Colossal angular magnetoresistance in ferrimagnetic nodal-line semiconductors.

Efficient magnetic control of electronic conduction is at the heart of spintronic functionality for memory and logic applications1,2. Magnets with topological band crossings serve as a good material platform for such control, because their topological band degeneracy can be readily tuned by spin configurations, dramatically modulating electronic conduction3-10. Here we propose that the topological nodal-line degeneracy of spin-polarized bands in magnetic semiconductors induces an extremely large angular response of magnetotransport. Taking a layered ferrimagnet, Mn3Si2Te6, and its derived compounds as a model system, we show that the topological band degeneracy, driven by chiral molecular orbital states, is lifted depending on spin orientation, which leads to a metal-insulator transition in the same ferrimagnetic phase. The resulting variation of angular magnetoresistance with rotating magnetization exceeds a trillion per cent per radian, which we call colossal angular magnetoresistance. Our findings demonstrate that magnetic nodal-line semiconductors are a promising platform for realizing extremely sensitive spin- and orbital-dependent functionalities.

Emergent Quantum Phenomena of a Noncentrosymmetric Charge Density Wave in 1T-Transition Metal Dichalcogenides.

1T-transition metal dichalcogenides (TMDs) have been an exciting platform for exploring the intertwinement of charge density waves and strong correlation phenomena. While the David star structure has been conventionally considered as the underlying charge order in the literature, recent scanning tunneling probe experiments on several monolayer 1T-TMD materials have motivated a new, alternative structure, namely, the anion-centered David star structure. In this Letter, we show that this novel anion-centered David star structure manifestly breaks inversion symmetry, resulting in flat bands with pronounced Rashba spin-orbit couplings. These distinctive features unlock novel possibilities and functionalities for 1T-TMDs, including the giant spin Hall effect, the emergence of Chern bands, and spin liquid that spontaneously breaks crystalline rotational symmetry. Our findings establish promising avenues for exploring emerging quantum phenomena of monolayer 1T-TMDs with this novel noncentrosymmetric structure.

Control over a Wide Phase Diagram of 2D Correlated Electrons by Surface Doping; K/1T-TaS2.

We demonstrate the systematic tuning of a trivial insulator into a Mott insulator and a Mott insulator into a correlated metallic and a pseudogap state, which emerge in a quasi-two-dimensional electronic system of 1T-TaS2 through strong electron correlation. The band structure evolution is investigated upon surface doping by alkali adsorbates for two distinct phases occurring at around 220 and 10 K by angle-resolved photoelectron spectroscopy. We find contrasting behaviors upon doping that corroborate the fundamental difference of two electronic states: while the antibonding state of the spin-singlet insulator at 10 K is partially occupied to produce an emerging Mott insulating state, the presumed Mott insulating state at 220 K evolves into a correlated metallic state and then a pseudogap state. The work indicates that surface doping onto correlated 2D materials can be a powerful tool to systematically engineer a wide range of correlated electronic phases.

Robust Luttinger Liquid State of 1D Dirac Fermions in a Van der Waals System Nb9Si4Te18.

We report on the Tomonaga-Luttinger liquid (TLL) behavior in fully degenerate 1D Dirac Fermions. A ternary van der Waals material Nb9Si4Te18 incorporates in-plane NbTe2 chains, which produce a 1D Dirac band crossing Fermi energy. Tunneling conductance of electrons confined within NbTe2 chains is found to be substantially suppressed at Fermi energy, which follows a power law with a universal temperature scaling, hallmarking a TLL state. The obtained Luttinger parameter of ∼0.15 indicates a strong electron-electron interaction. The TLL behavior is found to be robust against atomic-scale defects, which might be related to the Dirac electron nature. These findings, combined with the tunability of the compound and the merit of a van der Waals material, offer a robust, tunable, and integrable platform to exploit non-Fermi liquid physics.

Tunable Mott Dirac and Kagome Bands Engineered on 1T-TaS2.

Strongly interacting electrons in hexagonal and kagome lattices exhibit rich phase diagrams of exotic quantum states, including superconductivity and correlated topological orders. However, material realizations of these electronic states have been scarce in nature or by design. Here, we theoretically propose an approach to realize artificial lattices by metal adsorption on a 2D Mott insulator 1T-TaS2. Alkali, alkaline-earth, and group 13 metal atoms are deposited in (√3 × âˆš3)R30° and 2 × 2 TaS2 superstructures of honeycomb- and kagome-lattice symmetries exhibiting Dirac and kagome bands, respectively. The strong electron correlation of 1T-TaS2 drives the honeycomb and kagome systems into correlated topological phases described by Kane-Mele-Hubbard and kagome-Hubbard models. We further show that the 2/3 or 3/4 band filling of Mott Dirac and flat bands can be achieved with a proper concentration of Mg adsorbates. Our proposal may be readily implemented in experiments, offering an attractive condensed-matter platform to exploit the interplay of correlated topological order and superconductivity.

Enhanced Berry Curvature Dipole and Persistent Spin Texture in the Bi(110) Monolayer.

Nonvanishing Berry curvature dipole (BCD) and persistent spin texture (PST) are intriguing physical manifestations of electronic states in noncentrosymmetric 2D materials. The former induces a nonlinear Hall conductivity while the latter offers a coherent spin current. Based on density-functional-theory (DFT) calculations, we demonstrate the coexistence of both phenomena in a Bi(110) monolayer with a distorted phosphorene structure. Both effects are concurrently enhanced due to the strong spin-orbit coupling of Bi while the structural distortion creates internal in-plane ferroelectricity with inversion asymmetry. We further succeed in fabricating a Bi(110) monolayer in the desired phosphorene structure on the NbSe2 substrate. Detailed atomic and electronic structures of the Bi(110)/NbSe2 heterostructure are characterized by scanning tunneling microscopy/spectroscopy and angle-resolved-photoemission spectroscopy. These results are consistent with DFT calculations which indicate the large BCD and PST are retained. Our results suggest the Bi(110)/NbSe2 heterostructure as a promising platform to exploit nonlinear Hall and coherent spin transport properties together.

Engineering Domain Wall Electronic States in Strongly Correlated van der Waals Material of 1T-TaS2.

Although a few physical methods were demonstrated for domain wall engineering in various electronic or ferroic materials with broken discrete symmetries, the direct control over the electronic properties of individual domain walls has been extremely limited. Here, we introduce a chemical method to tune the electronic property of domain walls in 1T tantalum disulfide. By using scanning tunneling microscopy and spectroscopy techniques, we find that indium adatoms on 1T-TaS2 have distinct behaviors on the domains with different bulk terminations. Moreover, the adatoms form their own chains along the edges of neighboring domains. The density functional theory calculations reveal a 1D Mott insulating state on a modified domain wall, resulting from the degenerated spin-polarized bands with electron doping from adsorbates and charge transfer from neighboring domains. This work suggests that chemical decoration by adsorbates can be widely used to tune local electronic states of domain walls and various 2D materials.

Distinguishing a Mott Insulator from a Trivial Insulator with Atomic Adsorbates.

In an electronic system with various interactions intertwined, revealing the origin of its many-body ground state is challenging and a direct experimental way to verify the correlated nature of an insulator has been lacking. Here we demonstrate a way to unambiguously distinguish a paradigmatic correlated insulator, a Mott insulator, from a trivial band insulator based on their distinct chemical behavior for a surface adsorbate using 1T-TaS_{2}, which has been debated between a spin-frustrated Mott insulator or a spin-singlet trivial insulator. We start from the observation of different sizes of spectral gaps on different surface terminations and show that potassium adatoms on these two surface layers behave in totally different ways. This can be straightforwardly understood from distinct properties of Mott and band insulators due to the fundamental difference of the half- and full-filled orbitals involved, respectively. This work not only solves an outstanding problem in this particularly interesting material but also provides a simple touchstone to identify the correlated ground state of electrons experimentally.

Pseudogap and Weak Multifractality in 2D Disordered Mott Charge-Density-Wave Insulator.

We investigate electronic states of Se-substituted 1T-TaS2 by scanning tunneling microscopy/spectroscopy (STM/STS), where superconductivity emerges from the unique Mott-charge-density-wave (Mott-CDW) state. Spatially resolved STS measurements reveal that a pseudogap replaces the Mott gap with the CDW gaps intact. The pseudogap has little correlation with the unit-cell-to-unit-cell variation in the local Se concentration but appears globally. The correlation length of the local density of states (LDOS) is substantially enhanced at the Fermi energy and decays rapidly at high energies. Furthermore, the statistical analysis of LDOS indicates the weak multifractal behavior of the wave functions. These findings suggest a correlated metallic state induced by disorder and provide a new insight into the emerging superconductivity in two-dimensional materials.

Defect-Selective Charge-Density-Wave Condensation in 2H-NbSe_{2}.

Defects have been known to substantially affect quantum states of materials including charge density wave (CDW). However, the microscopic mechanism of the influence of defects is often elusive due partly to the lack of atomic scale characterization of defects themselves. We investigate native defects of a prototypical CDW material 2H-NbSe_{2} and their microscopic interaction with CDW. Three prevailing types of atomic scale defects are classified by scanning tunneling microscope, and their atomic structures are identified by density functional theory calculations as Se vacancies and Nb intercalants. Above the transition temperature, two distinct CDW structures are found to be induced selectively by different types of defects. This intriguing phenomenon is explained by competing CDW ground states and local lattice strain fields induced by defects, providing a clear microscopic mechanism of the defect-CDW interaction.

Stable Flatbands, Topology, and Superconductivity of Magic Honeycomb Networks.

We propose a new principle to realize flatbands which are robust in real materials, based on a network superstructure of one-dimensional segments. This mechanism is naturally realized in the nearly commensurate charge-density wave of 1T-TaS_{2} with the honeycomb network of conducting domain walls, and the resulting flatband can naturally explain the enhanced superconductivity. We also show that corner states, which are a hallmark of the higher-order topological insulators, appear in the network superstructure.

Honeycomb-Lattice Mott Insulator on Tantalum Disulphide.

Effects of electron many-body interactions amplify in an electronic system with a narrow bandwidth opening a way to exotic physics. A narrow band in a two-dimensional (2D) honeycomb lattice is particularly intriguing as combined with Dirac bands and topological properties but the material realization of a strongly interacting honeycomb lattice described by the Kane-Mele-Hubbard model has not been identified. Here we report a novel approach to realize a 2D honeycomb-lattice narrow-band system with strongly interacting 5d electrons. We engineer a well-known triangular lattice 2D Mott insulator 1T-TaS_{2} into a honeycomb lattice utilizing an adsorbate superstructure. Potassium (K) adatoms at an optimum coverage deplete one-third of the unpaired d electrons and the remaining electrons form a honeycomb lattice with a very small hopping. Ab initio calculations show extremely narrow Z_{2} topological bands mimicking the Kane-Mele model. Electron spectroscopy detects an order of magnitude bigger charge gap confirming the substantial electron correlation as confirmed by dynamical mean field theory. It could be the first artificial Mott insulator with a finite spin Chern number.

Dynamical Metal to Charge-Density-Wave Junctions in an Atomic Wire Array.

We investigated the atomic scale electronic phase separation emerging from a quasi-1D charge-density-wave (CDW) state of the In atomic wire array on a Si(111) surface. Spatial variations of the CDW gap and amplitude are quantified for various interfaces of metallic and insulating CDW domains by scanning tunneling microscopy and spectroscopy (STS). The strong anisotropy in the metal-insulator junctions is revealed with an order of magnitude difference in the interwire and intrawire junction lengths of 0.4 and 7 nm, respectively. The intrawire junction length is reduced dramatically by an atomic scale impurity, indicating the tunability of the metal-insulator junction in an atomic scale. Density functional theory calculations disclose the dynamical nature of the intrawire junction formation and tunability.

Large anomalous Hall current induced by topological nodal lines in a ferromagnetic van der Waals semimetal.

Topological semimetals host electronic structures with several band-contact points or lines and are generally expected to exhibit strong topological responses. Up to now, most work has been limited to non-magnetic materials and the interplay between topology and magnetism in this class of quantum materials has been largely unexplored. Here we utilize theoretical calculations, magnetotransport and angle-resolved photoemission spectroscopy to propose Fe3GeTe2, a van der Waals material, as a candidate ferromagnetic (FM) nodal line semimetal. We find that the spin degree of freedom is fully quenched by the large FM polarization, but the line degeneracy is protected by crystalline symmetries that connect two orbitals in adjacent layers. This orbital-driven nodal line is tunable by spin orientation due to spin-orbit coupling and produces a large Berry curvature, which leads to a large anomalous Hall current, angle and factor. These results demonstrate that FM topological semimetals hold significant potential for spin- and orbital-dependent electronic functionalities.

Topological Landscape of Competing Charge Density Waves in 2H-NbSe_{2}.

Despite decades of studies of the charge density wave (CDW) of 2H-NbSe_{2}, the origin of its incommensurate CDW ground state has not been understood. We discover that the CDW of 2H-NbSe_{2} is composed of two different, energetically competing, structures. The lateral heterostructures of two CDWs are entangled as topological excitations, which give rise to a CDW phase shift and the incommensuration without a conventional domain wall. A partially melted network of topological excitations and their vertices explain an unusual landscape of domains. The unconventional topological role of competing phases disclosed here can be widely applied to various incommensuration or phase coexistence phenomena in materials.

Electrical Tuning of the Excitonic Insulator Ground State of Ta_{2}NiSe_{5}.

We demonstrate that the excitonic insulator ground state of Ta_{2}NiSe_{5} can be electrically controlled by electropositive surface adsorbates. Our studies utilizing angle-resolved photoemission spectroscopy reveal intriguing wave-vector-dependent deformations of the characteristic flattop valence band of this material upon potassium adsorption. The observed band deformation indicates a reduction of the single-particle band gap due to the Stark effect near the surface. The present study provides the foundation for the electrical tuning of the many-body quantum states in excitonic insulators.

Nanoscale Superconducting Honeycomb Charge Order in IrTe2.

Entanglement of charge orderings and other electronic orders such as superconductivity is in the core of challenging physics issues of complex materials including high temperature superconductivity. Here, we report on the observation of a unique nanometer scale honeycomb charge ordering of the cleaved IrTe2 surface, which hosts a superconducting state. IrTe2 was recently established to exhibit an intriguing cascade of stripe charge orders. The stripe phases coexist with a hexagonal phase, which is formed locally and falls into a superconducting state below 3 K. The atomic and electronic structures of the honeycomb and hexagon pattern of this phase are consistent with the charge order nature, but the superconductivity does not survive on neighboring stripe charge order domains. The present work provides an intriguing physics issue and a new direction of functionalization for two-dimensional materials.

Sublattice Interference as the Origin of σ Band Kinks in Graphene.

Kinks near the Fermi level observed in angle-resolved photoemission spectroscopy (ARPES) have been widely accepted to represent electronic coupling to collective excitations, but kinks at higher energies have eluded a unified description. We identify the mechanism leading to such kink features by means of ARPES and tight-binding band calculations on σ bands of graphene, where anomalous kinks at energies as high as ∼4 eV were reported recently [Phys. Rev. Lett. 111, 216806 (2013)]. We found that two σ bands show a strong intensity modulation with abruptly vanishing intensity near the kink features, which is due to sublattice interference. The interference induced local singularity in the matrix element is a critical factor that gives rise to apparent kink features, as confirmed by our spectral simulations without involving any coupling to collective excitations.

Nonvortical Rashba Spin Structure on a Surface with C_{1h} Symmetry.

A totally anisotropic peculiar Rashba-Bychkov (RB) splitting of electronic bands was found on the Tl/Si(110)-(1×1) surface with C_{1h} symmetry by angle- and spin-resolved photoelectron spectroscopy and first-principles theoretical calculation. The constant energy contour of the upper branch of the RB split band has a warped elliptical shape centered at a k point located between Γ[over ¯] and the edge of the surface Brillouin zone, i.e., at a point without time-reversal symmetry. The spin-polarization vector of this state is in-plane and points almost the same direction along the whole elliptic contour. This novel nonvortical RB spin structure is confirmed as a general phenomenon originating from the C_{1h} symmetry of the surface.