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.

Probing spin correlations using angle-resolved photoemission in a coupled metallic/Mott insulator system.

A nearly free electron metal and a Mott insulating state can be thought of as opposite ends of the spectrum of possibilities for the motion of electrons in a solid. Understanding their interaction lies at the heart of the correlated electron problem. In the magnetic oxide metal PdCrO2, nearly free and Mott-localized electrons exist in alternating layers, forming natural heterostructures. Using angle-resolved photoemission spectroscopy, quantitatively supported by a strong coupling analysis, we show that the coupling between these layers leads to an "intertwined" excitation that is a convolution of the charge spectrum of the metallic layer and the spin susceptibility of the Mott layer. Our findings establish PdCrO2 as a model system in which to probe Kondo lattice physics and also open new routes to use the a priori nonmagnetic probe of photoemission to gain insights into the spin susceptibility of correlated electron materials.

Weyl-like points from band inversions of spin-polarised surface states in NbGeSb.

Band inversions are key to stabilising a variety of novel electronic states in solids, from topological surface states to the formation of symmetry-protected three-dimensional Dirac and Weyl points and nodal-line semimetals. Here, we create a band inversion not of bulk states, but rather between manifolds of surface states. We realise this by aliovalent substitution of Nb for Zr and Sb for S in the ZrSiS family of nonsymmorphic semimetals. Using angle-resolved photoemission and density-functional theory, we show how two pairs of surface states, known from ZrSiS, are driven to intersect each other near the Fermi level in NbGeSb, and to develop pronounced spin splittings. We demonstrate how mirror symmetry leads to protected crossing points in the resulting spin-orbital entangled surface band structure, thereby stabilising surface state analogues of three-dimensional Weyl points. More generally, our observations suggest new opportunities for engineering topologically and symmetry-protected states via band inversions of surface states.

Crossover from lattice to plasmonic polarons of a spin-polarised electron gas in ferromagnetic EuO.

Strong many-body interactions in solids yield a host of fascinating and potentially useful physical properties. Here, from angle-resolved photoemission experiments and ab initio many-body calculations, we demonstrate how a strong coupling of conduction electrons with collective plasmon excitations of their own Fermi sea leads to the formation of plasmonic polarons in the doped ferromagnetic semiconductor EuO. We observe how these exhibit a significant tunability with charge carrier doping, leading to a polaronic liquid that is qualitatively distinct from its more conventional lattice-dominated analogue. Our study thus suggests powerful opportunities for tailoring quantum many-body interactions in solids via dilute charge carrier doping.

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.

Maximal Rashba-like spin splitting via kinetic-energy-coupled inversion-symmetry breaking.

Engineering and enhancing the breaking of inversion symmetry in solids-that is, allowing electrons to differentiate between 'up' and 'down'-is a key goal in condensed-matter physics and materials science because it can be used to stabilize states that are of fundamental interest and also have potential practical applications. Examples include improved ferroelectrics for memory devices and materials that host Majorana zero modes for quantum computing. Although inversion symmetry is naturally broken in several crystalline environments, such as at surfaces and interfaces, maximizing the influence of this effect on the electronic states of interest remains a challenge. Here we present a mechanism for realizing a much larger coupling of inversion-symmetry breaking to itinerant surface electrons than is typically achieved. The key element is a pronounced asymmetry of surface hopping energies-that is, a kinetic-energy-coupled inversion-symmetry breaking, the energy scale of which is a substantial fraction of the bandwidth. Using spin- and angle-resolved photoemission spectroscopy, we demonstrate that such a strong inversion-symmetry breaking, when combined with spin-orbit interactions, can mediate Rashba-like spin splittings that are much larger than would typically be expected. The energy scale of the inversion-symmetry breaking that we achieve is so large that the spin splitting in the CoO2- and RhO2-derived surface states of delafossite oxides becomes controlled by the full atomic spin-orbit coupling of the 3d and 4d transition metals, resulting in some of the largest known Rashba-like spin splittings. The core structural building blocks that facilitate the bandwidth-scaled inversion-symmetry breaking are common to numerous materials. Our findings therefore provide opportunities for creating spin-textured states and suggest routes to interfacial control of inversion-symmetry breaking in designer heterostructures of oxides and other material classes.

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.

Strain Control of Fermiology and Many-Body Interactions in Two-Dimensional Ruthenates.

Here we demonstrate how the Fermi surface topology and quantum many-body interactions can be manipulated via epitaxial strain in the spin-triplet superconductor Sr_{2}RuO_{4} and its isoelectronic counterpart Ba_{2}RuO_{4} using oxide molecular beam epitaxy, in situ angle-resolved photoemission spectroscopy, and transport measurements. Near the topological transition of the γ Fermi surface sheet, we observe clear signatures of critical fluctuations, while the quasiparticle mass enhancement is found to increase rapidly and monotonically with increasing Ru-O bond distance. Our work demonstrates the possibilities for using epitaxial strain as a disorder-free means of manipulating emergent properties, many-body interactions, and potentially the superconductivity in correlated materials.

Tailoring the nature and strength of electron-phonon interactions in the SrTiO3(001) 2D electron liquid.

Surfaces and interfaces offer new possibilities for tailoring the many-body interactions that dominate the electrical and thermal properties of transition metal oxides. Here, we use the prototypical two-dimensional electron liquid (2DEL) at the SrTiO3(001) surface to reveal a remarkably complex evolution of electron-phonon coupling with the tunable carrier density of this system. At low density, where superconductivity is found in the analogous 2DEL at the LaAlO3/SrTiO3 interface, our angle-resolved photoemission data show replica bands separated by 100 meV from the main bands. This is a hallmark of a coherent polaronic liquid and implies long-range coupling to a single longitudinal optical phonon branch. In the overdoped regime the preferential coupling to this branch decreases and the 2DEL undergoes a crossover to a more conventional metallic state with weaker short-range electron-phonon interaction. These results place constraints on the theoretical description of superconductivity and allow a unified understanding of the transport properties in SrTiO3-based 2DELs.

Formation and Observation of a Quasi-Two-Dimensional dxy Electron Liquid in Epitaxially Stabilized Sr(2-x)La(x)TiO4 Thin Films.

We report the formation and observation of an electron liquid in Sr(2-x)La(x)TiO4, the quasi-two-dimensional counterpart of SrTiO3, through reactive molecular-beam epitaxy and in situ angle-resolved photoemission spectroscopy. The lowest lying states are found to be comprised of Ti 3d_{xy} orbitals, analogous to the LaAlO3/SrTiO3 interface and exhibit unusually broad features characterized by quantized energy levels and a reduced Luttinger volume. Using model calculations, we explain these characteristics through an interplay of disorder and electron-phonon coupling acting cooperatively at similar energy scales, which provides a possible mechanism for explaining the low free carrier concentrations observed at various oxide heterostructures such as the LaAlO3/SrTiO3 interface.

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.

Interplay of spin-orbit interactions, dimensionality, and octahedral rotations in semimetallic SrIrO(3).

We employ reactive molecular-beam epitaxy to synthesize the metastable perovskite SrIrO(3) and utilize in situ angle-resolved photoemission to reveal its electronic structure as an exotic narrow-band semimetal. We discover remarkably narrow bands which originate from a confluence of strong spin-orbit interactions, dimensionality, and both in- and out-of-plane IrO(6) octahedral rotations. The partial occupation of numerous bands with strongly mixed orbital characters signals the breakdown of the single-band Mott picture that characterizes its insulating two-dimensional counterpart, Sr(2)IrO(4), illustrating the power of structure-property relations for manipulating the subtle balance between spin-orbit interactions and electron-electron interactions.

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.

Atomic-scale control of competing electronic phases in ultrathin LaNiO3.

In an effort to scale down electronic devices to atomic dimensions, the use of transition-metal oxides may provide advantages over conventional semiconductors. Their high carrier densities and short electronic length scales are desirable for miniaturization, while strong interactions that mediate exotic phase diagrams open new avenues for engineering emergent properties. Nevertheless, understanding how their correlated electronic states can be manipulated at the nanoscale remains challenging. Here, we use angle-resolved photoemission spectroscopy to uncover an abrupt destruction of Fermi liquid-like quasiparticles in the correlated metal LaNiO3 when confined to a critical film thickness of two unit cells. This is accompanied by the onset of an insulating phase as measured by electrical transport. We show how this is driven by an instability to an incipient order of the underlying quantum many-body system, demonstrating the power of artificial confinement to harness control over competing phases in complex oxides with atomic-scale precision.

Quasiparticle dynamics and spin-orbital texture of the SrTiO3 two-dimensional electron gas.

Two-dimensional electron gases (2DEGs) in SrTiO3 have become model systems for engineering emergent behaviour in complex transition metal oxides. Understanding the collective interactions that enable this, however, has thus far proved elusive. Here we demonstrate that angle-resolved photoemission can directly image the quasiparticle dynamics of the d-electron subband ladder of this complex-oxide 2DEG. Combined with realistic tight-binding supercell calculations, we uncover how quantum confinement and inversion symmetry breaking collectively tune the delicate interplay of charge, spin, orbital and lattice degrees of freedom in this system. We reveal how they lead to pronounced orbital ordering, mediate an orbitally enhanced Rashba splitting with complex subband-dependent spin-orbital textures and markedly change the character of electron-phonon coupling, co-operatively shaping the low-energy electronic structure of the 2DEG. Our results allow for a unified understanding of spectroscopic and transport measurements across different classes of SrTiO3-based 2DEGs, and yield new microscopic insights on their functional properties.

Electronic structure of a quasi-freestanding MoS2 monolayer.

Several transition-metal dichalcogenides exhibit a striking crossover from indirect to direct band gap semiconductors as they are thinned down to a single monolayer. Here, we demonstrate how an electronic structure characteristic of the isolated monolayer can be created at the surface of a bulk MoS2 crystal. This is achieved by intercalating potassium in the interlayer van der Waals gap, expanding its size while simultaneously doping electrons into the conduction band. Our angle-resolved photoemission measurements reveal resulting electron pockets centered at the K̅ and K' points of the Brillouin zone, providing the first momentum-resolved measurements of how the conduction band dispersions evolve to yield an approximately direct band gap of ∼1.8 eV in quasi-freestanding monolayer MoS2. As well as validating previous theoretical proposals, this establishes a novel methodology for manipulating electronic structure in transition-metal dichalcogenides, opening a new route for the generation of large-area quasi-freestanding monolayers for future fundamental study and use in practical applications.

Evidence for topologically protected surface states and a superconducting phase in [Tl4](Tl(1-x)Sn(x))Te3 using photoemission, specific heat, and magnetization measurements, and density functional theory.

We report the discovery of surface states in the perovskite superconductor [Tl4]TlTe3 (Tl5Te3) and its nonsuperconducting tin-doped derivative [Tl4](Tl0.4Sn0.6)Te3 as observed by angle-resolved photoemission spectroscopy. Density functional theory calculations predict that the surface states are protected by a Z2 topology of the bulk band structure. Specific heat and magnetization measurements show that Tl5Te3 has a superconducting volume fraction in excess of 95%. Thus Tl5Te3 is an ideal material in which to study the interplay of bulk band topology and superconductivity.

Microscopic origin of electron accumulation in In2O3.

Angle-resolved photoemission spectroscopy reveals the presence of a two-dimensional electron gas at the surface of In(2)O(3)(111). Quantized subband states arise within a confining potential well associated with surface electron accumulation. Coupled Poisson-Schrödinger calculations suggest that downward band bending for the conduction band must be much bigger than band bending in the valence band. Surface oxygen vacancies acting as doubly ionized shallow donors are shown to provide the free electrons within this accumulation layer. Identification of the origin of electron accumulation in transparent conducting oxides has significant implications in the realization of devices based on these compounds.