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Layered transition metal dichalcogenides (TMDs) stabilize in multiple structural forms with profoundly distinct and exotic electronic phases. Interfacing different layer types is a promising route to manipulate TMDs' properties, not only as a means to engineer quantum devices, but also as a route to explore fundamental physics in complex matter. Here we use angle-resolved photoemission (ARPES) to investigate a strong layering-dependent enhancement of superconductivity in TaS$_2$, in which the superconducting transition temperature, $T_c$, of its $2H$ structural phase is nearly tripled when insulating $1T$ layers are inserted into the system. The study is facilitated by a novel vanadium-intercalation approach to synthesizing various TaS$_2$ polytypes, which improves the quality of ARPES data while leaving key aspects of the electronic structure and properties intact. The spectra show the clear opening of the charge density wave gap in the pure $2H$ phase and its suppression when $1T$ layers are introduced to the system. Moreover, in the mixed-layer $4Hb$ system, we observe a strongly momentum-anisotropic increase in electron-phonon coupling near the Fermi level relative to the $2H$ phase. Both phenomena help to account for the increased $T_c$ in mixed $2H$/$1T$ layer structures.

Altermagnets constitute a novel, third fundamental class of collinear magnetic ordered materials, alongside with ferro- and antiferromagnets. They share with conventional antiferromagnets the feature of a vanishing net magnetization. At the same time they show a spin-splitting of electronic bands, just as in ferromagnets, caused by the atomic exchange interaction. On the other hand, topology has recently revolutionized our understanding of condensed matter physics, introducing new phases of matter classified by intrinsic topological order. Here we connect the worlds of altermagnetism and topology, showing that the electronic structure of the altermagnet CrSb is topological and hosts a novel Weyl semimetallic state. Using high-resolution and spin angleresolved photoemission spectroscopy, we observe a large momentum-dependent spin-splitting in CrSb, reaching up to 1 eV, that induces altermagnetic Weyl nodes with an associated magnetic quantum number. At the surface we observe their spin-polarized topological Fermi-arcs. This establishes that in altermagnets the large energy scale intrinsic to the spin-splitting - orders of magnitude larger than the relativistic spin-orbit coupling - creates its own realm of robust electronic topology., Comment: Main text: 16 pages, 4 figures. Supplementary material: 23 pages, 15 figures. Comments are welcome

Tunable quantum materials hold great potential for applications. Of special interest are materials in which small lattice strain induces giant electronic responses. The kagome compounds AV3Sb5 (A = K, Rb, Cs) provide a testbed for such singular electronic states. In this study, through angle-resolved photoemission spectroscopy, we provide comprehensive spectroscopic measurements of the giant responses induced by compressive and tensile strains on the charge-density-wave (CDW) order parameter and high-order van Hove singularity (HO-VHS) in CsV3Sb5. We observe a tripling of the CDW gap magnitudes with ~1% strain, accompanied by the changes of both energy and mass of the saddle-point fermions. Our results reveal an anticorrelation between the unconventional CDW order parameter and the mass of a HO-VHS, and highlight the role of the latter in the superconducting pairing. The giant electronic responses uncover a rich strain tunability of the versatile kagome system in studying quantum interplays under lattice perturbations.

Recently, a novel magnetic phase called altermagnetism has been proposed, ushering in a third distinct magnetic phase beyond ferromagnetism and antiferromagnetism. It is expected that this groundbreaking phase exhibits unique physical properties such as C-paired spin-valley locking, anomalous Hall effect, nontrivial Berry phase, and giant magnetoresistance, etc. Among all the predicted candidates, several room temperature altermagnets are suggested to host significant potential applications in the near future. Nevertheless, direct evidence about the spin pattern of the room temperature altermagnet is still unrevealed. Previous studies found that RuO2 is identified as the most promising candidate for room temperature d-wave altermagnetism, exhibiting a substantial spin splitting of up to 1.4 eV. In this study, utilizing angle-resolved photoemission spectroscopy (ARPES), we report experimental observation of the spin splitting in RuO2. Furthermore, employing spin-ARPES, we directly observed the d-wave spin pattern. Our results unequivocally show that RuO2 is a perfect d-wave altermagnet with great potential for upcoming spintronic applications., Comment: 32 pages, 12 figures

Van Hove singularities (VHss) in the vicinity of the Fermi energy often play a dramatic role in the physics of strongly correlated electron materials. The divergence of the density of states generated by VHss can trigger the emergence of new phases such as superconductivity, ferromagnetism, metamagnetism, and density wave orders. A detailed understanding of the electronic structure of these VHss is therefore essential for an accurate description of such instabilities. Here, we study the low-energy electronic structure of the trilayer strontium ruthenate Sr$_4$Ru$_3$O$_{10}$, identifying a rich hierarchy of VHss using angle-resolved photoemission spectroscopy and millikelvin scanning tunneling microscopy. Comparison of $k$-resolved electron spectroscopy and quasiparticle interference allows us to determine the structure of the VHss and demonstrate the crucial role of spin-orbit coupling in shaping them. We use this to develop a minimal model from which we identify a new mechanism for driving a field-induced Lifshitz transition in ferromagnetic metals., Comment: 25 pages, 4 figures and supplementary material

Quantum phases can be classified by topological invariants, which take on discrete values capturing global information about the quantum state. Over the past decades, these invariants have come to play a central role in describing matter, providing the foundation for understanding superfluids, magnets, the quantum Hall effect, topological insulators, Weyl semimetals and other phenomena. Here we report a remarkable linking number (knot theory) invariant associated with loops of electronic band crossings in a mirror-symmetric ferromagnet. Using state-of-the-art spectroscopic methods, we directly observe three intertwined degeneracy loops in the material's bulk Brillouin zone three-torus, $\mathbb{T}^3$. We find that each loop links each other loop twice. Through systematic spectroscopic investigation of this linked loop quantum state, we explicitly draw its link diagram and conclude, in analogy with knot theory, that it exhibits linking number $(2,2,2)$, providing a direct determination of the invariant structure from the experimental data. On the surface of our samples, we further predict and observe Seifert boundary states protected by the bulk linked loops, suggestive of a remarkable Seifert bulk-boundary correspondence. Our observation of a quantum loop link motivates the application of knot theory to the exploration of exotic properties of quantum matter., Comment: See popular summary at https://research.princeton.edu/news/electrons-crystal-exhibit-linked-and-knotted-quantum-twists

The growth of Bi films deposited on both A and B faces of InAs(111) has been investigated by low-energy electron diffraction, scanning tunneling microscopy, and photoelectron spectroscopy using synchrotron radiation. The changes upon Bi deposition of the In 4d and Bi 5d5/2 photoelectron signals allow to get a comprehensive picture of the Bi/InAs(1 1 1) interface. From the initial stages the Bi growth on the A face (In-terminated InAs) is epitaxial, contrary to that on the B face (As- terminated InAs) that proceeds via the formation of islands. Angle-resolved photoelectron spectra show that the electronic structure of a $\approx 10$~BL deposit on the A face is identical to that of bulk Bi, while more than $\approx 30$ BL are needed for the B face. Both bulk and surface states are well accounted for by fully relativistic ab initio spin-resolved photoemission calculations., Comment: 7 pages, 7 figures

InBi(001) is formed epitaxially on InAs(111)-A by depositing Bi on to an In-rich surface. Angle-resolved photoemission measurements reveal topological electronic surface states, close to the M bar high symmetry point. This demonstrates a heteroepitaxial system entirely in the III-V family with topological electronic properties. InBi shows coexistence of Bi and In surface terminations, in contradiction with other III-V materials. For the Bi termination, the study gives a consistent physical picture of the topological surface electronic structure of InBi(001) terminated by a Bi bilayer rather than a surface formed by splitting to a Bi monolayer termination. Theoretical calculations based on relativistic density functional theory and the one-step model of photoemission clarify the relationship between the InBi(001) surface termination and the topological surface states, supporting a predominant role of the Bi bilayer termination. Furthermore, a tight-binding model based on this Bi bilayer termination with only Bi-Bi hopping terms, and no Bi-In interaction, gives a deeper insight into the spin texture., Comment: 5 figures, 12 pages (+ Sup.)

Free-standing ferromagnetic nano-membranes with thicknesses below 10 nm could effectively be used for spin selective filtering of electrons. Such membranes can work both as spin detectors in electron-spectroscopy, -microscopy and -diffraction as well as a source of spin polarized electrons. Theoretical studies and previous work has indicated that ferromagnetic membranes of a few nm have Sherman functions in the 30-60 % range and would provide an effective alternative to current spin detection technology. Here we demonstrate the fabrication of gold capped Co nano-membranes with a 2.6 nm Co layer and a total thickness below 10 nm. The membranes have a Sherman function $S\approx 0.41$ and a transmission of $3.7\times 10^{-2}$ for electron energies of 2 eV. The integration of such spin-filtering membranes in a hemispherical electron analyzer is shown to provide massively parallel detection capabilities and a "2-dimensional" figure of merit $FOM_\mathrm{2D}$ = 67.2, the highest reported to date., Comment: 5 pages, 3 figures + 6 pages, 6 figures supplementary information

Transition-metal dichalcogenides (TMDs) are renowned for their rich and varied properties. They range from metals and superconductors to strongly spin-orbit-coupled semiconductors and charge-density-wave systems, with their single-layer variants one of the most prominent current examples of two-dimensional materials beyond graphene. Their varied ground states largely depend on the 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 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., Comment: 10 pages, 4 figures

The detailed nature of electronic states mediating ferromagnetic coupling in dilute magnetic semiconductors, specifically (Ga,Mn)As, has been an issue of long debate. Two confronting models have been discussed emphasizing host band vs. impurity band carriers. Using angle resolved photoemission we are for the first time able to identify a highly dispersive Mn-induced energy band in (Ga,Mn)As. Our results show that the electronic structure of the (Ga,Mn)As system is significantly modified from that of GaAs throughout the valence band. Close to the Fermi energy, the presence of Mn induces a strong mixing of the bulk bands of GaAs, which results in the appearance of a highly dispersive band in the gap region of GaAs. For Mn concentrations above 1% the band reaches the Fermi level, and can thus host the delocalized holes needed for ferromagnetic coupling. Overall, our data provide a firm evidence of delocalized carriers belonging to the modified host valence band.

The metallic transition-metal dichalcogenides (TMDCs) are benchmark systems for studying and controlling intertwined electronic orders in solids, with superconductivity developing upon cooling 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 highly controversial. Here, we study a prototypical example, $2H$-NbSe$_2$, by spin- and angle-resolved photoemission and first-principles theory. We find that the normal state, from which its hallmark collective phases emerge, is characterised 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. Non-negligible interlayer coupling further drives a rich three-dimensional momentum-dependence of the underlying Fermi surface spin texture. Together, these findings necessitate a fundamental re-investigation of the nature of charge order and superconducting pairing in NbSe$_2$ and related TMDCs., Comment: 7 pages, 4 figures

A comprehensive understanding of spin-polarized photoemission is crucial for accessing the electronic structure of spin-orbit coupled materials. Yet, the impact of the final state in the photoemission process on the photoelectron spin has been difficult to assess in these systems. We present experiments for the spin-orbit split states in a Bi-Ag surface alloy showing that the alteration of the final state with energy may cause a complete reversal of the photoelectron spin polarization. We explain the effect on the basis of ab initio one-step photoemission theory and describe how it originates from linear dichroism in the angular distribution of photoelectrons. Our analysis shows that the modulated photoelectron spin polarization reflects the intrinsic spin density of the surface state being sampled differently depending on the final state, and it indicates linear dichroism as a natural probe of spin-orbit coupling at surfaces., Comment: New manuscript with a changed interpretation and theoretical description of the experimental results

The high index (441) surface of bismuth has been studied using Scanning Tunnelling Microscopy (STM), Angle Resolved Photoemission Spectroscopy (APRES) and spin-resolved ARPES. The surface is strongly corrugated, exposing a regular array of (110)-like terraces. Two surface localised states are observed, both of which are linearly dispersing in one in-plane direction ($k_x$), and dispersionless in the orthogonal in-plane direction ($k_y$), and both of which have a Dirac-like crossing at $k_x$=0. Spin ARPES reveals a strong in-plane polarisation, consistent with Rashba-like spin-orbit coupling. One state has a strong out-of-plane spin component, which matches with the miscut angle, suggesting its {possible} origin as an edge-state. The electronic structure of Bi(441) has significant similarities with topological insulator surface states and is expected to support one dimensional Quantum Spin Hall-like coupled spin-charge transport properties with inhibited backscattering, without requiring a topological insulator bulk.

New detailed angle-resolved photoemission data are presented, revealing the existence of an Mn-induced state that extends into the band gap of GaAs. In sharp contrast to recent reports we observe that the state is highly dispersive. Spin resolved photoemission shows that the band is spin polarized even at room temperature. The results are not consistent with any of the currently discussed band models for ferromagnetism., Comment: 18 pages, 4 figures

Methods to generate spin-polarised electronic states in non-magnetic solids are strongly desired to enable all-electrical manipulation of electron spins for new quantum devices. This is generally accepted to require breaking global structural inversion symmetry. In contrast, here we present direct evidence from spin- and angle-resolved photoemission spectroscopy for a strong spin polarisation of bulk states in the centrosymmetric transition-metal dichalcogenide WSe$_2$. We show how this arises due to a lack of inversion symmetry in constituent structural units of the bulk crystal where the electronic states are localised, leading to enormous spin splittings up to $\sim\!0.5$ eV, with a spin texture that is strongly modulated in both real and momentum space. As well as providing the first experimental evidence for a recently-predicted `hidden' spin polarisation in inversion-symmetric materials, our study sheds new light on a putative spin-valley coupling in transition-metal dichalcogenides, of key importance for using these compounds in proposed valleytronic devices., Comment: 6 pages, 4 figures

Understanding the spin-texture behavior of boundary modes in ultrathin topological insulator films is critically essential for the design and fabrication of functional nano-devices. Here by using spin-resolved photoemission spectroscopy with p-polarized light in topological insulator Bi2Se3 thin films, we report tunneling-dependent evolution of spin configuration in topological insulator thin films across the metal-to-insulator transition. We observe strongly binding energy- and wavevector-dependent spin polarization for the topological surface electrons in the ultra-thin gapped-Dirac-cone limit. The polarization decreases significantly with enhanced tunneling realized systematically in thin insulating films, whereas magnitude of the polarization saturates to the bulk limit faster at larger wavevectors in thicker metallic films. We present a theoretical model which captures this delicate relationship between quantum tunneling and Fermi surface spin polarization. Our high-resolution spin-based spectroscopic results suggest that the polarization current can be tuned to zero in thin insulating films forming the basis for a future spin-switch nano-device., Comment: To appear in Nature Communications (2014); Expanded version of http://arxiv.org/abs/1307.5485

Quantitative understanding of the relationship between quantum tunneling and Fermi surface spin polarization is key to device design using topological insulator surface states. By using spin-resolved photoemission spectroscopy with p-polarized light in topological insulator Bi2Se3 thin films across the metal-to-insulator transition, we observe that for a given film thickness, the spin polarization is large for momenta far from the center of the surface Brillouin zone. In addition, the polarization decreases significantly with enhanced tunneling realized systematically in thin insulating films, whereas magnitude of the polarization saturates to the bulk limit faster at larger wavevectors in thicker metallic films. Our theoretical model calculations capture this delicate relationship between quantum tunneling and Fermi surface spin polarization. Our results suggest that the polarization current can be tuned to zero in thin insulating films forming the basis for a future spin-switch nano-device., Comment: 8 pages, 4 figures

Angle-resolved photoemission spectroscopy reveals pronounced kinks in the dispersion of the sigma band of graphene. Such kinks are usually caused by the combination of a strong electron-boson interaction and the cut-off in the Fermi-Dirac distribution. They are therefore not expected for the $\sigma$ band of graphene that has a binding energy of more than 3.5 eV. We argue that the observed kinks are indeed caused by the electron-phonon interaction, but the role of the Fermi-Dirac distribution cutoff is assumed by a cut-off in the density of $\sigma$ states. The existence of the effect suggests a very weak coupling of holes in the $\sigma$ band not only to the $\pi$ electrons of graphene but also to the substrate electronic states. This is confirmed by the presence of such kinks for graphene on several different substrates that all show a strong coupling constant of lambda=1.

Understanding and control of spin degrees of freedom on the surfaces of topological materials are key to future applications as well as for realizing novel physics such as the axion electrodynamics associated with time-reversal (TR) symmetry breaking on the surface. We experimentally demonstrate magnetically induced spin reorientation phenomena simultaneous with a Dirac-metal to gapped-insulator transition on the surfaces of manganese-doped Bi2Se3 thin films. The resulting electronic groundstate exhibits unique hedgehog-like spin textures at low energies, which directly demonstrate the mechanics of TR symmetry breaking on the surface. We further show that an insulating gap induced by quantum tunnelling between surfaces exhibits spin texture modulation at low energies but respects TR invariance. These spin phenomena and the control of their Fermi surface geometrical phase first demonstrated in our experiments pave the way for the future realization of many predicted exotic magnetic phenomena of topological origin., Comment: 38 pages, 18 Figures, Includes new text, additional datasets and interpretation beyond arXiv:1206.2090, for the final published version see Nature Physics (2012)

We study the nature of (001) surface states in Pb_{0.73}Sn_{0.27}Se in the newly discovered topological-crystalline-insulator (TCI) phase as well as the corresponding topologically trivial state above the band-gap-inversion temperature. Our calculations predict not only metallic surface states with a nontrivial chiral spin structure for the TCI case, but also nonmetallic (gapped) surface states with nonzero spin polarization when the system is a normal insulator. For both phases, angle- and spin-resolved photoelectron spectroscopy measurements provide conclusive evidence for the formation of these (001) surface states in Pb_{0.73}Sn_{0.27}Se, as well as for their chiral spin structure., Comment: 6 pages, 2 figures

We present a spectroscopic study that reveals that the metal-insulator transition of strained VO$_2$ thin films may be driven towards a purely electronic transition, which does not rely on the Peierls dimerization, by the application of mechanical strain. Comparison with a moderately strained system, which does involve the lattice, demonstrates the crossover from Peierls- to Mott-like transitions.

Using synchrotron based photoemission, we have investigated the Mn-induced changes in Ga 3d core level spectra from as-grown ${\rm Ga}_{1-x}{\rm Mn}_{x}{\rm As}$. Although Mn is located in Ga substitutional sites, and does therefore not have any Ga nearest neighbours, the impact of Mn on the Ga core level spectra is pronounced even at Mn concentrations in the range of 0.5%. The analysis shows that each Mn atom affects a volume corresponding to a sphere with around 1.4 nm diameter., Comment: Submitted to Physical Review B, Brief Report

The surface of topological insulators is proposed as a promising platform for spintronics and quantum information applications. In particular, when time- reversal symmetry is broken, topological surface states are expected to exhibit a wide range of exotic spin phenomena for potential implementation in electronics. Such devices need to be fabricated using nanoscale artificial thin films. It is of critical importance to study the spin behavior of artificial topological MBE thin films associated with magnetic dopants, and with regards to quantum size effects related to surface-to-surface tunneling as well as experimentally isolate time-reversal breaking from non-intrinsic surface electronic gaps. Here we present observation of the first (and thorough) study of magnetically induced spin reorientation phenomena on the surface of a topological insulator. Our results reveal dramatic rearrangements of the spin configuration upon magnetic doping contrasted with chemically similar nonmagnetic doping as well as with quantum tunneling phenomena in ultra-thin high quality MBE films. While we observe that the spin rearrangement induced by quantum tunneling occurs in a time-reversal invariant fashion, we present critical and systematic observation of an out-of-plane spin texture evolution correlated with magnetic interactions, which breaks time-reversal symmetry, demonstrating microscopic TRB at a Kramers' point on the surface., Comment: 12 pages, 3 Figures, Related results at http://online.kitp.ucsb.edu/online/topomat11/hasan/oh/01.html