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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.
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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.
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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.
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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.
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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.
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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.
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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.
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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.
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The electron mobility is one of the key parameters that characterize the charge-carrier transport properties of materials, as exemplified by the quantum Hall effect as well as high-efficiency thermoelectric and solar energy conversions. For thermoelectric applications, introduction of chemical disorder is an important strategy for reducing the phonon-mediated thermal conduction, but is usually accompanied by mobility degradation. Here, we show a multilayered semimetal ß-CuAgSe overcoming such a trade-off between disorder and mobility. The polycrystalline ingot shows a giant positive magnetoresistance and Shubnikov de Haas oscillations, indicative of a high-mobility small electron pocket derived from the Ag s-electron band. Ni doping, which introduces chemical and lattice disorder, further enhances the electron mobility up to 90,000 cm(2) V(-1) s(-1) at 10 K, leading not only to a larger magnetoresistance but also a better thermoelectric figure of merit. This Ag-based layered semimetal with a glassy lattice is a new type of promising thermoelectric material suitable for chemical engineering.
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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.
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We investigate the two-dimensional highly spin-polarized electron accumulation layers commonly appearing near the surface of n-type polar semiconductors BiTeX (X=I, Br, and Cl) by angular-resolved photoemission spectroscopy. Because of the polarity and the strong spin-orbit interaction built in the bulk atomic configurations, the quantized conduction-band subbands show giant Rashba-type spin splitting. The characteristic 2D confinement effect is clearly observed also in the valence bands down to the binding energy of 4 eV. The X-dependent Rashba spin-orbit coupling is directly estimated from the observed spin-split subbands, which roughly scales with the inverse of the band-gap size in BiTeX.
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There has been increasing interest in phenomena emerging from relativistic electrons in a solid, which have a potential impact on spintronics and magnetoelectrics. One example is the Rashba effect, which lifts the electron-spin degeneracy as a consequence of spin-orbit interaction under broken inversion symmetry. A high-energy-scale Rashba spin splitting is highly desirable for enhancing the coupling between electron spins and electricity relevant for spintronic functions. Here we describe the finding of a huge spin-orbit interaction effect in a polar semiconductor composed of heavy elements, BiTeI, where the bulk carriers are ruled by large Rashba-like spin splitting. The band splitting and its spin polarization obtained by spin- and angle-resolved photoemission spectroscopy are well in accord with relativistic first-principles calculations, confirming that the spin splitting is indeed derived from bulk atomic configurations. Together with the feasibility of carrier-doping control, the giant-Rashba semiconductor BiTeI possesses excellent potential for application to various spin-dependent electronic functions.
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We study the magnetic susceptibility of a layered semiconductor BiTeI with giant Rashba spin splitting both theoretically and experimentally to explore its orbital magnetism. Apart from the core contributions, a large temperature-dependent diamagnetic susceptibility is observed when the Fermi energy E(F) is near the crossing point of the Rashba spin-split conduction bands at the time-reversal symmetry point A. On the other hand, when E(F) is below this band crossing, the susceptibility turns to be paramagnetic. These features are consistent with first-principles calculations, which also predict an enhanced orbital magnetic susceptibility with both positive and negative signs as a function of E(F) due to band (anti)crossings. Based on these observations, we propose two mechanisms for the enhanced paramagnetic orbital susceptibility.
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We study the magneto-optical (MO) response of the polar semiconductor BiTeI with giant bulk Rashba spin splitting at various carrier densities. Despite being nonmagnetic, the material is found to yield a huge MO activity in the infrared region under moderate magnetic fields (up to 3 T). Our first-principles calculations show that the enhanced MO response of BiTeI comes mainly from the intraband transitions between the Rashba-split bulk conduction bands. These transitions connecting electronic states with opposite spin directions become active due to the presence of strong spin-orbit interaction and give rise to distinct features in the MO spectra with a systematic doping dependence. We predict an even more pronounced enhancement in the low-energy MO response and dc Hall effect near the crossing (Dirac) point of the conduction bands.
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We demonstrate the formation of a two-dimensional electron gas (2DEG) at the (100) surface of the 5d transition-metal oxide KTaO3. From angle-resolved photoemission, we find that quantum confinement lifts the orbital degeneracy of the bulk band structure and leads to a 2DEG composed of ladders of subband states of both light and heavy carriers. Despite the strong spin-orbit coupling, our measurements provide a direct upper bound for the potential Rashba spin splitting of only Δk(parallel)}~0.02 Å(-1) at the Fermi level. The polar nature of the KTaO3(100) surface appears to help mediate the formation of the 2DEG as compared to nonpolar SrTiO3(100).
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The transitions between the spin-split bands by spin-orbit interaction are relevant to many novel phenomena such as the resonant dynamical magnetoelectric effect and the spin Hall effect. We perform optical spectroscopy measurements combined with first-principles calculations to study these transitions in the recently discovered giant bulk Rashba spin-splitting system BiTeI. Several novel features are observed in the optical spectra of the material including a sharp edge singularity due to the reduced dimensionality of the joint density of states and a systematic doping dependence of the intraband transitions between the Rashba-split branches. These confirm the bulk nature of the Rashba-type splitting in BiTeI and manifest the relativistic nature of the electron dynamics in a solid.
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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.
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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.
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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.
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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.