…
Spontaneous polarization and bulk photovoltaic effect (BPVE) are two concomitant physical properties in ferroelectric materials. The flipping of ferroelectric order usually accompanies with the switching of BPVE as both of them are reversed under the inversion symmetry. In this study, we report the distinctive BPVE characters in two-dimensional (2D) interlayer sliding ferroelectric materials featuring unswitchable in-plane BPVE (light-induced photocurrent in the xy plane) and switchable out-of-plane BPVE (light-induced polarization along the z-direction). Symmetry analysis within abstract bila…
Two-dimensional materials with ferroelectric properties break the size effect of conventional ferroelectric materials and unlock unprecedented potentials of ferroelectric-related application at small length scales. In this work, using density functional theory (DFT) calculations, we discover a tribo-ferroelectricity behavior in a group of bilayer group-IV monochalcogenides (MX, with M = Ge, Sn and X = S, Se). Upon interlayer sliding over an in-plane unit cell length, the top layer exhibits a reversible intralayer ferroelectric switching, leading to a reversible transition between the ferroelec…
The bulk photovoltaic effect that is intimately associated with crystalline symmetry has been extensively studied in various nonmagnetic materials, especially ferroelectrics with a switchable electric polarization. In order to further engineer the symmetry, one could resort to spin-polarized systems possessing an extra magnetic degree of freedom. Here, we investigate the bulk photovoltaic effect in two-dimensional magnetic sliding ferroelectric (MSFE) systems, illustrated in VSe2, FeCl2, and CrI3 bilayers. The transition metal elements in these systems exhibit intrinsic spin polarization, and …
University of Wollongong（伍伦贡大学）；Singapore University of Technology and Design（新加坡科技设计大学）；Tiangong University（天津工业大学）；The Hong Kong Polytechnic University（香港理工大学）
When the atomic layers in a non-centrosymmetric van der Waals structure slide against each other, the interfacial charge transfer results in a reversal of the structures spontaneous polarization. This phenomenon is known as sliding ferroelectricity and it is markedly different from conventional ferroelectric switching mechanisms relying on ion displacement. Here, we present layer dependence as a new dimension to control sliding ferroelectricity. By fabricating 3R MoS2 of various thicknesses into dual-gate field-effect transistors, we obtain anomalous intermediate polarization states in multila…
Domain-Wall-Mediated Ultralow-Barrier Sliding and Pinning in Ferroelectric Moiré Superlattices Revealed by Machine Learning
National Center for Nanoscience and Technology, Chinese Academy of Sciences（中国科学院国家纳米科学中心）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；Songshan Lake Materials Laboratory（松山湖材料实验室）
Quadratic piezoelectricity from stacking-engineered interference in multilayer sliding ferroelectrics
Inner Mongolia University（内蒙古大学）；Nanjing University（南京大学）；Institute of Metal Research, Chinese Academy of Sciences（中国科学院金属研究所）；University of Science and Technology of China（中国科学技术大学）
The so-called interlayer-sliding ferroelectricity was recently proposed as an unconventional route to pursuit electric polarity in van der Waals multi-layers, which was already experimentally confirmed in WTe$_2$ bilayer even though it is metallic. Very recently, another van der Waals system, i.e., the ZrI$_2$ bilayer, was predicted to exhibit the interlayer-sliding ferroelectricity with both in-plane and out-of-plane polarizations [Phys. Rev. B \textbf{103}, 165420 (2021)]. Here the ZrI$_2$ bulk is studied, which owns two competitive phases ($α$ \textit{vs} $β$), both of which are derived fro…
The intertwined ferroelectricity and band topology will enable the non-volatile control of the topological states, which is of importance for nanoelectrics with low energy costing and high response speed. Nonetheless, the principle to design the novel system is unclear and the feasible approach to achieve the coexistence of two parameter orders is absent. Here, we propose a general paradigm to design 2D ferroelectric topological insulators by sliding topological multilayers on the basis of first-principles calculations. Taking trilayer Bi2Te3 as a model system, we show that in the van der Waal…
Superconducting cavity probes sliding ferroelectricity in small-angle twisted WSe$_2$
Tata Institute of Fundamental Research（塔塔基础研究所）；Université Grenoble Alpes, CNRS, Grenoble INP, Institut Néel（格勒诺布尔阿尔卑斯大学、法国国家科学研究中心、格勒诺布尔理工学院、内耳研究所）；Indian Institute of Science（印度科学学院）；National Institute for Materials Science（日本国立材料研究所）
The ability to switch between distinct states of polarization comprises the defining property of ferroelectrics. However, the microscopic mechanism responsible for switching is not well understood and theoretical estimates based on coherent monodomain switching typically overestimate experimentally determined coercive fields by orders of magnitude. In this work we present a detailed first principles characterization of domain walls (DWs) in two-dimensional ferroelectric GeS, GeSe, SnS and SnSe. In particular, we calculate the formation energies and migration barriers for 180 and 90 DWs, and th…
We present an extensive study of the electric, magnetic and elastic responses of tetragonal ferroelectrics under illumination, using a new theory intertwining material and wave symmetries. Optical rectification, photomagnetic, photovoltaic and phototoroidal vector responses are worked out as functions of the wave vector and wave polarization directions. Second-order response tensors associated with photoelastic, photomagnetoelectric, photorefractive effects and photoconductivity are described. We discuss in detail the photo-Hall and a new non-linear optical effect in tungsten bronzes. Finally,…
Low dimensional ferroelectrics are highly desired for applications and full of exotic physics. Here a functionalized MXene Hf$_2$CF$_2$ monolayer is theoretically studied, which manifests a nonpolar to polar transition upon moderate biaxial compressive strain. Accompanying this structural transition, a metal-semiconductor transition occurs. The in-plane shift of unilateral fluorine layer leads to a polarization pointing out-of-plane. Such ferroelectricity is unconventional, similar to the recently-proposed interlayer-sliding ferroelectricity but not identical. Due to its specific hexapetalous …
