Jinghao Deng#, Deping Guo#, Yao Wen, Shuangzan Lu, Zhengbo Cheng, Zemin Pan, Tao Jian, Yusong Bai, Hui Zhang, Wei Ji*, Jun He*, Chendong Zhang*
Abstract:
Multiferroicity allows magnetism to be controlled using electric fields or vice versa, which has gained tremendous interest in both fundamental research and device applications. A reduced dimensionality of multiferroic materials is highly desired for device miniaturization, but the coexistence of ferroelectricity and magnetism at the two-dimensional limit is still debated. Here, we used a NbSe2 substrate to break both the C3 rotational and inversion symmetries in monolayer VCl3 and thus introduced exceptional in-plane ferroelectricity into a two dimensional magnet. Scanning tunnelling spectroscopy directly visualized ferroelectric domains and manipulated their domain boundaries in monolayer VCl3, where coexisting antiferromagnetic order with canted magnetic moments was verified by vibrating sample magnetometer measurements. Our density functional theory calculations highlight the crucial role that highly directional interfacial Cl–Se interactions play in breaking the symmetries and thus in introducing in-plane ferroelectricity, which was further verified by examining an ML-VCl3/graphene sample. Our work demonstrates an approach to manipulate the ferroelectric states in monolayered magnets through van der Waals interfacial interactions.
Fig. 1. Morphology and atomic structure of ML-VCl3 on a NbSe2 substrate.
Fig. 2. IP electric polarizations characterized by band bending near DWs.
Fig. 3. Experimental and theoretical investigations of the magnetic order in epitaxy ML-VCl3.
Fig. 4. Anisotropic charge transfer–induced IP ferroelectricity and comparison with the VCl3-graphene interface.
Miniaturizing van der Waals (vdW) ferroelectric materials to atomic scales is essential for modern devices like nonvolatile memory and sensors. To unlock their full potential, their growth mechanisms, interface effects, and stabilization are preferably investigated, particularly for ultrathin 2D nanosheets with single-unit cell thickness. This study focuses on Bi2TeO5 (BTO) and utilizes precise control over growth kinetics at the nucleation temperature to create specific interfacial reconfiguration layers. Ultrathin BTO nanosheets with planar ferroelectricity at a single-unit cell thickness are successfully grown. Atomic-scale characterization reveals a disordered distribution of elements in the interfacial layer, which buffers strain from lattice mismatch. The theoretical calculations support these observations. Furthermore, this strategy also can be extended to the growth of a variety of 2D ternary oxide nanosheets. This work contributes to a better understanding of growth and stability mechanisms in 2D ultrathin nanosheets.
The structure and dynamics of ferroelectric domain walls are essential for polarization switching in ferroelectrics, which remains relatively unexplored in two-dimensional ferroelectric α-In2Se3. Interlayer interactions engineering via selecting the stacking order in two-dimensional materials allows modulation of ferroelectric properties. Here, we report stacking-dependent ferroelectric domain walls in 2H and 3R stacked α-In2Se3, elucidating the resistance switching mechanism in ferroelectric semiconductor-metal junction devices. In 3R α-In2Se3, the in-plane movement of out-of-plane ferroelectric domain walls yield a large hysteresis window. Conversely, 2H α-In2Se3 devices favor in-plane domain walls and out-of-plane domain wall motion, producing a small hysteresis window. High electric fields induce a ferro-paraelectric phase transition of In2Se3, where 3R In2Se3 reaches the transition through intralayer atomic gliding, while 2H In2Se3 undergoes a complex process comprising intralayer bond dissociation and interlayer bond reconstruction. Our findings demonstrate tunable ferroelectric properties via stacking configurations, offering an expanded dimension for material engineering in ferroelectric devices.
Yangliu Wu, Zhaozhuo Zeng, Haipeng Lu, Xiaocang Han, Chendi Yang, Nanshu Liu, Xiaoxu Zhao, Liang Qiao, Wei Ji*, Renchao Che, Longjiang Deng*, Peng Yan* and Bo Peng*
Abstract:
Multiferroic materials have been intensively pursued to achieve the mutual control of electric and magnetic properties. The breakthrough progress in 2D magnets and ferroelectrics encourages the exploration of low-dimensional multiferroics, which holds the promise of understanding inscrutable magnetoelectric coupling and inventing advanced spintronic devices. However, confirming ferroelectricity with optical techniques is challenging in 2D materials, particularly in conjunction with antiferromagnetic orders in single- and few-layer multiferroics. Here, we report the discovery of 2D vdW multiferroic with out-of plane ferroelectric polarization in trilayer NiI2 device, as revealed by scanning reflective magnetic circular dichroism microscopy and ferroelectric hysteresis loops. The evolution between ferroelectric and antiferroelectric phases has been unambiguously observed. Moreover, the magnetoelectric interaction is directly probed by magnetic control of the multiferroic domain switching. This work opens up opportunities for exploring new multiferroic orders and multiferroic physics at the limit of single or few atomic layers, and for creating advanced magnetoelectronic devices.
Deping Guo (郭的坪)#, Cong Wang (王聪)#, Lvjin Wang (王侣锦), Yunhao Lu (陆赟豪), Hua Wu (吴骅), Yanning Zhang (张妍宁), and Wei Ji (季威)*
Abstract:
Two-dimensional (2D) van der Waals magnetic materials have promising and versatile electronic and magnetic properties in the 2D limit, indicating a considerable potential to advance spintronic applications. Theoretical predictions thus far have not ascertained whether monolayer VCl3 is a ferromagnetic (FM) or anti-FM monolayer; this also remains to be experimentally verified. We theoretically investigate the influence of potential factors, including 𝐶3 symmetry breaking, orbital ordering, epitaxial strain, and charge doping, on the magnetic ground state. Utilizing first-principles calculations, we predict a collinear type-III FM ground state in monolayer VCl3 with a broken 𝐶3 symmetry, wherein only the former two of three 𝑡2g orbitals (𝑎1g, 𝑒 𝜋 g2 and 𝑒 𝜋 g1) are occupied. The atomic layer thickness and bond angles of monolayer VCl3 undergo abrupt changes driven by an orbital ordering switch, resulting in concomitant structural and magnetic phase transitions. Introducing doping to the underlying Cl atoms of monolayer VCl3 without 𝐶3 symmetry simultaneously induces in- and out-of-plane polarizations. This can achieve a multiferroic phase transition if combined with the discovered adjustments of magnetic ground state and polarization magnitude under strain. The establishment of an orbital-ordering driven regulatory mechanism can facilitate deeper exploration and comprehension of magnetic properties of strongly correlated systems in monolayer VCl3.