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.

Van der Waals Epitaxy of Weyl-Semimetal Td-WTe2.

Epitaxial growth of WTe2 offers significant advantages, including the production of high-quality films, possible long-range in-plane ordering, and precise control over layer thicknesses. However, the mean island size of WTe2 grown by molecular beam epitaxy (MBE) in the literature is only a few tens of nanometers, which is not suitable for the implementation of devices at large lateral scales. Here we report the growth of Td -WTe2 ultrathin films by MBE on monolayer (ML) graphene, reaching a mean flake size of ≃110 nm, which is, on overage, more than three times larger than previous results. WTe2 films thicker than 5 nm have been successfully synthesized and exhibit the expected Td phase atomic structure. We rationalize the epitaxial growth of Td-WTe2 and propose a simple model to estimate the mean flake size as a function of growth parameters that can be applied to other transition metal dichalcogenides (TMDCs). Based on nucleation theory and the Kolmogorov-Johnson-Meh-Avrami (KJMA) equation, our analytical model supports experimental data showing a critical coverage of 0.13 ML above which WTe2 nucleation becomes negligible. The quality of monolayer WTe2 films is demonstrated by electronic band structure analysis using angle-resolved photoemission spectroscopy (ARPES), which is in agreement with first-principles calculations performed on free-standing WTe2 and previous reports. We found electron pockets at the Fermi level, indicating a n-type doping of WTe2 with an electron density of n = 2.0 ± 0.5 × 1012 cm-2 for each electron pocket.

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.

Emergence of Weyl fermions by ferrimagnetism in a noncentrosymmetric magnetic Weyl semimetal.

Condensed matter physics has often provided a platform for investigating the interplay between particles and fields in cases that have not been observed in high-energy physics. Here, using angle-resolved photoemission spectroscopy, we provide an example of this by visualizing the electronic structure of a noncentrosymmetric magnetic Weyl semimetal candidate NdAlSi in both the paramagnetic and ferrimagnetic states. We observe surface Fermi arcs and bulk Weyl fermion dispersion as well as the emergence of new Weyl fermions in the ferrimagnetic state. Our results establish NdAlSi as a magnetic Weyl semimetal and provide an experimental observation of ferrimagnetic regulation of Weyl fermions in condensed matter.

Quasi van der Waals Epitaxy of Rhombohedral-Stacked Bilayer WSe2 on GaP(111) Heterostructure.

The growth of bilayers of two-dimensional (2D) materials on conventional 3D semiconductors results in 2D/3D hybrid heterostructures, which can provide additional advantages over more established 3D semiconductors while retaining some specificities of 2D materials. Understanding and exploiting these phenomena hinge on knowing the electronic properties and the hybridization of these structures. Here, we demonstrate that a rhombohedral-stacked bilayer (AB stacking) can be obtained by molecular beam epitaxy growth of tungsten diselenide (WSe2) on a gallium phosphide (GaP) substrate. We confirm the presence of 3R-stacking of the WSe2 bilayer structure using scanning transmission electron microscopy (STEM) and micro-Raman spectroscopy. Also, we report high-resolution angle-resolved photoemission spectroscopy (ARPES) on our rhombohedral-stacked WSe2 bilayer grown on a GaP(111)B substrate. Our ARPES measurements confirm the expected valence band structure of WSe2 with the band maximum located at the Γ point of the Brillouin zone. The epitaxial growth of WSe2/GaP(111)B helps to understand the fundamental properties of these 2D/3D heterostructures, toward their implementation in future devices.

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.

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.

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.

Direct visualization of Rashba-split bands and spin/orbital-charge interconversion at KTaO3 interfaces.

Rashba interfaces have emerged as promising platforms for spin-charge interconversion through the direct and inverse Edelstein effects. Notably, oxide-based two-dimensional electron gases display a large and gate-tunable conversion efficiency, as determined by transport measurements. However, a direct visualization of the Rashba-split bands in oxide two-dimensional electron gases is lacking, which hampers an advanced understanding of their rich spin-orbit physics. Here, we investigate KTaO3 two-dimensional electron gases and evidence their Rashba-split bands using angle resolved photoemission spectroscopy. Fitting the bands with a tight-binding Hamiltonian, we extract the effective Rashba coefficient and bring insight into the complex multiorbital nature of the band structure. Our calculations reveal unconventional spin and orbital textures, showing compensation effects from quasi-degenerate band pairs which strongly depend on in-plane anisotropy. We compute the band-resolved spin and orbital Edelstein effects, and predict interconversion efficiencies exceeding those of other oxide two-dimensional electron gases. Finally, we suggest design rules for Rashba systems to optimize spin-charge interconversion performance.

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.

Fermi surface and kink structures in [Formula: see text] revealed by synchrotron-based ARPES.

The low-energy electronic structure, including the Fermi surface topology, of the itinerant metamagnet [Formula: see text] is investigated for the first time by synchrotron-based angle-resolved photoemission. Well-defined quasiparticle band dispersions with matrix element dependencies on photon energy or photon polarization are presented. Four bands crossing the Fermi-level, giving rise to four Fermi surface sheets are resolved; and their complete topography, effective mass as well as their electron and hole character are determined. These data reveal the presence of kink structures in the near-Fermi-level band dispersion, with energies ranging from 30 to 69 meV. Together with previously reported Raman spectroscopy and lattice dynamic calculation studies, the data suggest that these kinks originate from strong electron-phonon coupling present in [Formula: see text]. Considering that the kink structures of [Formula: see text] are similar to those of the other three members of the Ruddlesden Popper structured ruthenates, the possible universality of strong coupling of electrons to oxygen-related phonons in [Formula: see text] compounds is proposed.

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.

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 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.

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.

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.