Temperature-Driven Rotation Symmetry-Breaking States in an Atomic Kagome Metal KV3Sb5.

Kagome lattice AV3Sb5 has attracted tremendous interest because it hosts correlated and topological physics. However, an in-depth understanding of the temperature-driven electronic states in AV3Sb5 is elusive. Here we use scanning tunneling microscopy to directly capture the rotational symmetry-breaking effect in KV3Sb5. Through both topography and spectroscopic imaging of defect-free KV3Sb5, we observe a charge density wave (CDW) phase transition from an a0 × a0 atomic lattice to a robust 2a0 × 2a0 superlattice upon cooling the sample to 60 K. An individual Sb-atom vacancy in KV3Sb5 further gives rise to the local Friedel oscillation (FO), visible as periodic charge modulations in spectroscopic maps. The rotational symmetry of the FO tends to break at the temperature lower than 40 K. Moreover, the FO intensity shows an obvious competition against the intensity of the CDW. Our results reveal a tantalizing electronic nematicity in KV3Sb5, highlighting the multiorbital correlation in the kagome lattice framework.

Nonvolatile Multistate Manipulation of Topological Magnetism in Monolayer CrI3 through Quadruple-Well Ferroelectric Materials.

Nonvolatile multistate manipulation of two-dimensional (2D) magnetic materials holds promise for low dissipation, highly integrated, and versatile spintronic devices. Here, utilizing density functional theory calculations and Monte Carlo simulations, we report the realization of nonvolatile and multistate control of topological magnetism in monolayer CrI3 by constructing multiferroic heterojunctions with quadruple-well ferroelectric (FE) materials. The Pt2Sn2Te6/CrI3 heterojunction exhibits multiple magnetic phases upon modulating FE polarization states of FE layers and interlayer sliding. These magnetic phases include Bloch-type skyrmions and ferromagnetism, as well as a newly discovered topological magnetic structure. We reveal that the Dzyaloshinskii-Moriya interaction (DMI) induced by interfacial coupling plays a crucial role in magnetic skyrmion manipulation, which aligns with the Fert-Levy mechanism. Moreover, a regular magnetic skyrmion lattice survives when removing a magnetic field, demonstrating its robustness. The work sheds light on an effective approach to nonvolatile and multistate control of 2D magnetic materials.

Orbital distortion and electric field control of sliding ferroelectricity in a boron nitride bilayer.

Recent experiments confirm that two-dimensional boron nitride (BN) films possess room-temperature out-of-plane ferroelectricity when each BN layer is sliding with respect to each other. This ferroelectricity is attributed to the interlayered orbital hybridization or interlayer charge transfer in previous work. In this work, we attempt to understand the sliding ferroelectricity from the perspective of orbital distortion of long-pair electrons. Using the maximally localized Wannier function method and first-principles calculations, the out-of-planepzorbitals of BN are investigated. Our results indicate that the interlayer van der Waals interaction causes the distortion of the Npzorbitals. Based on the picture of out-of-plane orbital distortion, we propose a possible mechanism to tune the ferroelectric polarization by external fields, including electric field and stress field. It is found that both the polarization intensity and direction can be modulated under the electric field. The polarization intensity of the system can also be controlled by stress field perpendicular to the plane. This study will provide theoretical help in the device design based on sliding ferroelectrics.

Tunable Topological States in Stacked Chern Insulator Bilayers.

The emergence of intrinsic quantum anomalous Hall (QAH) insulators with a long-range ferromagnetic (FM) order triggers unprecedented prosperity for combining topology and magnetism in low dimensions. Built upon atom-thin Chern insulator monolayer MnBr3, we propose that the topologically nontrivial electronic states can be systematically tuned by inherent magnetic orders and external electric/optical fields in stacked Chern insulator bilayers. The FM bilayer illustrates a high-Chern-number QAH state characterized by both quantized Hall plateaus and specific magneto-optical Kerr angles. In antiferromagnetic bilayers, Berry curvature singularity induced by electrostatic fields or lasers emerges, which further leads to a novel implementation of the layer Hall effect depending on the chirality of irradiated circularly polarized light. These results demonstrate that abundant tunable topological properties can be achieved in stacked Chern insulator bilayers, thereby suggesting a universal routine to modulate d-orbital-dominated topological Dirac fermions.

Unveiling Electronic Behaviors in Heterochiral Charge-Density-Wave Twisted Stacking Materials with 1.25 nm Unit Dependence.

Layered charge-density-wave (CDW) materials have gained increasing interest due to their CDW stacking-dependent electronic properties for practical applications. Among the large family of CDW materials, those with star of David (SOD) patterns are very important due to the potentials for quantum spin liquid and related device applications. However, the spatial extension and the spin coupling information down to the nanoscale remain elusive. Here, we report the study of heterochiral CDW stackings in bilayer (BL) NbSe2 with high spatial resolution. We reveal that there exist well-defined heterochiral stackings, which have inhomogeneous electronic states among neighboring CDW units (star of David, SOD), significantly different from the homogeneous electronic states in the homochiral stackings. Intriguingly, the different electronic behaviors are spatially localized within each SOD with a unit size of 1.25 nm, and the gap sizes are determined by the different types of SOD stackings. Density functional theory (DFT) calculations match the experimental measurements well and reveal the SOD-stacking-dependent correlated electronic states and antiferromagnetic/ferromagnetic couplings. Our findings give a deep understanding of the spatial distribution of interlayer stacking and the delicate modulation of the spintronic states, which is very helpful for CDW-based nanoelectronic devices.

Rational Design of Heteroanionic Two-Dimensional Materials with Emerging Topological, Magnetic, and Dielectric Properties.

Designing and tuning the physical properties of two-dimensional (2D) materials at the atomic level are crucial to the development of 2D technologies. Here, we introduce heteroanions into metal-centered octahedral structural units of a 2D crystal breaking the Oh symmetry, together with the synergistic effect of anions' electrons and electronegativity, to realize ternary 2D materials with emerging topological, magnetic, and dielectric properties. Using an intrinsic heteroanionic van der Waals layered material, VOCl, as a prototype, 20 2D monolayers VXY (X = B, C, N, O, or F; Y = F, Cl, Br, or I) are obtained and investigated by means of first-principles calculations. The anion engineering in this family significantly reshapes the electronic properties of VOCl, leading to nonmagnetic topological insulators with nontrivial edge states in VCY, ferromagnetic half-semimetals with a nodal ring around the Fermi energy in VNY, and insulators with dielectric constants in VOY higher than that of h-BN. This work demonstrates the rationality and validity of the design strategy of multiple-anion engineering to achieve superior properties in the 2D monolayers with potential application in electronics and spintronics.

Manipulating Weyl quasiparticles by orbital-selective photoexcitation in WTe2.

Optical control of structural and electronic properties of Weyl semimetals allows development of switchable and dissipationless topological devices at the ultrafast scale. An unexpected orbital-selective photoexcitation in type-II Weyl material WTe2 is reported under linearly polarized light (LPL), inducing striking transitions among several topologically-distinct phases mediated by effective electron-phonon couplings. The symmetry features of atomic orbitals comprising the Weyl bands result in asymmetric electronic transitions near the Weyl points, and in turn a switchable interlayer shear motion with respect to linear light polarization, when a near-infrared laser pulse is applied. Consequently, not only annihilation of Weyl quasiparticle pairs, but also increasing separation of Weyl points can be achieved, complementing existing experimental observations. In this work, we provide a new perspective on manipulating the Weyl node singularity and coherent control of electron and lattice quantum dynamics simultaneously.

Type-II Interface Band Alignment in the vdW PbI2-MoSe2 Heterostructure.

Energy band alignments at heterostructure interfaces play key roles in device performance, especially between two-dimensional atomically thin materials. Herein, van der Waals PbI2-MoSe2 heterostructures fabricated by in situ PbI2 deposition on monolayer MoSe2 are comprehensively studied using scanning tunneling microscopy/spectroscopy, atomic force microscopy, photoemission spectroscopy, and Raman and photoluminescence (PL) spectroscopy. PbI2 grows on MoSe2 in a quasi layer-by-layer epitaxial mode. A type-II interface band alignment is proposed between PbI2 and MoSe2 with the conduction band minimum (valence band maximum) located at PbI2 (MoSe2), which is confirmed by first-principles calculations and the existence of interfacial excitons revealed using temperature-dependent PL. Our findings provide a scalable method to fabricate PbI2-MoSe2 heterostructures and new insights into the electronic structures for future device design.

Orbital design of topological insulators from two-dimensional semiconductors.

Two-dimensional (2D) materials have attracted much attention because they exhibit various intrinsic properties, which are, however, usually not interchangeable. Here we propose a generic approach to convert 2D semiconductors to 2D topological insulators (TIs) via atomic adsorption. The approach is underlined by an orbital design principle that involves introducing an extrinsic s-orbital state of the adsorbate into the intrinsic sp-bands of a 2D semiconductor, so as to induce s-p band inversion for a TI phase, as demonstrated by tight-binding model analyses. Based on first-principles calculations, we successfully apply this approach to convert CuS, CuSe and CuTe into TIs by adsorbing one adatom per unit cell of Na, Na0.5K0.5 and K as well as Rb and Cs. Moreover, if the chalcogens in the 2D semiconductor have a decreasing ability of accepting electrons, the adsorbates should have an increasing ability of donating electrons. Our findings open a new door to discovering TIs by predictive material design beyond finding preexisting TIs.

Evidence of Topological Edge States in Buckled Antimonene Monolayers.

Two-dimensional topological materials have attracted intense research efforts owing to their promise in applications for low-energy, high-efficiency quantum computations. Group-VA elemental thin films with strong spin-orbit coupling have been predicted to host topologically nontrivial states as excellent two-dimensional topological materials. Herein, we experimentally demonstrated for the first time that the epitaxially grown high-quality antimonene monolayer islands with buckled configurations exhibit significantly robust one-dimensional topological edge states above the Fermi level. We further demonstrated that these topologically nontrivial edge states arise from a single p-orbital manifold as a general consequence of atomic spin-orbit coupling. Thus, our findings establish monolayer antimonene as a new class of topological monolayer materials hosting the topological edge states for future low-power electronic nanodevices and quantum computations.

Spin-Orientation-Dependent Topological States in Two-Dimensional Antiferromagnetic NiTl2S4 Monolayers.

The topological states of matter arising from the nontrivial magnetic configuration provide a better understanding of physical properties and functionalities of solid materials. Such studies benefit from the active control of spin orientation in any solid, which is known to take place rarely in the two-dimensional (2D) limit. Here we demonstrate by the first-principles calculations that spin-orientation-dependent topological states can appear in the geometrically frustrated monolayer antiferromagnet (AFM). Different topological states including the quantum anomalous Hall (QAH) effect and time-reversal-symmetry (TRS) broken quantum spin Hall (QSH) effect can be obtained by changing the spin orientation in the NiTl2S4 monolayer. Remarkably, the dilated nc-AFM NiTl2S4 monolayer gives birth to the QAH effect with the hitherto reported largest number of quantized conducting channels (Chern number [Formula: see text] = -4) in 2D materials. Interestingly, under tunable chemical potential, the nc-AFM NiTl2S4 monolayer hosts a novel state supporting the coexistence of QAH and TRS broken QSH effects with a Chern number of [Formula: see text] = 3 and a spin Chern number of [Formula: see text] = 1. This work manifests a promising concept and material realization of topological spintronics in 2D antiferromagnets by manipulating their spin degree of freedom.

Screening Magnetic Two-Dimensional Atomic Crystals with Nontrivial Electronic Topology.

To date, only a few two-dimensional (2D) magnetic crystals have been experimentally confirmed, such as CrI3 and CrGeTe3, all with very low Curie temperatures ( TC). High-throughput first-principles screening over a large set of materials yields 89 magnetic monolayers including 56 ferromagnetic (FM) and 33 antiferromagnetic compounds. Among them, 24 FM monolayers are promising candidates possessing TC higher than that of CrI3. High TC monolayers with fascinating electronic phases are identified: (i) quantum anomalous Hall and valley Hall effects coexist in a single material RuCl3 or VCl3, leading to a valley-polarized quantum anomalous Hall state; (ii) TiBr3, Co2NiO6, and V2H3O5 are revealed to be half-metals. More importantly, a new type of fermion dubbed type-II Weyl ring is discovered in ScCl. Our work provides a database of 2D magnetic materials, which could guide experimental realization of high-temperature magnetic monolayers with exotic electronic states for future spintronics and quantum computing applications.

Photoinduced Nonequilibrium Topological States in Strained Black Phosphorus.

Black phosphorus (BP), an elemental semiconductor, has attracted tremendous interest because it exhibits a wealth of interesting electronic and optoelectronic properties in equilibrium condition. The nonequilibrium electronic structures of bulk BP under a periodic field of laser remain unexplored, but can lead to intriguing topological optoelectronic properties. Here we show that, under the irradiation of circularly polarized light (CPL), BP exhibits a photon-dressed Floquet-Dirac semimetal state, which can be continuously tuned by changing the direction, intensity, and frequency of the incident laser. The topological phase transition from type-I to type-II Floquet-Dirac fermions manifests a new form of type-III phase, which exists in a wide range of intensities and frequencies of the incident laser. Furthermore, topological surface states exhibit nonequilibrium electron transport in a direction locked by the helicity of CPL. Our findings not only deepen our understanding of fundamental properties of BP in relation to topology but also extend optoelectronic device applications of BP to the nonequilibrium regime.

Epitaxial Growth of Honeycomb Monolayer CuSe with Dirac Nodal Line Fermions.

2D transition metal chalcogenides have attracted tremendous attention due to their novel properties and potential applications. Although 2D transition metal dichalcogenides are easily fabricated due to their layer-stacked bulk phase, 2D transition metal monochalcogenides are difficult to obtain. Recently, a single atomic layer transition metal monochalcogenide (CuSe) with an intrinsic pattern of nanoscale triangular holes is fabricated on Cu(111). The first-principles calculations show that free-standing monolayer CuSe with holes is not stable, while hole-free CuSe is endowed with the Dirac nodal line fermion (DNLF), protected by mirror reflection symmetry. This very rare DNLF state is evidenced by topologically nontrivial edge states situated inside the spin-orbit coupling gaps. Motivated by the promising properties of hole-free honeycomb CuSe, monolayer CuSe is fabricated on Cu(111) surfaces by molecular beam epitaxy and confirmed success with high resolution scanning tunneling microscopy. The good agreement of angle resolved photoemission spectra with the calculated band structures of CuSe/Cu(111) demonstrates that the sample is monolayer CuSe with a honeycomb lattice. These results suggest that the honeycomb monolayer transition metal monochalcogenide can be a new platform to study 2D DNLFs.

Epitaxial Growth of Flat Antimonene Monolayer: A New Honeycomb Analogue of Graphene.

Group-V elemental monolayers were recently predicted to exhibit exotic physical properties such as nontrivial topological properties, or a quantum anomalous Hall effect, which would make them very suitable for applications in next-generation electronic devices. The free-standing group-V monolayer materials usually have a buckled honeycomb form, in contrast with the flat graphene monolayer. Here, we report epitaxial growth of atomically thin flat honeycomb monolayer of group-V element antimony on a Ag(111) substrate. Combined study of experiments and theoretical calculations verify the formation of a uniform and single-crystalline antimonene monolayer without atomic wrinkles, as a new honeycomb analogue of graphene monolayer. Directional bonding between adjacent Sb atoms and weak antimonene-substrate interaction are confirmed. The realization and investigation of flat antimonene honeycombs extends the scope of two-dimensional atomically-thick structures and provides a promising way to tune topological properties for future technological applications.

Hidden spin polarization in the 1T-phase layered transition-metal dichalcogenides MX2 (M = Zr, Hf; X = S, Se, Te).

The recent discovery of hidden spin polarization emerging in layered materials of specific nonmagnetic crystal is a fascinating phenomenon, though hardly explored yet. Here, we have studied hidden spin textures in layered nonmagnetic 1T-phase transition-metal dichalcogenides MX2 (M = Zr, Hf; X = S, Se, Te) by using first-principles calculations. Spin-layer locking effect, namely, energy-degenerate opposite spins spatially separated in the top and bottom layer respectively, has been identified. In particular, the hidden spin polarization of ß-band can be easily probed, which is strongly affected by the strength of spin-orbit coupling. The hidden spin polarization of ξ-band locating at high symmetry M point (conduction band minimum) has a strong anisotropy. In the bilayer, the hidden spin polarization is preserved at the upmost Se layer, while being suppressed if the ZrSe2 layer is taken as the symmetry partner. Our results on hidden spin polarization in 1T-phase dichalcogenides, verifiable by spin-resolved and angle-resolved photoemission spectroscopy (ARPES), enrich our understanding of spin physics and provide important clues to search for specific spin polarization in two dimensional materials for spintronic and quantum information applications.

Intrinsic valley polarization of magnetic VSe2 monolayers.

Intrinsic valley polarization can be obtained in VSe2 monolayers with broken inversion symmetry and time reversal symmetry. First-principles investigations reveal that the magnitude of the valley splitting in magnetic VSe2 induced by spin-orbit coupling reaches as high as 78.2 meV and can be linearly tuned by biaxial strain. Besides conventional polarized light, hole doping or illumination with light of proper frequency can offer effective routes to realize valley polarization. Moreover, spin-orbit coupling in monolayer VSe2 breaks not only the valley degeneracy but also the three-fold rotational symmetry in band structure. The intrinsic and tunable valley splitting and the breaking of optical isotropy bring additional benefits to valleytronic and optoelectronic applications.

All-Silicon Switchable Magnetoelectric Effect through Interlayer Exchange Coupling.

The magnetoelectric (ME) effect originating from the effective coupling between electric field and magnetism is an exciting frontier in nanoscale science such as magnetic tunneling junction (MTJ), ferroelectric/piezoelectric heterojunctions etc. The realization of switchable ME effect under external electric field in d0 semiconducting materials of single composition is needed especially for all-silicon spintronics applications because of its natural compatibility with current industry. We employ density functional theory (DFT) to reveal that the pristine Si(111)-3×3 R30° (Si3 hereafter) reconstructed surfaces of thin films with a thickness smaller than eleven bilayers support a sizeable linear ME effect with switchable direction of magnetic moment under external electric field. This is achieved through the interlayer exchange coupling effect in the antiferromagnetic regime, where the spin-up and spin-down magnetized density is located on opposite surfaces of Si3 thin films. The obtained coefficient for the linear ME effect can be four times larger than that of ferromagnetic Fe films, which fail to have the reversal switching capabilities. The larger ME effect originates from the spin-dependent screening of the spin-polarized Dirac fermion. The prediction will promote the realization of well-controlled and switchable data storage in all-silicon electronics.

Epitaxial Growth and Air-Stability of Monolayer Antimonene on PdTe2.

Monolayer antimonene is fabricated on PdTe2 by an epitaxial method. Monolayer antimonene is theoretically predicted to have a large bandgap for nanoelectronic devices. Air-exposure experiments indicate amazing chemical stability, which is great for device fabrication. A method to fabricate high-quality monolayer antimonene with several great properties for novel electronic and optoelectronic applications is provided.

Nonlinear Rashba spin splitting in transition metal dichalcogenide monolayers.

Single-layer transition-metal dichalcogenides (TMDs) such as MoS2 and MoSe2 exhibit unique electronic band structures ideal for hosting many exotic spin-orbital orderings. It has been widely accepted that Rashba spin splitting (RSS) is linearly proportional to the external field in heterostructure interfaces or to the potential gradient in polar materials. Surprisingly, an extraordinary nonlinear dependence of RSS is found in semiconducting TMD monolayers under a gate field. In contrast to small and constant RSS in polar materials, the potential gradient in non-polar TMDs gradually increases with the gate bias, resulting in nonlinear RSS with a Rashba coefficient an order-of-magnitude larger than the linear one. Most strikingly, under a large gate field MoSe2 demonstrates the largest anisotropic spin splitting among all known semiconductors to our knowledge. Based on the k·p model via symmetry analysis, we identify that the third-order contributions are responsible for the large nonlinear Rashba splitting. The gate tunable spin splitting found in semiconducting pristine TMD monolayers promises future spintronics applications in that spin polarized electrons can be generated by external gating in an experimentally accessible way.