Ferroelectric-tunable quantum nonlinearity of chiral Bloch electrons in a moiré system
Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所，北京凝聚态物理国家研究中心）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；Research Center for Functional Materials, National Institute for Materials Science（国立材料研究所功能材料研究中心）；International Center for Materials Nanoarchitectonics, National Institute for Materials Science（国立材料研究所国际纳米结构材料中心）
Sliding ferroelectricity in van der Waals materials shows great potential for designing robust memory devices. However, its thermodynamic behaviors and the coupling with certain quantum effects remain largely unexplored. Here, we demonstrate ferroelectric control over quantum nonlinear transport in a hexagonal boron nitride (hBN) encapsulated twisted double-bilayer graphene moiré heterostructure. The ferroelectricity is attributed to the presence of rhombohedral stacking in the top hBN, confirmed by both electrical transport and optical second harmonic generation (SHG) measurements. Remarkably, the polarization magnitude remains temperature-independent across 1.7-200 K, while nucleation time exhibits thermally activated behavior, decreasing with increasing temperature. Furthermore, we demonstrate a ferroelectric-switchable nonlinear Hall effect, attributed to the chiral scattering induced by Berry curvature, with outstanding fatigue-resistant and nonvolatility, demonstrating direct coupling between sliding ferroelectricity and quantum geometric properties. Our results establish sliding ferroelectrics as a platform for exploring electrically programmable Berry curvature physics.
Moiré materials, with superlattice periodicity many times the atomic length scale, have enabled the studies of strong electronic correlations and band topology with unprecedented tunability. However, nonvolatile control of the moiré potentials, which could allow on-demand switching of the superlattice effects, has not been achieved to date. Here we demonstrate the switching of the correlated and moiré band insulating states and the associated nonlinear anomalous Hall effect by the ferroelectric effect. This is achieved in a ferroelectric WTe2 bilayer of the Td structure with a centered-rectang…
Moiré exciton features tunable Dirac dispersion and spatially dependent optical selection rules. With the long lifetime due to its interlayer nature, it is promising to realize a Bose-Einstein condensation of moiré excitons. Here we study the properties of moiré exciton condensate within the mean-field theory, with special focus on exciton-exciton interaction effect on the nonlinear Bloch band and Bloch waves of exciton condensate in moiré potential. We find the nonlinear dispersion of the moiré exciton condensate exhibits complex loop structure induced by exciton-exciton interaction. A nonlin…
It is well known that stacking domains form in moiré superlattices due to the competition between the interlayer van der Waals forces and intralayer elastic forces, which can be recognized as polar domains due to the local spontaneous polarization in bilayers without centrosymmetry. We propose a theoretical model which captures the effect of an applied electric field on the domain structure. The coupling between the spontaneous polarization and field leads to uneven relaxation of the domains, and a net polarization in the superlattice at nonzero fields, which is sensitive to the moiré period. …
Achieving Bloch oscillations of free carriers under a direct current, a long-sought-after collective many-body behavior, has been challenging due to stringent constraints on the band properties. We argue that the flat bands in moiré graphene fulfill the basic requirements for observing Bloch oscillations, offering an appealing alternative to the stacked quantum wells used in previous work aiming to access this regime. Bloch-oscillating moiré superlattices emit a comb-like spectrum of incommensurate frequencies, a property of interest for converting direct currents into high-frequency currents …
The discovery of unconventional ferroelectric behavior in twisted bilayers has prompted the consideration of moiré heterostructures as polar materials. However, misconceptions about the nature and origin of the observed ferroelectricity indicate that a better theoretical understanding of the polar properties of moiré heterostructures is needed. In this paper, it is proposed, and verified with first-principles calculations, that all moiré heterostructures exhibit an out-of-plane moiré polar domain (MPD) structure. In transition metal dichalcogenide bilayers, an interlayer charge transfer occurs…
The relative orientation (twist) of successive layers of stacked two-dimensional (2D) materials creates variations in the interlayer atomic registry. The variations often form a super lattice, called a moiré pattern, which can alter electronic properties. In this work we introduce a classification of the single-particle electronic structures that can occur in twisted stacks of 2D layers by characterizing them as "moiré molecules" or "moiré crystals". The molecules generate localized electronic states and moiré flat bands, while the crystals are sometimes unconventional and produce electronic b…
Twistronic van der Waals heterostrutures offer exciting opportunities for engineering optoelectronic properties of nanomaterials. Here, we use multiscale modeling to study trapping of charge carriers and excitons by ferroelectric polarisation and piezoelectric charges by domain structures in twistronic WX$_2$/MoX$_2$ bilayers (X=S,Se). For almost aligned 2H-type bilayers, we find that holes and electrons are trapped in the opposite -- WMo and XX (tungsten over molybdenum {\it versus} overlaying chalcogens) -- corners of the honeycomb domain wall network, swapping their position at a twist angl…
Ferroelectric hysteresis in singly aligned graphene-hBN moiré superlattices
CIC nanoGUNE（纳米科技联合研究中心）；University of the Basque Country (UPV/EHU)（巴斯克大学）；National Institute for Materials Science（物质材料研究机构）；Centro de Física de Materiales (CFM-MPC) Centro Mixto CSIC-UPV/EHU（物质物理中心（CFM-MPC）CSIC-巴斯克大学联合中心）
Theoretical investigation demonstrates that the composite bilayer (i.e., chiral-magnetic/ferroelectric bilayer) offers the possibility of electric-induced magnetic Skyrmions [Phys. Rev. B \textbf{94}, 014311 (2016)]. In this Article, we propose a micromagnetic model to physically manipulate magnetic Bloch Skyrmions propagating in a chiral-magnetic thin film with a polarized ferroelectric essential to drive the system through the converse magnetoelectric effect. Effects caused by different velocities of the propagation, sizes of the thin film, and strength of the magnetoelectric couplings stron…
Lattice reconstruction in twisted transition-metal dichalcogenide (TMD) bilayers gives rise to piezo- and ferroelectric moiré potentials for electrons and holes, as well as a modulation of the hybridisation across the bilayer. Here, we develop hybrid $\mathbf{k}\cdot \mathbf{p}$ tight-binding models to describe electrons and holes in the relevant valleys of twisted TMD homobilayers with parallel (P) and anti-parallel (AP) orientations of the monolayer unit cells. We apply these models to describe moiré superlattice effects in twisted WSe${}_2$ bilayers, in conjunction with microscopic \emph{ab…
Several moiré systems created by various twisted bilayers have manifested magnetism under flatband conditions leading to enhanced interaction effects. We theoretically study stability of moiré flatband ferromagnetism against collective excitations, with a focus on the effects of Bloch band quantum geometry. The spin magnon spectrum is calculated using different approaches, including Bethe-Salpeter equation, single mode approximation, and an analytical theory. One of our main results is an analytical expression for the spin stiffness in terms of the Coulomb interaction potential, the Berry curv…
The second-order nonlinear Hall effect illuminates a frequency-doubling transverse current emerging in quantum materials with broken inversion symmetry even when time-reversal symmetry is preserved. This nonlinear response originates from both the Berry curvature dipole and the chiral Bloch electron skew scatterings, reflecting various information of the lattice symmetries, band dispersions, and topology of the electron wavefunctions. Even though many efforts have been put in detecting the nonlinear Hall effect in diverse condensed matter systems, effective manipulation of the two principal me…
Spontaneous order of layer pseudospins in two-dimensional bilayers is common in quantum Hall systems, where it is responsible for hysteretic responses to gate fields in states with Ising order, and giant drag voltages in states with XY (spontaneous inter-layer phase coherence) order. In this article we predict that layer pseudospin order will also occur in double-moiré strongly correlated two-dimensional electron systems. We comment on similarities and differences in the competition between the two types of order in quantum Hall and double-moiré systems, and relate our findings to previous wor…
The 212 species of structural phase transitions which break macroscopic symmetry are analyzed with respect to the occurrence of time-reversal invariant vector and bidirector order parameters. The possibility of discerning the orientational domain states of the low-symmetry phase by these `vectorlike' physical properties has been derived using a computer algorithm exploiting the concept of polar, axial, chiral and neutral dipoles. It is argued that for species 32 > 3, 422 > 4 and 622 > 6, Bogdanov-Yablonskii phenomenological theory for a ferromagnetic Bloch Skyrmions applies also to the ferroel…
Moiré enabled spin pumping and preservation in MoSe2/WS2 heterobilayers
Stanford University（斯坦福大学）；SLAC National Accelerator Laboratory（SLAC国家加速器实验室）；National Institute for Materials Science（国立材料研究所）；University of Cambridge（剑桥大学）
2D ferroelectrics with robust polarization down to atomic thicknesses provide novel building blocks for functional heterostructures. Experimental reports, however, remain scarce because of the requirement of a layered polar crystal. Here, we demonstrate a rational design approach to engineering 2D ferroelectrics from a non-ferroelectric parent compound via employing van der Waals assembly. Parallel-stacked bilayer boron nitride is shown to exhibit out-of-plane electric polarization that reverses depending on the stacking order. The polarization switching is probed via the resistance of an adja…
Moiré structures in small-angle-twisted bilayers of two-dimensional semiconductors with a broken-symmetry interface form arrays of ferroelectric domains with periodically alternating out-of-plane polarization. Here, we propose a network theory for the tunability of such FE domain structure by applying an electric field perpendicular to the 2D crystal. Using multiscale analysis, we derive a fully parametrized string-theory-like description of the domain wall network and show that it undergoes a qualitative change, after the arcs of partial dislocation like domain walls merge (near the network n…
Van der Waals (vdW) materials have greatly expanded our design space of heterostructures by allowing individual layers to be stacked at non-equilibrium configurations, for example via control of the twist angle. Such heterostructures not only combine characteristics of the individual building blocks, but can also exhibit emergent physical properties absent in the parent compounds through interlayer interactions. Here we report on a new family of emergent, nanometer-thick, semiconductor 2D ferroelectrics, where the individual constituents are well-studied non-ferroelectric monolayer transition …
Electrons moving through a spatially periodic lattice potential develop a quantized energy spectrum consisting of discrete Bloch bands. In two dimensions, electrons moving through a magnetic field also develop a quantized energy spectrum, consisting of highly degenerate Landau energy levels. In 1976 Douglas Hofstadter theoretically considered the intersection of these two problems and discovered that 2D electrons subjected to both a magnetic field and a periodic electrostatic potential exhibit a self-similar recursive energy spectrum. Known as Hofstadter's butterfly, this complex spectrum resu…
Nonlinear Hall quantum oscillations to probe topological Brown-Zak fermions in graphene moiré systems
Key Laboratory of Advanced Optoelectronic Quantum Architecture and Measurement (MOE), School of Physics, Beijing Institute of Technology（北京理工大学物理学院先进光电子量子结构与测量教育部重点实验室）；School of Physics and Electronics, Hunan University（湖南大学物理与电子信息学院）；School of Physical Sciences and CAS Center for Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences（中国科学院大学物理科学学院及中国科学院拓扑量子计算卓越创新中心）；International Center for Quantum Materials, Beijing Institute of Technology, Zhuhai（北京理工大学珠海国际量子材料中心）
The electronic bands of twisted bilayer graphene (TBLG) with a large-period moiré superlattice fracture to form narrow Bloch minibands that are spectrally isolated by forbidden energy gaps from remote dispersive bands. When these gaps are sufficiently large, one can study a band-projected Hamiltonian that correctly represents the dynamics within the minibands. This inevitably introduces nontrivial geometrical constraints that arise from the assumed form of the projection. Here we show that this choice has a profound consequence in a low-energy experimentally-observable signature which therefor…
High-field Josephson effect enabled by a moiré Hofstadter spectrum
Ludwig-Maximilians-Universität（路德维希-马克西米利安大学）；Munich Center for Quantum Science and Technology (MCQST)（慕尼黑量子科学与技术中心）；Nanomaterials and Nanotechnology Research Center (CINN-CSIC), Universidad de Oviedo (UO)（阿斯图里亚斯大学纳米材料与纳米技术研究中心（CINN-CSIC））；Yale University（耶鲁大学）；Aalto University（阿尔托大学）；National Institute for Materials Science（国立材料研究所）
The mechanism of charge carrier interaction in twisted bilayer graphene (TBG) remains an unresolved problem, where some researchers proposed the dominance of the electron-phonon interaction, while the others showed evidence for electron-electron or electron-magnon interactions. Here we propose to resolve this problem by generalizing the Bloch-Grüneisen equation and using it for the analysis of the temperature dependent resistivity in TBG. It is a well-established theoretical result that the Bloch-Grüneisen equation power-law exponent, n, exhibits exact integer values for certain mechanisms. Fo…
Quantum geometry is a key quantity that distinguishes electrons in a crystal from those in the vacuum. Its study continues to provide insights into quantum materials, uncovering new design principles for their discovery. However, unlike the Berry curvature, an intuitive understanding of the quantum metric is lacking. Here, we show that the quantum metric of Bloch electrons leads to a momentum-space gravity. In particular, by extending the semiclassical formulation of electron dynamics to second order, we find that the resulting velocity is modified by a geodesic term and becomes the momentum-s…
