Bias-Free Access to Orbital Angular Momentum in Two-Dimensional Quantum Materials.

The demonstration of a topological band inversion constitutes the most elementary proof of a quantum spin Hall insulator (QSHI). On a fundamental level, such an inverted band gap is intrinsically related to the bulk Berry curvature, a gauge-invariant fingerprint of the wave function's quantum geometric properties in Hilbert space. Intimately tied to orbital angular momentum (OAM), the Berry curvature can be, in principle, extracted from circular dichroism in angle-resolved photoemission spectroscopy (CD-ARPES), were it not for interfering final state photoelectron emission channels that obscure the initial state OAM signature. Here, we outline a full-experimental strategy to avoid such interference artifacts and isolate the clean OAM from the CD-ARPES response. Bench-marking this strategy for the recently discovered atomic monolayer system indenene, we demonstrate its distinct QSHI character and establish CD-ARPES as a scalable bulk probe to experimentally classify the topology of two-dimensional quantum materials with time reversal symmetry.

Achieving environmental stability in an atomically thin quantum spin Hall insulator via graphene intercalation.

Atomic monolayers on semiconductor surfaces represent an emerging class of functional quantum materials in the two-dimensional limit - ranging from superconductors and Mott insulators to ferroelectrics and quantum spin Hall insulators. Indenene, a triangular monolayer of indium with a gap of ~ 120 meV is a quantum spin Hall insulator whose micron-scale epitaxial growth on SiC(0001) makes it technologically relevant. However, its suitability for room-temperature spintronics is challenged by the instability of its topological character in air. It is imperative to develop a strategy to protect the topological nature of indenene during ex situ processing and device fabrication. Here we show that intercalation of indenene into epitaxial graphene provides effective protection from the oxidising environment, while preserving an intact topological character. Our approach opens a rich realm of ex situ experimental opportunities, priming monolayer quantum spin Hall insulators for realistic device fabrication and access to topologically protected edge channels.

Moiré Pattern Formation in Epitaxial Growth on a Covalent Substrate: Sb on InSb(111)A.

Structural moiré superstructures arising from two competing lattices may lead to unexpected electronic behavior. Sb is predicted to show thickness-dependent topological properties, providing potential applications for low-energy-consuming electronic devices. Here we successfully synthesize ultrathin Sb films on semi-insulating InSb(111)A. Despite the covalent nature of the substrate, which has dangling bonds on the surface, we prove by scanning transmission electron microscopy that the first layer of Sb atoms grows in an unstrained manner. Rather than compensating for the lattice mismatch of -6.4% by structural modifications, the Sb films form a pronounced moiré pattern as we evidence by scanning tunneling microscopy. Our model calculations assign the moiré pattern to a periodic surface corrugation. In agreement with theoretical predictions, irrespective of the moiré modulation, the topological surface state known on a thick Sb film is experimentally confirmed to persist down to small film thicknesses, and the Dirac point shifts toward lower binding energies with a decrease in Sb thickness.

Observation of room temperature excitons in an atomically thin topological insulator.

Optical spectroscopy of ultimately thin materials has significantly enhanced our understanding of collective excitations in low-dimensional semiconductors. This is particularly reflected by the rich physics of excitons in atomically thin crystals which uniquely arises from the interplay of strong Coulomb correlation, spin-orbit coupling (SOC), and lattice geometry. Here we extend the field by reporting the observation of room temperature excitons in a material of non-trivial global topology. We study the fundamental optical excitation spectrum of a single layer of bismuth atoms epitaxially grown on a SiC substrate (hereafter bismuthene or Bi/SiC) which has been established as a large-gap, two-dimensional (2D) quantum spin Hall (QSH) insulator. Strongly developed optical resonances are observed to emerge around the direct gap at the K and K' points of the Brillouin zone, indicating the formation of bound excitons with considerable oscillator strength. These experimental findings are corroborated, concerning both the character of the excitonic resonances as well as their energy scale, by ab-initio GW and Bethe-Salpeter equation calculations, confirming strong Coulomb interaction effects in these optical excitations. Our observations provide evidence of excitons in a 2D QSH insulator at room temperature, with excitonic and topological physics deriving from the very same electronic structure.

Ultrafast Momentum-Resolved Hot Electron Dynamics in the Two-Dimensional Topological Insulator Bismuthene.

Two-dimensional quantum spin Hall (QSH) insulators are a promising material class for spintronic applications based on topologically protected spin currents in their edges. Yet, they have not lived up to their technological potential, as experimental realizations are scarce and limited to cryogenic temperatures. These constraints have also severely restricted characterization of their dynamical properties. Here, we report on the electron dynamics of the novel room-temperature QSH candidate bismuthene after photoexcitation using time- and angle-resolved photoemission spectroscopy. We map the transiently occupied conduction band and track the full relaxation pathway of hot photocarriers. Intriguingly, we observe photocarrier lifetimes much shorter than those in conventional semiconductors. This is ascribed to the presence of topological in-gap states already established by local probes. Indeed, we find spectral signatures consistent with these earlier findings. Demonstration of the large band gap and the view into photoelectron dynamics mark a critical step toward optical control of QSH functionalities.

Design and realization of topological Dirac fermions on a triangular lattice.

Large-gap quantum spin Hall insulators are promising materials for room-temperature applications based on Dirac fermions. Key to engineer the topologically non-trivial band ordering and sizable band gaps is strong spin-orbit interaction. Following Kane and Mele's original suggestion, one approach is to synthesize monolayers of heavy atoms with honeycomb coordination accommodated on templates with hexagonal symmetry. Yet, in the majority of cases, this recipe leads to triangular lattices, typically hosting metals or trivial insulators. Here, we conceive and realize "indenene", a triangular monolayer of indium on SiC exhibiting non-trivial valley physics driven by local spin-orbit coupling, which prevails over inversion-symmetry breaking terms. By means of tunneling microscopy of the 2D bulk we identify the quantum spin Hall phase of this triangular lattice and unveil how a hidden honeycomb connectivity emerges from interference patterns in Bloch px ± ipy-derived wave functions.

A Living-Dead Magnetic Layer at the Surface of Ferrimagnetic DyTiO3 Thin Films.

When ferromagnetic films become ultrathin, key properties such as the Curie temperature and the saturation magnetization are usually depressed. This effect is thoroughly investigated in magnetic oxides such as half-metallic manganites, but much less in ferrimagnetic insulating perovskites such as rare-earth titanates RTiO3 , despite their appeal to design correlated 2D electron gases. Here, the magnetic properties of epitaxial DyTiO3 thin films are reported. While films thicker than about 50 nm show a bulk-like response, at low thickness a surprising increase of the saturation magnetization is observed. This behavior is described using a classical model of a "dead layer" but assuming that this layer is actually "living," that is, it responds to the magnetic field with a strong paramagnetic susceptibility. Through depth-dependent X-ray absorption and photoemission spectroscopy, it is shown that the "living-dead layer" corresponds to surface regions where magnetic (S = 1/2) Ti3+ ions are replaced by nonmagnetic Ti4+ ions. Hysteresis cycles at the Dy M 5 and Ti L 3 edges indicate that the surface Ti4+ ions decouple the Dy3+ ions, thus unleashing their strong paramagnetic response. Finally, it is shown how capping the DyTiO3 film can help increase the Ti3+ content near the surface and thus recover a better ferrimagnetic behavior.

Tailoring Materials for Mottronics: Excess Oxygen Doping of a Prototypical Mott Insulator.

The Mott transistor is a paradigm for a new class of electronic devices-often referred to by the term Mottronics-which are based on charge correlations between the electrons. Since correlation-induced insulating phases of most oxide compounds are usually very robust, new methods have to be developed to push such materials right to the boundary to the metallic phase in order to enable the metal-insulator transition to be switched by electric gating. Here, it is demonstrated that thin films of the prototypical Mott insulator LaTiO3 grown by pulsed laser deposition under oxygen atmosphere are readily tuned by excess oxygen doping across the line of the band-filling controlled Mott transition in the electronic phase diagram. The detected insulator to metal transition is characterized by a strong change in resistivity of several orders of magnitude. The use of suitable substrates and capping layers to inhibit oxygen diffusion facilitates full control of the oxygen content and renders the films stable against exposure to ambient conditions. These achievements represent a significant advancement in control and tuning of the electronic properties of LaTiO3+x thin films making it a promising channel material in future Mottronic devices.

In Situ Control of Separate Electronic Phases on SrTiO3 Surfaces by Oxygen Dosing.

Insulating SrTiO3 (STO) can host 2D electron systems (2DESs) on its surfaces, caused by oxygen defects. This study shows that the STO surface exhibits phase separation once the 2DES is formed and relates this inhomogeneity to recently reported magnetic order at STO surfaces and interfaces. The results open pathways to exploit oxygen defects for engineering the electronic and magnetic properties of oxides.

Two-Dimensional, but not Flat: An All-Boron Graphene with a Corrugated Structure.

The construction of single-atom-thick sheets of boron on a silver substrate, which was published in late 2015, represents a significant advance towards the realization of useful two-dimensional materials based solely on boron. This Highlight provides background information on the topic of boron allotropes and an outlook for further work in this area.

Interface-induced modulation of charge and polarization in thin film Fe(3)O(4).

Charge and polarization modulations in Fe3 O4 are controlled by taking advantage of interfacial strain effects. The feasibility of oxidation state control by strain modification is demonstrated and it is shown that this approach offers a stable configuration at room temperature. Direct evidence of how a local strain field changes the atomic coordination and introduces atomic displacements leading to polarization of Fe ions is presented.

Absence of metallicity in K-doped picene: importance of electronic correlations.

Potassium-doped picene (K(x)picene) has recently been reported to be a superconductor at x=3 with critical temperatures up to 18 K. Here we study the electronic structure of K-doped picene films by photoelectron spectroscopy and ab initio density functional theory combined with dynamical mean-field theory (DFT+DMFT). Experimentally we observe that, except for spurious spectral weight due to the lack of a homogeneous chemical potential at low K concentrations (x≈1), the spectra always display a finite energy gap. This result is supported by our DFT+DMFT calculations which provide clear evidence that K(x)picene is a Mott insulator for integer doping concentrations x=1, 2, and 3. We discuss various scenarios to understand the discrepancies with previous reports of superconductivity and metallic behavior.

Magnetic order in a frustrated two-dimensional atom lattice at a semiconductor surface.

Two-dimensional electron systems, as exploited for device applications, can lose their conducting properties because of local Coulomb repulsion, leading to a Mott-insulating state. In triangular geometries, any concomitant antiferromagnetic spin ordering can be prevented by geometric frustration, spurring speculations about 'melted' phases, known as spin liquid. Here we show that for a realization of a triangular electron system by epitaxial atom adsorption on a semiconductor, such spin disorder, however, does not appear. Our study compares the electron excitation spectra obtained from theoretical simulations of the correlated electron lattice with data from high-resolution photoemission. We find that an unusual row-wise antiferromagnetic spin alignment occurs that is reflected in the photoemission spectra as characteristic 'shadow bands' induced by the spin pattern. The magnetic order in a frustrated lattice of otherwise non-magnetic components emerges from longer-range electron hopping between the atoms. This finding can offer new ways of controlling magnetism on surfaces.

Momentum spectrometer for electron-electron coincidence studies on superconductors.

We present a new experimental setup to study electron-electron coincidences from superconducting surfaces. In our approach, electrons emitted from a surface are projected onto a time- and position-sensitive microchannel plate detector with delayline position readout. Electrons that are emitted within 2 π solid angle with respect to the surface are detected in coincidence. The detector used is a hexagonal delayline detector with enhanced multiple hit capabilities. It is read out with a Flash analog-to-digital converter. The three-dimensional momentum vector is obtained for each electron. The intrinsic dead time of the detector has been greatly reduced by implementing a new algorithm for pulse analysis. The sample holder has been matched to fit the spectrometer while being capable of cooling down the sample to 4.5 K during the measurement and heating it up to 420 K for the cleaning procedure.

High purity chemical etching and thermal passivation process for Ge(001) as nanostructure template.

An advanced two-step cleaning process of the Ge(001) surface for nanoscience requirements is presented. First, wet-chemical etching with a variant of the Piranha solution (H(2)SO(4), H(2)O(2), H(2)O) is used to remove contaminants as well as the native oxide layer. Second, passivation of the surface is achieved by a rapid thermal oxidation step, leading to a homogeneous protective oxide layer. The thickness of the oxide layer is tuned to be thick enough to protect the surface, yet thin enough to be completely removed by thermal treatment in ultra-high vacuum. The application of this recipe results in an outstandingly clean and atomically flat surface, with carbon contamination at the detection limit of x-ray photoelectron spectroscopy. Scanning tunneling microscopy and electron diffraction reveal a long range ordered surface with typical terrace diameters of ~100 nm, suitable for the growth of atomic-scale nanostructures.