Two-dimensional (2D) van der Waals ferroelectrics provide an unprecedented architectural freedom for the creation of artificial multiferroics and non-volatile electronic devices based on vertical and co-planar heterojunctions of 2D ferroic materials. Nevertheless, controlled microscopic manipulation of ferroelectric domains is still rare in monolayer-thick 2D ferroelectrics with in-plane polarization. Here we report the discovery of robust ferroelectricity with a critical temperature close to 400 K in SnSe monolayer plates grown on graphene, and the demonstration of controlled room temperature ferroelectric domain manipulation by applying appropriate bias voltage pulses to the tip of a scanning tunneling microscope (STM). This study shows that STM is a powerful tool for detecting and manipulating the microscopic domain structures in 2D ferroelectric monolayers, which is difficult for conventional approaches such as piezoresponse force microscopy, thus facilitating the hunt for other 2D ferroelectric monolayers with in-plane polarization with important technological applications.
NaCl-Assisted Growth of Ferroelectric SnSe Nanosheets with Spin Glass-like Behavior
Beijing Key Laboratory of Optoelectronic Functional Materials & Micro-nano Devices, School of Physics, Renmin University of China（中国人民大学物理学院光电功能材料与微纳器件北京市重点实验室）；Key Laboratory of Quantum State Construction and Manipulation (Ministry of Education), Renmin University of China（中国人民大学量子态构建与操控教育部重点实验室）
Materials with reduced dimensionality often exhibit exceptional properties that are different from their bulk counterparts. Here we report the emergence of a commensurate 2 $\times$ 2 charge density wave (CDW) in monolayer and bilayer SnSe$_2$ films by scanning tunneling microscope. The visualized spatial modulation of CDW phase becomes prominent near the Fermi level, which is pinned inside the semiconductor band gap of SnSe$_2$. We show that both CDW and Fermi level pinning are intimately correlated with band bending and virtual induced gap states at the semiconductor heterointerface. Through…
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…
The local atomic structure of SnSe was characterized across its orthorhmbic-to-orthorhombic structural phase transition using x-ray pair distribution function analysis. Substantial Sn off-centering distortions persist in the high symmetry high temperature phase, with symmetry different from that of ordered distortions below the transition. The analysis implies that the transition is neither order-disorder nor displacive, but rather a complex crossover where the character of coupling changes from 3D-like at low temperature to 2D-like at high temperature. Robust ferro-coupled SnSe intra-layer di…
Anharmonic Phonon Renormalization and Defect Tolerance of the Thermoelectric Power Factor in Monolayer SnSe
Faculty of Physics and Physics Engineering, University of Science（物理与物理工程学院，科学大学）；Viet Nam National University Ho Chi Minh City（越南国立大学胡志明市分校）；Advanced Materials Technology Institute Vietnam National University Ho Chi Minh City（先进材料技术研究所，越南国立大学胡志明市分校）；University of Health Sciences (UHS), Viet Nam National University Ho Chi Minh City（卫生科学学院（UHS），越南国立大学胡志明市分校）；Frontier Research Institute for Interdisciplinary Sciences, Tohoku University（前沿跨学科学研究院，东北大学）
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 …
Tuning exciton emission via ferroelectric polarization at a heterogeneous interface between a monolayer transition metal dichalcogenide and a perovskite oxide membrane
2D Ferroelectric materials are promising for designing low-dimensional memory devices. Here, we explore strain tunable ferroelectric properties of group-IV monochalcogenides MX (M=Ge, Sn; X=S, Se) and their potential application in lateral field tunnel junction devices. We find that these monolayers have in-plane ferroelectricity, with their ferroelectric parameters being on par with other known 2D ferroelectric materials. Amongst SnSe, SnS, GeSe, and GeS, we find that GeS has the best ferroelectric parameters for device applications, which can be improved further by applying uniaxial tensile …
Two-dimensional polarity is intriguing but remains in the early stage. Here a structural evolution diagram is established for GeS monolayer, which leads a noncollinear ferrielectric $δ$-phase energetically as stable as the ferroelectric $α$-phase. Its ferrielectricity is induced by the phonon frustration, i.e., the competition between ferroelectric and antiferroelectric modes, providing more routes to tune its polarity. Besides its prominent properties like large band gap, large polarization, and high Curie temperature, more interestingly, the morphotropic phase boundary between $α$- and $δ$-p…
Two-dimensional (2D) multiferroics have been casted great attention owing to their promising prospects for miniaturized electronic and memory devices.Here, we proposed a highly stable 2D multiferroic, VOF monolayer, which is an intrinsic ferromagnetic half semiconductor with large spin polarization ~2 $μ_{B}/V$ atom and a significant uniaxial magnetic anisotropy along a-axis (410 $μeV/V$ atom). Meanwhile, it shows excellent ferroelectricity with a large spontaneous polarization 32.7 $μC/cm^{2}$ and a moderate energy barrier (~43 meV/atom) between two ferroelectric states, which can be ascribed…
We demonstrate a 2D ferroelectric heterostructure with monolayer MoSe$_2$ and CuInP$_2$S$_6$ (CIPS). In the heterostructure, the electric polarization of CIPS results in c electronic modulation in monolayer MoSe$_2$.
We propose energy band engineering to enhance tunneling electroresistance (TER) in ferroelectric tunnel junctions (FTJs). We predict that an ultrathin dielectric layer with a smaller band gap, embedded into a ferroelectric barrier layer, acts as a switch controlling high and low conductance states of an FTJ depending on polarization orientation. Using first-principles modeling based on density functional theory, we investigate this phenomenon for a prototypical SrRuO3/BaTiO3/SrRuO3 FTJ with a BaSnO3 monolayer embedded in the BaTiO3 barrier. We show that in such a composite-barrier FTJ, ferroel…
Cornell University（康奈尔大学）；University of Nebraska, Lincoln（内布拉斯加大学林肯分校）；Leibniz-Institut für Kristallzüchtung（莱布尼茨晶体生长研究所）；Pacific Northwest National Laboratory（太平洋西北国家实验室）；The Pennsylvania State University（宾夕法尼亚州立大学）；University of California, Berkeley（加州大学伯克利分校）；Rice University（莱斯大学）；Kavli Institute at Cornell for Nanoscale Science（康奈尔卡弗里纳米科学研究所）；Princeton University（普林斯顿大学）
The bulk photovoltaic effect (BPVE) refers to the phenomenon of generating photocurrent or photovoltage in homogeneous noncentrosymmetric materials under illumination, and the intrinsic contribution to the BPVE is known as the shift current effect. We calculate the shift current conductivities of the ferroelectric SnTe monolayer using first-principles methods. We find that the monolayer SnTe has giant shift-current conductivity near the valley points. More remarkably, the linear optical absorption coefficient at this energy is very small, and therefore leads to an enormous Glass coefficient th…
Phase Switchable Photocatalytic Water Splitting via a Paraelectric-Ferroelectric Transition in Zr2Ge2S6 Monolayer: A Comprehensive Theoretical Insights
