Visualizing Higher-Fold Topology in Chiral Crystals.

Novel topological phases of matter are fruitful platforms for the discovery of unconventional electromagnetic phenomena. Higher-fold topology is one example, where the low-energy description goes beyond standard model analogs. Despite intensive experimental studies, conclusive evidence remains elusive for the multigap topological nature of higher-fold chiral fermions. In this Letter, we leverage a combination of fine-tuned chemical engineering and photoemission spectroscopy with photon energy contrast to discover the higher-fold topology of a chiral crystal. We identify all bulk branches of a higher-fold chiral fermion for the first time, critically important for allowing us to explore unique Fermi arc surface states in multiple interband gaps, which exhibit an emergent ladder structure. Through designer chemical gating of the samples in combination with our measurements, we uncover an unprecedented multigap bulk boundary correspondence. Our demonstration of multigap electronic topology will propel future research on unconventional topological responses.

Visualizing Giant Ferroelectric Gating Effects in Large-Scale WSe2/BiFeO3 Heterostructures.

Multilayers based on quantum materials (complex oxides, topological insulators, transition-metal dichalcogenides, etc.) have enabled the design of devices that could revolutionize microelectronics and optoelectronics. However, heterostructures incorporating quantum materials from different families remain scarce, while they would immensely broaden the range of possible applications. Here we demonstrate the large-scale integration of compounds from two highly multifunctional families: perovskite oxides and transition-metal dichalcogenides (TMDs). We couple BiFeO3, a room-temperature multiferroic oxide, and WSe2, a semiconducting two-dimensional material with potential for photovoltaics and photonics. WSe2 is grown by molecular beam epitaxy and transferred on a centimeter-scale onto BiFeO3 films. Using angle-resolved photoemission spectroscopy, we visualize the electronic structure of 1 to 3 monolayers of WSe2 and evidence a giant energy shift as large as 0.75 eV induced by the ferroelectric polarization direction in the underlying BiFeO3. Such a strong shift opens new perspectives in the efficient manipulation of TMD properties by proximity effects.

Electronic Structure and Enhanced Charge-Density Wave Order of Monolayer VSe2.

How the interacting electronic states and phases of layered transition-metal dichalcogenides evolve when thinned to the single-layer limit is a key open question in the study of two-dimensional materials. Here, we use angle-resolved photoemission to investigate the electronic structure of monolayer VSe2 grown on bilayer graphene/SiC. While the global electronic structure is similar to that of bulk VSe2, we show that, for the monolayer, pronounced energy gaps develop over the entire Fermi surface with decreasing temperature below Tc = 140 ± 5 K, concomitant with the emergence of charge-order superstructures evident in low-energy electron diffraction. These observations point to a charge-density wave instability in the monolayer that is strongly enhanced over that of the bulk. Moreover, our measurements of both the electronic structure and of X-ray magnetic circular dichroism reveal no signatures of a ferromagnetic ordering, in contrast to the results of a recent experimental study as well as expectations from density functional theory. Our study thus points to a delicate balance that can be realized between competing interacting states and phases in monolayer transition-metal dichalcogenides.

Surface Tomonaga-Luttinger-Liquid State on Bi/InSb(001).

A 1D metallic surface state was created on an anisotropic InSb(001) surface covered with Bi. Angle-resolved photoelectron spectroscopy (ARPES) showed a 1D Fermi contour with almost no 2D distortion. Close to the Fermi level (E_{F}), the angle-integrated photoelectron spectra showed power-law scaling with the binding energy and temperature. The ARPES plot above E_{F}, obtained thanks to a thermally broadened Fermi edge at room temperature, showed a 1D state with continuous metallic dispersion across E_{F} and power-law intensity suppression around E_{F}. These results strongly suggest a Tomonaga-Luttinger liquid on the Bi/InSb(001) surface.

Rashba-like Spin Textures in Graphene Promoted by Ferromagnet-Mediated Electronic Hybridization with a Heavy Metal.

Epitaxial graphene/ferromagnetic metal (Gr/FM) heterostructures deposited onto heavy metals have been proposed for the realization of spintronic devices because of their perpendicular magnetic anisotropy and sizable Dzyaloshinskii-Moriya interaction (DMI), allowing for both enhanced thermal stability and stabilization of chiral spin textures. However, establishing routes toward this goal requires the fundamental understanding of the microscopic origin of their unusual properties. Here, we elucidate the nature of the induced spin-orbit coupling (SOC) at Gr/Co interfaces on Ir. Through spin- and angle-resolved photoemission spectroscopy along with density functional theory, we show that the interaction of the heavy metals with the Gr layer via hybridization with the FM is the source of strong SOC in the Gr layer. Furthermore, our studies on ultrathin Co films underneath Gr reveal an energy splitting of ∼100 meV for in-plane and negligible for out-of-plane spin polarized Gr π-bands, consistent with a Rashba-SOC at the Gr/Co interface, which is either the fingerprint or the origin of the DMI. This mechanism vanishes at large Co thicknesses, where neither in-plane nor out-of-plane spin-orbit splitting is observed, indicating that Gr π-states are electronically decoupled from the heavy metal. The present findings are important for future applications of Gr-based heterostructures in spintronic devices.

Dirac cone with helical spin polarization in ultrathin α-Sn(001) films.

Spin-split two-dimensional electronic states have been observed on ultrathin Sn(001) films grown on InSb(001) substrates. Angle-resolved photoelectron spectroscopy (ARPES) performed on these films revealed Dirac-cone-like linear dispersion around the Γ¯ point of the surface Brillouin zone, suggesting nearly massless electrons belonging to 2D surface states. The states disperse across a band gap between bulklike quantum well states in the films. Moreover, both circular dichroism of ARPES and spin-resolved ARPES studies show helical spin polarization of the Dirac-cone-like surface states, suggesting a topologically protected character as in a bulk topological insulator (TI). These results indicate that a quasi-3D TI phase can be realized in ultrathin films of zero-gap semiconductors.

Orbital dependent Rashba splitting and electron-phonon coupling of 2D Bi phase on Cu(100) surface.

A monolayer of bismuth deposited on the Cu(100) surface forms a highly ordered c(2×2) reconstructed phase. The low energy single particle excitations of the c(2×2) Bi/Cu(100) present Bi-induced states with a parabolic dispersion in the energy region close to the Fermi level, as observed by angle-resolved photoemission spectroscopy. The electronic state dispersion, the charge density localization, and the spin-orbit coupling have been investigated combining photoemission spectroscopy and density functional theory, unraveling a two-dimensional Bi phase with charge density well localized at the interface. The Bi-induced states present a Rashba splitting, when the charge density is strongly localized in the Bi plane. Furthermore, the temperature dependence of the spectral density close to the Fermi level has been evaluated. Dispersive electronic states offer a large number of decay channels for transitions coupled to phonons and the strength of the electron-phonon coupling for the Bi/Cu(100) system is shown to be stronger than for Bi surfaces and to depend on the electronic state symmetry and localization.

Exploring spin-polarization in Bi-based high-Tc cuprates.

The role of spin-orbit interaction has been recently reconsidered in high-[Formula: see text] cuprates, stimulated by the recent experimental observations of spin-polarized electronic states. However, due to the complexity of the spin texture reported, the origin of the spin polarization in high-[Formula: see text] cuprates remains unclear. Here, we present the spin- and angle-resolved photoemission spectroscopy (ARPES) data on the facing momentum points that are symmetric with respect to the [Formula: see text] point, to ensure the intrinsic spin nature related to the initial state. We consistently found the very weak spin polarization only along the nodal direction, with no indication of spin-splitting of the band. Our findings thus call for a revision of the simple application of the spin-orbit interaction, which has been treated within the standard framework of the Rashba interaction in high-[Formula: see text] cuprates.

Weak electronic correlations observed in magnetic Weyl Semimetal Mn3Ge.

Using angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT) calculations, we systematically studied the electronic band structure of Mn3Ge in the vicinity of the Fermi level. We observe several bands crossing the Fermi level, confirming the metallic nature of the studied system. We further observe several flat bands along various high symmetry directions, consistent with the DFT calculations. The calculated partial density of states suggests a dominant Mn 3dorbital contribution to the total valence band DOS. With the help of orbital-resolved band structure calculations, we qualitatively identify the orbital information of the experimentally obtained band dispersions. Out-of-plane electronic band dispersions are explored by measuring the ARPES data at various photon energies. Importantly, our study suggests relatively weaker electronic correlations in Mn3Ge compared to Mn3Sn.

Quantum Confinement and Electronic Structure at the Surface of van der Waals Ferroelectric α-In2Se3.

Two-dimensional (2D) ferroelectric (FE) materials are promising compounds for next-generation nonvolatile memories due to their low energy consumption and high endurance. Among them, α-In2Se3 has drawn particular attention due to its in- and out-of-plane ferroelectricity, whose robustness has been demonstrated down to the monolayer limit. This is a relatively uncommon behavior since most bulk FE materials lose their ferroelectric character at the 2D limit due to the depolarization field. Using angle resolved photoemission spectroscopy (ARPES), we unveil another unusual 2D phenomenon appearing in 2H α-In2Se3 single crystals, the occurrence of a highly metallic two-dimensional electron gas (2DEG) at the surface of vacuum-cleaved crystals. This 2DEG exhibits two confined states, which correspond to an electron density of approximately 1013 electrons/cm2, also confirmed by thermoelectric measurements. Combination of ARPES and density functional theory (DFT) calculations reveals a direct band gap of energy equal to 1.3 ± 0.1 eV, with the bottom of the conduction band localized at the center of the Brillouin zone, just below the Fermi level. Such strong n-type doping further supports the quantum confinement of electrons and the formation of the 2DEG.

Breakdown of bulk-projected isotropy in surface electronic states of topological Kondo insulator SmB6(001).

The topology and spin-orbital polarization of two-dimensional (2D) surface electronic states have been extensively studied in this decade. One major interest in them is their close relationship with the parities of the bulk (3D) electronic states. In this context, the surface is often regarded as a simple truncation of the bulk crystal. Here we show breakdown of the bulk-related in-plane rotation symmetry in the topological surface states (TSSs) of the Kondo insulator SmB6. Angle-resolved photoelectron spectroscopy (ARPES) performed on the vicinal SmB6(001)-p(2 × 2) surface showed that TSSs are anisotropic and that the Fermi contour lacks the fourfold rotation symmetry maintained in the bulk. This result emphasizes the important role of the surface atomic structure even in TSSs. Moreover, it suggests that the engineering of surface atomic structure could provide a new pathway to tailor various properties among TSSs, such as anisotropic surface conductivity, nesting of surface Fermi contours, or the number and position of van Hove singularities in 2D reciprocal space.

Spin-Charge Interconversion in KTaO3 2D Electron Gases.

Oxide interfaces exhibit a broad range of physical effects stemming from broken inversion symmetry. In particular, they can display non-reciprocal phenomena when time reversal symmetry is also broken, e.g., by the application of a magnetic field. Examples include the direct and inverse Edelstein effects (DEE, IEE) that allow the interconversion between spin currents and charge currents. The DEE and IEE have been investigated in interfaces based on the perovskite SrTiO3 (STO), albeit in separate studies focusing on one or the other. The demonstration of these effects remains mostly elusive in other oxide interface systems despite their blossoming in the last decade. Here, the observation of both the DEE and IEE in a new interfacial two-dimensional electron gas (2DEG) based on the perovskite oxide KTaO3 is reported. 2DEGs are generated by the simple deposition of Al metal onto KTaO3 single crystals, characterized by angle-resolved photoemission spectroscopy and magnetotransport, and shown to display the DEE through unidirectional magnetoresistance and the IEE by spin-pumping experiments. Their spin-charge interconversion efficiency is then compared with that of STO-based interfaces, related to the 2DEG electronic structure, and perspectives are given for the implementation of KTaO3 2DEGs into spin-orbitronic devices is compared.

Imaging the itinerant-to-localized transmutation of electrons across the metal-to-insulator transition in V2O3.

In solids, strong repulsion between electrons can inhibit their movement and result in a "Mott" metal-to-insulator transition (MIT), a fundamental phenomenon whose understanding has remained a challenge for over 50 years. A key issue is how the wave-like itinerant electrons change into a localized-like state due to increased interactions. However, observing the MIT in terms of the energy- and momentum-resolved electronic structure of the system, the only direct way to probe both itinerant and localized states, has been elusive. Here we show, using angle-resolved photoemission spectroscopy (ARPES), that in V2O3, the temperature-induced MIT is characterized by the progressive disappearance of its itinerant conduction band, without any change in its energy-momentum dispersion, and the simultaneous shift to larger binding energies of a quasi-localized state initially located near the Fermi level.

Engineering Co2 MnAlx Si1- x Heusler Compounds as a Model System to Correlate Spin Polarization, Intrinsic Gilbert Damping, and Ultrafast Demagnetization.

Engineering of magnetic materials for developing better spintronic applications relies on the control of two key parameters: the spin polarization and the Gilbert damping, responsible for the spin angular momentum dissipation. Both of them are expected to affect the ultrafast magnetization dynamics occurring on the femtosecond timescale. Here, engineered Co2 MnAlx Si1- x Heusler compounds are used to adjust the degree of spin polarization at the Fermi energy, P, from 60% to 100% and to investigate how they correlate with the damping. It is experimentally demonstrated that the damping decreases when increasing the spin polarization from 1.1 × 10-3 for Co2 MnAl with 63% spin polarization to an ultralow value of 4.6 × 10-4 for the half-metallic ferromagnet Co2 MnSi. This allows the investigation of the relation between these two parameters and the ultrafast demagnetization time characterizing the loss of magnetization occurring after femtosecond laser pulse excitation. The demagnetization time is observed to be inversely proportional to 1 - P and, as a consequence, to the magnetic damping, which can be attributed to the similarity of the spin angular momentum dissipation processes responsible for these two effects. Altogether, the high-quality Heusler compounds allow control over the band structure and therefore the channel for spin angular momentum dissipation.

Electronic Band Structure of Ultimately Thin Silicon Oxide on Ru(0001).

Silicon oxide can be formed in a crystalline form, when prepared on a metallic substrate. It is a candidate support catalyst and possibly the ultimately thin version of a dielectric host material for two-dimensional materials and heterostructures. We determine the atomic structure and chemical bonding of the ultimately thin version of the oxide, epitaxially grown on Ru(0001). In particular, we establish the existence of two sublattices defined by metal-oxygen-silicon bridges involving inequivalent substrate sites. We further discover four electronic bands below the Fermi level, at high binding energy, two of them having a linear dispersion at their crossing K point (Dirac cones) and two others forming semiflat bands. While the latter two correspond to hybridized states between the oxide and the metal, the former relate to the topmost silicon-oxygen plane, which is not directly coupled to the substrate. Our analysis is based on high-resolution X-ray photoelectron spectroscopy, angle-resolved photoemission spectroscopy, scanning tunneling microscopy, and density functional theory calculations.

Surface electronic states of Au-induced nanowires on Ge(0 0 1).

The electronic states of Au-induced atomic nanowires on Ge(0 0 1) (Au/Ge(0 0 1) NWs) have been studied by angle-resolved photoelectron spectroscopy with linearly polarized light. We have found three electron pockets around the [Formula: see text] line, where the Fermi surfaces are closed in a surface Brillouin zone (SBZ). The results indicate 2D Fermi surfaces of Au/Ge(0 0 1) NWs whereas the atomic structure is 1D. On the basis of the polarization-dependent spectra, the relation between SBZ and the direction of the atomic NW, and the symmetry of the surface state are clarified. These are very useful for further studies on the atomic structure of NWs.

Tuning across the BCS-BEC crossover in the multiband superconductor Fe1+y Se x Te1-x : An angle-resolved photoemission study.

The crossover from Bardeen-Cooper-Schrieffer (BCS) superconductivity to Bose-Einstein condensation (BEC) is difficult to realize in quantum materials because, unlike in ultracold atoms, one cannot tune the pairing interaction. We realize the BCS-BEC crossover in a nearly compensated semimetal, Fe1+y Se x Te1-x , by tuning the Fermi energy εF via chemical doping, which permits us to systematically change Δ/εF from 0.16 to 0.50, where Δ is the superconducting (SC) gap. We use angle-resolved photoemission spectroscopy to measure the Fermi energy, the SC gap, and characteristic changes in the SC state electronic dispersion as the system evolves from a BCS to a BEC regime. Our results raise important questions about the crossover in multiband superconductors, which go beyond those addressed in the context of cold atoms.

Tunable Doping in Hydrogenated Single Layered Molybdenum Disulfide.

Structural defects in the molybdenum disulfide (MoS2) monolayer are widely known for strongly altering its properties. Therefore, a deep understanding of these structural defects and how they affect MoS2 electronic properties is of fundamental importance. Here, we report on the incorporation of atomic hydrogen in monolayered MoS2 to tune its structural defects. We demonstrate that the electronic properties of single layer MoS2 can be tuned from the intrinsic electron (n) to hole (p) doping via controlled exposure to atomic hydrogen at room temperature. Moreover, this hydrogenation process represents a viable technique to completely saturate the sulfur vacancies present in the MoS2 flakes. The successful incorporation of hydrogen in MoS2 leads to the modification of the electronic properties as evidenced by high resolution X-ray photoemission spectroscopy and density functional theory calculations. Micro-Raman spectroscopy and angle resolved photoemission spectroscopy measurements show the high quality of the hydrogenated MoS2 confirming the efficiency of our hydrogenation process. These results demonstrate that the MoS2 hydrogenation could be a significant and efficient way to achieve tunable doping of transition metal dichalcogenides (TMD) materials with non-TMD elements.

A novel artificial condensed matter lattice and a new platform for one-dimensional topological phases.

Engineered lattices in condensed matter physics, such as cold-atom optical lattices or photonic crystals, can have properties that are fundamentally different from those of naturally occurring electronic crystals. We report a novel type of artificial quantum matter lattice. Our lattice is a multilayer heterostructure built from alternating thin films of topological and trivial insulators. Each interface within the heterostructure hosts a set of topologically protected interface states, and by making the layers sufficiently thin, we demonstrate for the first time a hybridization of interface states across layers. In this way, our heterostructure forms an emergent atomic chain, where the interfaces act as lattice sites and the interface states act as atomic orbitals, as seen from our measurements by angle-resolved photoemission spectroscopy. By changing the composition of the heterostructure, we can directly control hopping between lattice sites. We realize a topological and a trivial phase in our superlattice band structure. We argue that the superlattice may be characterized in a significant way by a one-dimensional topological invariant, closely related to the invariant of the Su-Schrieffer-Heeger model. Our topological insulator heterostructure demonstrates a novel experimental platform where we can engineer band structures by directly controlling how electrons hop between lattice sites.

Rashba coupling amplification by a staggered crystal field.

There has been increasing interest in materials where relativistic effects induce non-trivial electronic states with promise for spintronics applications. One example is the splitting of bands with opposite spin chirality produced by the Rashba spin-orbit coupling in asymmetric potentials. Sizable splittings have been hitherto obtained using either heavy elements, where this coupling is intrinsically strong, or large surface electric fields. Here by means of angular resolved photoemission spectroscopy and first-principles calculations, we give evidence of a large Rashba coupling of 0.25 eV Å, leading to a remarkable band splitting up to 0.15 eV with hidden spin-chiral polarization in centrosymmetric BaNiS2. This is explained by a huge staggered crystal field of 1.4 V Å(-1), produced by a gliding plane symmetry, that breaks inversion symmetry at the Ni site. This unexpected result in the absence of heavy elements demonstrates an effective mechanism of Rashba coupling amplification that may foster spin-orbit band engineering.