Giant valley-Zeeman coupling in the surface layer of an intercalated transition metal dichalcogenide.

Spin-valley locking is ubiquitous among transition metal dichalcogenides with local or global inversion asymmetry, in turn stabilizing properties such as Ising superconductivity, and opening routes towards 'valleytronics'. The underlying valley-spin splitting is set by spin-orbit coupling but can be tuned via the application of external magnetic fields or through proximity coupling. However, only modest changes have been realized to date. Here, we investigate the electronic structure of the V-intercalated transition metal dichalcogenide V1/3NbS2 using microscopic-area spatially resolved and angle-resolved photoemission spectroscopy. Our measurements and corresponding density functional theory calculations reveal that the bulk magnetic order induces a giant valley-selective Ising coupling exceeding 50 meV in the surface NbS2 layer, equivalent to application of a ~250 T magnetic field. This energy scale is of comparable magnitude to the intrinsic spin-orbit splittings, and indicates how coupling of local magnetic moments to itinerant states of a transition metal dichalcogenide monolayer provides a powerful route to controlling their valley-spin splittings.

Tomographic mapping of the hidden dimension in quasi-particle interference.

Quasiparticle interference (QPI) imaging is well established to study the low-energy electronic structure in strongly correlated electron materials with unrivalled energy resolution. Yet, being a surface-sensitive technique, the interpretation of QPI only works well for anisotropic materials, where the dispersion in the direction perpendicular to the surface can be neglected and the quasiparticle interference is dominated by a quasi-2D electronic structure. Here, we explore QPI imaging of galena, a material with an electronic structure that does not exhibit pronounced anisotropy. We find that the quasiparticle interference signal is dominated by scattering vectors which are parallel to the surface plane however originate from bias-dependent cuts of the 3D electronic structure. We develop a formalism for the theoretical description of the QPI signal and demonstrate how this quasiparticle tomography can be used to obtain information about the 3D electronic structure and orbital character of the bands.

Berry curvature generation detected by Nernst responses in ferroelectric Weyl semimetal.

The quest for nonmagnetic Weyl semimetals with high tunability of phase has remained a demanding challenge. As the symmetry-breaking control parameter, the ferroelectric order can be steered to turn on/off the Weyl semimetals phase, adjust the band structures around the Fermi level, and enlarge/shrink the momentum separation of Weyl nodes which generate the Berry curvature as the emergent magnetic field. Here, we report the realization of a ferroelectric nonmagnetic Weyl semimetal based on indium-doped Pb1- x Sn x Te alloy in which the underlying inversion symmetry as well as mirror symmetry are broken with the strength of ferroelectricity adjustable via tuning the indium doping level and Sn/Pb ratio. The transverse thermoelectric effect (i.e., Nernst effect), both for out-of-plane and in-plane magnetic field geometry, is exploited as a Berry curvature-sensitive experimental probe to manifest the generation of Berry curvature via the redistribution of Weyl nodes under magnetic fields. The results demonstrate a clean, nonmagnetic Weyl semimetal coupled with highly tunable ferroelectric order, providing an ideal platform for manipulating the Weyl fermions in nonmagnetic systems.

Interplay of spin-orbit coupling and Coulomb interaction in ZnO-based electron system.

Spin-orbit coupling (SOC) is pivotal for various fundamental spin-dependent phenomena in solids and their technological applications. In semiconductors, these phenomena have been so far studied in relatively weak electron-electron interaction regimes, where the single electron picture holds. However, SOC can profoundly compete against Coulomb interaction, which could lead to the emergence of unconventional electronic phases. Since SOC depends on the electric field in the crystal including contributions of itinerant electrons, electron-electron interactions can modify this coupling. Here we demonstrate the emergence of the SOC effect in a high-mobility two-dimensional electron system in a simple band structure MgZnO/ZnO semiconductor. This electron system also features strong electron-electron interaction effects. By changing the carrier density with Mg-content, we tune the SOC strength and achieve its interplay with electron-electron interaction. These systems pave a way to emergent spintronic phenomena in strong electron correlation regimes and to the formation of quasiparticles with the electron spin strongly coupled to the density.

Switching of band inversion and topological surface states by charge density wave.

Topologically nontrivial materials host protected edge states associated with the bulk band inversion through the bulk-edge correspondence. Manipulating such edge states is highly desired for developing new functions and devices practically using their dissipation-less nature and spin-momentum locking. Here we introduce a transition-metal dichalcogenide VTe2, that hosts a charge density wave (CDW) coupled with the band inversion involving V3d and Te5p orbitals. Spin- and angle-resolved photoemission spectroscopy with first-principles calculations reveal the huge anisotropic modification of the bulk electronic structure by the CDW formation, accompanying the selective disappearance of Dirac-type spin-polarized topological surface states that exist in the normal state. Thorough three dimensional investigation of bulk states indicates that the corresponding band inversion at the Brillouin zone boundary dissolves upon the CDW formation, by transforming into anomalous flat bands. Our finding provides a new insight to the topological manipulation of matters by utilizing CDWs' flexible characters to external stimuli.

Evolution of Electronic States and Emergence of Superconductivity in the Polar Semiconductor GeTe by Doping Valence-Skipping Indium.

GeTe is a chemically simple IV-VI semiconductor which bears a rich plethora of different physical properties induced by doping and external stimuli. Here, we report a superconductor-semiconductor-superconductor transition controlled by finely-tuned In doping. Our results reveal the existence of a critical doping concentration x_{c}=0.12 in Ge_{1-x}In_{x}Te, where various properties, including structure, resistivity, charge carrier type, and the density of states, take either an extremum or change their character. At the same time, we find indications of a change in the In-valence state from In^{3+} to In^{1+} with increasing x by core-level photoemission spectroscopy, suggesting that this system is a new promising playground to probe valence fluctuations and their possible impact on structural, electronic, and thermodynamic properties of their host.

Observation of Out-of-Plane Spin Texture in a SrTiO_{3}(111) Two-Dimensional Electron Gas.

We explore the second order bilinear magnetoelectric resistance (BMER) effect in the d-electron-based two-dimensional electron gas (2DEG) at the SrTiO_{3}(111) surface. We find evidence of a spin-split band structure with the archetypal spin-momentum locking of the Rashba effect for the in-plane component. Under an out-of-plane magnetic field, we find a BMER signal that breaks the sixfold symmetry of the electronic dispersion, which is a fingerprint for the presence of a momentum-dependent out-of-plane spin component. Relativistic electronic structure calculations reproduce this spin texture and indicate that the out-of-plane component is a ubiquitous property of oxide 2DEGs arising from strong crystal field effects. We further show that the BMER response of the SrTiO_{3}(111) 2DEG is tunable and unexpectedly large.

Fermiology and Superconductivity of Topological Surface States in PdTe_{2}.

We study the low-energy surface electronic structure of the transition-metal dichalcogenide superconductor PdTe_{2} by spin- and angle-resolved photoemission, scanning tunneling microscopy, and density-functional theory-based supercell calculations. Comparing PdTe_{2} with its sister compound PtSe_{2}, we demonstrate how enhanced interlayer hopping in the Te-based material drives a band inversion within the antibonding p-orbital manifold well above the Fermi level. We show how this mediates spin-polarized topological surface states which form rich multivalley Fermi surfaces with complex spin textures. Scanning tunneling spectroscopy reveals type-II superconductivity at the surface, and moreover shows no evidence for an unconventional component of its superconducting order parameter, despite the presence of topological surface states.

Ubiquitous formation of bulk Dirac cones and topological surface states from a single orbital manifold in transition-metal dichalcogenides.

Transition-metal dichalcogenides (TMDs) are renowned for their rich and varied bulk properties, while their single-layer variants have become one of the most prominent examples of two-dimensional materials beyond graphene. Their disparate ground states largely depend on transition metal d-electron-derived electronic states, on which the vast majority of attention has been concentrated to date. Here, we focus on the chalcogen-derived states. From density-functional theory calculations together with spin- and angle-resolved photoemission, we find that these generically host a co-existence of type-I and type-II three-dimensional bulk Dirac fermions as well as ladders of topological surface states and surface resonances. We demonstrate how these naturally arise within a single p-orbital manifold as a general consequence of a trigonal crystal field, and as such can be expected across a large number of compounds. Already, we demonstrate their existence in six separate TMDs, opening routes to tune, and ultimately exploit, their topological physics.

Author Correction: Full-gap superconductivity in spin-polarised surface states of topological semimetal ß-PdBi2.

The original version of this article contained an error in Fig. 3. The calculated patterns of quasiparticle interference in the figure were incorrect due to the wrong Wannier transformation in the calculation. This correction does not affect the discussion or the conclusion of the article.

Superconductivity at the Polar-Nonpolar Phase Boundary of SnP with an Unusual Valence State.

Structural, magnetic, and electrical characterizations reveal that SnP with an unusual valence state (nominally Sn^{3+}) undergoes a ferroelectriclike structural transition from a simple NaCl-type structure to a polar tetragonal structure at approximately 250 K at ambient pressure. First-principles calculations indicate that the experimentally observed tetragonal distortion enhances the charge transfer from Sn to P, thereby making the polar tetragonal phase energetically more stable than the nonpolar cubic phase. Hydrostatic pressure is found to promptly suppress the structural phase transition in SnP, leading to the emergence of bulk superconductivity in a phase-competitive manner. These findings suggest that control of ferroelectriclike instability in a metal can be a promising way for creating novel superconductors.

Full-gap superconductivity in spin-polarised surface states of topological semimetal ß-PdBi2.

A bulk superconductor possessing a topological surface state at the Fermi level is a promising system to realise long-sought topological superconductivity. Although several candidate materials have been proposed, experimental demonstrations concurrently exploring spin textures and superconductivity at the surface have remained elusive. Here we perform spectroscopic-imaging scanning tunnelling microscopy on the centrosymmetric superconductor ß-PdBi2 that hosts a topological surface state. By combining first-principles electronic-structure calculations and quasiparticle interference experiments, we determine the spin textures at the surface, and show not only the topological surface state but also all other surface bands exhibit spin polarisations parallel to the surface. We find that the superconducting gap fully opens in all the spin-polarised surface states. This behaviour is consistent with a possible spin-triplet order parameter expected for such in-plane spin textures, but the observed superconducting gap amplitude is comparable to that of the bulk, suggesting that the spin-singlet component is predominant in ß-PdBi2.Although several materials have been proposed as topological superconductors, spin textures and superconductivity at the surface remain elusive. Here, Iwaya et al. determine the spin textures at the surface of a superconductor ß-PdBi2 and find the superconducting gap opening in all spin-polarised surface states.

Polar metal phase stabilized in strained La-doped BaTiO3films.

Ferroelectric polarization and metallic conduction are two seemingly irreconcilable properties that cannot normally coexist in a single system, as the latter tends to screen the former. Polar metals, however, defy this rule and have thus attracted considerable attention as a new class of ferroelectrics exhibiting novel properties. Here, we fabricate a new polar metal film based on the typical ferroelectric material BaTiO3by combining chemical doping and epitaxial strain induced by a substrate. The temperature dependences of the c-axis lattice constant and the second harmonic generation intensity of La-doped BaTiO3films indicate the existence of polar transitions. In addition, through La doping, films become metallic at the polar phase, and metallicity enhancement at the polar state occurs in low-La-doped films. This intriguing behaviour is effectively explained by our first-principles calculations. Our demonstration suggests that the carrier doping to ferroelectric material with epitaxial strain serves as a new way to explore polar metals.

Observation of anomalous Hall effect in a non-magnetic two-dimensional electron system.

Anomalous Hall effect, a manifestation of Hall effect occurring in systems without time-reversal symmetry, has been mostly observed in ferromagnetically ordered materials. However, its realization in high-mobility two-dimensional electron system remains elusive, as the incorporation of magnetic moments deteriorates the device performance compared to non-doped structure. Here we observe systematic emergence of anomalous Hall effect in various MgZnO/ZnO heterostructures that exhibit quantum Hall effect. At low temperatures, our nominally non-magnetic heterostructures display an anomalous Hall effect response similar to that of a clean ferromagnetic metal, while keeping a large anomalous Hall effect angle θAHE≈20°. Such a behaviour is consistent with Giovannini-Kondo model in which the anomalous Hall effect arises from the skew scattering of electrons by localized paramagnetic centres. Our study unveils a new aspect of many-body interactions in two-dimensional electron systems and shows how the anomalous Hall effect can emerge in a non-magnetic system.

Spin-valley locking in the normal state of a transition-metal dichalcogenide superconductor.

Metallic transition-metal dichalcogenides (TMDCs) are benchmark systems for studying and controlling intertwined electronic orders in solids, with superconductivity developing from a charge-density wave state. The interplay between such phases is thought to play a critical role in the unconventional superconductivity of cuprates, Fe-based and heavy-fermion systems, yet even for the more moderately-correlated TMDCs, their nature and origins have proved controversial. Here, we study a prototypical example, 2H-NbSe2, by spin- and angle-resolved photoemission and first-principles theory. We find that the normal state, from which its hallmark collective phases emerge, is characterized by quasiparticles whose spin is locked to their valley pseudospin. This results from a combination of strong spin-orbit interactions and local inversion symmetry breaking, while interlayer coupling further drives a rich three-dimensional momentum dependence of the underlying Fermi-surface spin texture. These findings necessitate a re-investigation of the nature of charge order and superconducting pairing in NbSe2 and related TMDCs.

Observation of the quantum Hall effect in δ-doped SrTiO3.

The quantum Hall effect is a macroscopic quantum phenomenon in a two-dimensional electron system. The two-dimensional electron system in SrTiO3 has sparked a great deal of interest, mainly because of the strong electron correlation effects expected from the 3d orbitals. Here we report the observation of the quantum Hall effect in a dilute La-doped SrTiO3-two-dimensional electron system, fabricated by metal organic molecular-beam epitaxy. The quantized Hall plateaus are found to be solely stemming from the low Landau levels with even integer-filling factors, ν=4 and 6 without any contribution from odd ν's. For ν=4, the corresponding plateau disappears on decreasing the carrier density. Such peculiar behaviours are proposed to be due to the crossing between the Landau levels originating from the two subbands composed of d orbitals with different effective masses. Our findings pave a way to explore unprecedented quantum phenomena in d-electron systems.

Observation of Zeeman effect in topological surface state with distinct material dependence.

Manipulating the spins of the topological surface states represents an essential step towards exploring the exotic quantum states emerging from the time reversal symmetry breaking via magnetic doping or external magnetic fields. The latter case relies on the Zeeman effect and thereby we need to estimate the g-factor of the topological surface state precisely. Here, we report the direct observations of the Zeeman effect at the surfaces of Bi2Se3 and Sb2Te2Se by spectroscopic-imaging scanning tunnelling microscopy. The Zeeman shift of the zero mode Landau level is identified unambiguously by appropriately excluding the extrinsic effects arising from the nonlinearity in the band dispersion of the topological surface state and the spatially varying potential. Surprisingly, the g-factors of the topological surface states in Bi2Se3 and Sb2Te2Se are very different (+18 and -6, respectively). Such remarkable material dependence opens up a new route to control the spins of the topological surface states.

Spin-Selective Electron Quantum Transport in Nonmagnetic MgZnO/ZnO Heterostructures.

We report magnetotransport measurements on a high-mobility two-dimensional electron system at the nonmagnetic MgZnO/ZnO heterointerface showing distinct behavior for electrons with spin-up and spin-down orientations. The low-field Shubnikov-de Haas oscillations manifest alternating resistance peak heights which can be attributed to distinct scattering rates for different spin orientations. The tilt-field measurements at a half-integer filling factor reveal that the majority spins show usual diffusive behavior, i.e., peaks with the magnitude proportional to the index of the Landau level at the Fermi energy. By contrast, the minority spins develop "plateaus" with the magnitude of dissipative resistivity that is fairly independent of the Landau level index and is of the order of the zero-field resistivity.

Negative electronic compressibility and tunable spin splitting in WSe2.

Tunable bandgaps, extraordinarily large exciton-binding energies, strong light-matter coupling and a locking of the electron spin with layer and valley pseudospins have established transition-metal dichalcogenides (TMDs) as a unique class of two-dimensional (2D) semiconductors with wide-ranging practical applications. Using angle-resolved photoemission (ARPES), we show here that doping electrons at the surface of the prototypical strong spin-orbit TMD WSe2, akin to applying a gate voltage in a transistor-type device, induces a counterintuitive lowering of the surface chemical potential concomitant with the formation of a multivalley 2D electron gas (2DEG). These measurements provide a direct spectroscopic signature of negative electronic compressibility (NEC), a result of electron-electron interactions, which we find persists to carrier densities approximately three orders of magnitude higher than in typical semiconductor 2DEGs that exhibit this effect. An accompanying tunable spin splitting of the valence bands further reveals a complex interplay between single-particle band-structure evolution and many-body interactions in electrostatically doped TMDs. Understanding and exploiting this will open up new opportunities for advanced electronic and quantum-logic devices.

Control of a two-dimensional electron gas on SrTiO3(111) by atomic oxygen.

We report on the formation of a two-dimensional electron gas (2DEG) at the bare surface of (111) oriented SrTiO3. Angle resolved photoemission experiments reveal highly itinerant carriers with a sixfold symmetric Fermi surface and strongly anisotropic effective masses. The electronic structure of the 2DEG is in good agreement with self-consistent tight-binding supercell calculations that incorporate a confinement potential due to surface band bending. We further demonstrate that alternate exposure of the surface to ultraviolet light and atomic oxygen allows tuning of the carrier density and the complete suppression of the 2DEG.