Growth, morphology and electronic properties of epitaxial graphene on vicinal Ir(332) surface.

Superlattice induced minigaps in graphene band structure due to underlying one-dimensional nanostructuration has been demonstrated. A superperiodic potential can be introduced in graphene if the substrate is periodically structured. The successful preparation of a periodically nanostructured substrate in large scale can be obtained by carefully studying the electronic structure with a spatial averaging technique such as high-energy resolution photoemission. In this work, we present two different growth methods such as temperature programmed growth (TPG) and chemical vapor deposition (CVD) studied by scanning tunnelling microscopy (STM) and low energy electron diffraction (LEED). In both methods, we show that the original steps of Ir(332) have modified with (111) terraces and step bunching after graphene growth. Graphene grows continuously over the terrace and the step bunching areas. We observe that while TPG growth does not give rise to a well-defined surface periodicity required for opening a bandgap, the CVD growth does. By combining with angle-resolved photoemission spectroscopy (ARPES) measurements, we correlate the obtained spatial periodicity to observed band gap opening in graphene.

Spin to Charge Conversion at Room Temperature by Spin Pumping into a New Type of Topological Insulator: α-Sn Films.

We present results on spin to charge current conversion in experiments of resonant spin pumping into the Dirac cone with helical spin polarization of the elemental topological insulator (TI) α-Sn. By angle-resolved photoelectron spectroscopy (ARPES), we first check that the Dirac cone (DC) at the α-Sn (0 0 1) surface subsists after covering Sn with Ag. Then we show that resonant spin pumping at room temperature from Fe through Ag into α-Sn layers induces a lateral charge current that can be ascribed to the inverse Edelstein effect by the DC states. Our observation of an inverse Edelstein effect length much longer than those generally found for Rashba interfaces demonstrates the potential of TIs for the conversion between spin and charge in spintronic devices. By comparing our results with data on the relaxation time of TI free surface states from time-resolved ARPES, we can anticipate the ultimate potential of the TI for spin to charge conversion and the conditions to reach it.

Semiconducting Graphene from Highly Ordered Substrate Interactions.

While numerous methods have been proposed to produce semiconducting graphene, a significant band gap has never been demonstrated. The reason is that, regardless of the theoretical gap formation mechanism, subnanometer disorder prevents the required symmetry breaking necessary to make graphene semiconducting. In this work, we show for the first time that semiconducting graphene can be made by epitaxial growth. Using improved growth methods, we show by direct band measurements that a band gap greater than 0.5 eV can be produced in the first graphene layer grown on the SiC(0001) surface. This work demonstrates that order, a property that remains lacking in other graphene systems, is key to producing electronically viable semiconducting graphene.

Ultrafast Atomic Diffusion Inducing a Reversible (2sqrt[3]×2sqrt[3])R30°â†”(sqrt[3]×sqrt[3])R30° Transition on Sn/Si(111)∶B.

Dynamical phase transitions are a challenge to identify experimentally and describe theoretically. Here, we study a new reconstruction of Sn on silicon and observe a reversible transition where the surface unit cell divides its area by a factor of 4 at 250 °C. This phase transition is explained by the 24-fold degeneracy of the ground state and a novel diffusive mechanism, where four Sn atoms arranged in a snakelike cluster wiggle at the surface exploring collectively the different quantum mechanical ground states.

Two-dimensional electron gas with six-fold symmetry at the (111) surface of KTaO3.

Two-dimensional electron gases (2DEGs) at transition-metal oxide (TMO) interfaces, and boundary states in topological insulators, are being intensively investigated. The former system harbors superconductivity, large magneto-resistance, and ferromagnetism. In the latter, honeycomb-lattice geometry plus bulk spin-orbit interactions lead to topologically protected spin-polarized bands. 2DEGs in TMOs with a honeycomb-like structure could yield new states of matter, but they had not been experimentally realized, yet. We successfully created a 2DEG at the (111) surface of KTaO3, a strong insulator with large spin-orbit coupling. Its confined states form a network of weakly-dispersing electronic gutters with 6-fold symmetry, a topology novel to all known oxide-based 2DEGs. If those pertain to just one Ta-(111) bilayer, model calculations predict that it can be a topological metal. Our findings demonstrate that completely new electronic states, with symmetries not realized in the bulk, can be tailored in oxide surfaces, promising for TMO-based devices.

Tuning a Schottky barrier in a photoexcited topological insulator with transient Dirac cone electron-hole asymmetry.

The advent of Dirac materials has made it possible to realize two-dimensional gases of relativistic fermions with unprecedented transport properties in condensed matter. Their photoconductive control with ultrafast light pulses is opening new perspectives for the transmission of current and information. Here we show that the interplay of surface and bulk transient carrier dynamics in a photoexcited topological insulator can control an essential parameter for photoconductivity-the balance between excess electrons and holes in the Dirac cone. This can result in a strongly out of equilibrium gas of hot relativistic fermions, characterized by a surprisingly long lifetime of more than 50 ps, and a simultaneous transient shift of chemical potential by as much as 100 meV. The unique properties of this transient Dirac cone make it possible to tune with ultrafast light pulses a relativistic nanoscale Schottky barrier, in a way that is impossible with conventional optoelectronic materials.

Nature of the bad metallic behavior of Fe1.06Te inferred from its evolution in the magnetic state.

We investigate with angle-resolved photoelectron spectroscopy the changes of the Fermi surface and the main bands from the paramagnetic state to the antiferromagnetic (AFM) state occurring below 72 K in Fe1.06Te. The evolution is completely different from that observed in Fe pnictides, as nesting is absent. The AFM state is a rather good metal, in agreement with our magnetic band structure calculation. On the other hand, the paramagnetic state is very anomalous with a large pseudogap of ~65 meV on the electron pocket that closes in the AFM state. We discuss this behavior in connection with spin fluctuations existing above the magnetic transition and the correlations predicted in the spin-freezing regime of the incoherent metallic state.

Circular dichroism and superdiffusive transport at the surface of BiTeI.

We investigate the electronic states of BiTeI after the optical pumping with circularly polarized photons. Our data show that photoexcited electrons reach an internal thermalization within 300 fs of the arrival of the pump pulse. Instead, the dichroic contrast generated by the circularly polarized light relaxes on a time scale shorter than 80 fs. This result implies that orbital and spin polarization created by the circular pump pulse rapidly decays via manybody interaction. The persistent dichroism at longer delay times is due to the helicity dependence of superdiffussive transport. We ascribe it to the lack of inversion symmetry in an electronic system far from equilibrium conditions.

Wide-gap semiconducting graphene from nitrogen-seeded SiC.

All carbon electronics based on graphene have been an elusive goal. For more than a decade, the inability to produce significant band-gaps in this material has prevented the development of graphene electronics. We demonstrate a new approach to produce semiconducting graphene that uses a submonolayer concentration of nitrogen on SiC sufficient to pin epitaxial graphene to the SiC interface as it grows. The resulting buckled graphene opens a band gap greater than 0.7 eV in the otherwise continuous metallic graphene sheet.

Large temperature dependence of the number of carriers in co-doped BaFe(2)As(2).

Using angle-resolved photoemission spectroscopy, we study the evolution of the number of carriers in Ba(Fe(1-x)Co(x))(2)As(2) as a function of Co content and temperature. We show that there is a k-dependent energy shift compared to density functional calculations, which is large below 100 K at low Co contents and reduces the volume of hole and electron pockets by a factor 2. This k shift becomes negligible at high Co content and could be due to interband charge or spin fluctuations. We further reveal that the bands shift with temperature, changing significantly the number of carriers they contain (up to 50%). We explain this evolution by thermal excitations of carriers among the narrow bands, possibly combined with a temperature evolution of the k-dependent fluctuations.

Direct observation of a highly spin-polarized organic spinterface at room temperature.

Organic semiconductors constitute promising candidates toward large-scale electronic circuits that are entirely spintronics-driven. Toward this goal, tunneling magnetoresistance values above 300% at low temperature suggested the presence of highly spin-polarized device interfaces. However, such spinterfaces have not been observed directly, let alone at room temperature. Thanks to experiments and theory on the model spinterface between phthalocyanine molecules and a Co single crystal surface, we clearly evidence a highly efficient spinterface. Spin-polarised direct and inverse photoemission experiments reveal a high degree of spin polarisation at room temperature at this interface. We measured a magnetic moment on the molecule's nitrogen π orbitals, which substantiates an ab-initio theoretical description of highly spin-polarised charge conduction across the interface due to differing spinterface formation mechanisms in each spin channel. We propose, through this example, a recipe to engineer simple organic-inorganic interfaces with remarkable spintronic properties that can endure well above room temperature.

Understanding the insulating nature of alkali-metal/Si(111):B interfaces.

We have recently revisited the phase diagram of alkali-metal/Si(111):B semiconducting interfaces previously suggested as the possible realization of a Mott-Hubbard insulator on a triangular lattice. The insulating character of the 2√[3] × 2√[3]R30 surface reconstruction observed at the saturation coverage, i.e. 0.5 ML, has been shown to find its origin in a giant alkali-metal-induced vertical distortion. Low energy electron diffraction, photoemission spectroscopy and scanning tunneling microscopy and spectroscopy experiments coupled with linear augmented plane-wave density functional theory calculations allow a full understanding of the k-resolved band structure, explaining both the inhomogeneous charge transfers into an Si-B hybridized surface state and the opening of a band gap larger than 1 eV. Moreover, √[3] × âˆš[3]R30, 3 × 3 and 2√[3] × 2√[3]R30 surface reconstructions observed as a function of coverage may reveal a filling-controlled transition from a half-filled correlated magnetic material to a strongly distorted band insulator at saturation.

Coherent phonon coupling to individual Bloch states in photoexcited bismuth.

We investigate the temporal evolution of the electronic states at the bismuth (111) surface by means of time- and angle-resolved photoelectron spectroscopy. The binding energy of bulklike bands oscillates with the frequency of the A(1g) phonon mode, whereas surface states are insensitive to the coherent displacement of the lattice. A strong dependence of the oscillation amplitude on the electronic wave vector is correctly reproduced by ab initio calculations of electron-phonon coupling. Besides these oscillations, all the electronic states also display a photoinduced shift towards higher binding energy whose dynamics follows the evolution of the electronic temperature.

Spin-polarized electron tunneling in bcc FeCo/MgO/FeCo(001) magnetic tunnel junctions.

In combining spin- and symmetry-resolved photoemission, magnetotransport measurements and ab initio calculations we detangled the electronic states involved in the electronic transport in Fe(1-x)Co(x)(001)/MgO/Fe(1-x)Co(x)(001) magnetic tunnel junctions. Contrary to previous theoretical predictions, we observe a large reduction in TMR (from 530 to 200% at 20 K) for Co content above 25 atomic% as well as anomalies in the conductance curves. We demonstrate that these unexpected behaviors originate from a minority spin state with Δ(1) symmetry that exists below the Fermi level for high Co concentration. Using angle-resolved photoemission, this state is shown to be a two-dimensional state that occurs at both Fe(1-x)Co(x)(001) free surface, and more importantly at the interface with MgO. The combination of this interface state with the peculiar density of empty states due to chemical disorder allows us to describe in details the complex conduction behavior in this system.

Ultrafast surface carrier dynamics in the topological insulator Bi2Te3.

We discuss the ultrafast evolution of the surface electronic structure of the topological insulator Bi(2)Te(3) following a femtosecond laser excitation. Using time and angle-resolved photoelectron spectroscopy, we provide a direct real-time visualization of the transient carrier population of both the surface states and the bulk conduction band. We find that the thermalization of the surface states is initially determined by interband scattering from the bulk conduction band, lasting for about 0.5 ps; subsequently, few picoseconds are necessary for the Dirac cone nonequilibrium electrons to recover a Fermi-Dirac distribution, while their relaxation extends over more than 10 ps. The surface sensitivity of our measurements makes it possible to estimate the range of the bulk-surface interband scattering channel, indicating that the process is effective over a distance of 5 nm or less. This establishes a correlation between the nanoscale thickness of the bulk charge reservoir and the evolution of the ultrafast carrier dynamics in the surface Dirac cone.

Giant anisotropy of spin-orbit splitting at the bismuth surface.

We investigate the bismuth (111) surface by means of time and angle resolved photoelectron spectroscopy. The parallel detection of the surface states below and above the Fermi level reveals a giant anisotropy of the spin-orbit spitting. These strong deviations from the Rashba-like coupling cannot be treated in k·p perturbation theory. Instead, first principles calculations could accurately reproduce the experimental dispersion of the electronic states. Our analysis shows that the giant anisotropy of the spin-orbit splitting is due to a large out-of plane buckling of the spin and orbital texture.

Giant alkali-metal-induced lattice relaxation as the driving force of the insulating phase of alkali-metal/Si(111):B.

Ab initio density-functional theory calculations, photoemission spectroscopy (PES), scanning tunneling microscopy, and spectroscopy (STM, STS) have been used to solve the 2sqrt[3]×2sqrt[3]R30 surface reconstruction observed previously by LEED on 0.5 ML K/Si:B. A large K-induced vertical lattice relaxation occurring only for 3/4 of Si adatoms is shown to quantitatively explain both the chemical shift of 1.14 eV and the ratio 1/3 measured on the two distinct B 1s core levels. A gap is observed between valence and conduction surface bands by ARPES and STS which is shown to have mainly a Si-B character. Finally, the calculated STM images agree with our experimental results. This work solves the controversy about the origin of the insulating ground state of alkali-metal/Si(111):B semiconducting interfaces which were believed previously to be related to many-body effects.

Two-dimensional electron gas with universal subbands at the surface of SrTiO(3).

As silicon is the basis of conventional electronics, so strontium titanate (SrTiO(3)) is the foundation of the emerging field of oxide electronics. SrTiO(3) is the preferred template for the creation of exotic, two-dimensional (2D) phases of electron matter at oxide interfaces that have metal-insulator transitions, superconductivity or large negative magnetoresistance. However, the physical nature of the electronic structure underlying these 2D electron gases (2DEGs), which is crucial to understanding their remarkable properties, remains elusive. Here we show, using angle-resolved photoemission spectroscopy, that there is a highly metallic universal 2DEG at the vacuum-cleaved surface of SrTiO(3) (including the non-doped insulating material) independently of bulk carrier densities over more than seven decades. This 2DEG is confined within a region of about five unit cells and has a sheet carrier density of ∼0.33 electrons per square lattice parameter. The electronic structure consists of multiple subbands of heavy and light electrons. The similarity of this 2DEG to those reported in SrTiO(3)-based heterostructures and field-effect transistors suggests that different forms of electron confinement at the surface of SrTiO(3) lead to essentially the same 2DEG. Our discovery provides a model system for the study of the electronic structure of 2DEGs in SrTiO(3)-based devices and a novel means of generating 2DEGs at the surfaces of transition-metal oxides.

Significant reduction of electronic correlations upon isovalent Ru substitution of BaFe2As2.

We investigate Ba(Fe0.65Ru0.35)2As2, a compound in which superconductivity appears at the expense of magnetism, by transport measurements and angle resolved photoemission spectroscopy. By resolving the different Fermi surface pockets and deducing from their volumes the number of hole and electron carriers, we show that Ru induces neither hole nor electron doping. However, the Fermi surface pockets are about twice larger than in BaFe2As2. A change of sign of the Hall coefficient with decreasing temperature evidences the contribution of both carriers to the transport. Fermi velocities increase significantly with respect to BaFe2As2, suggesting a reduction of correlation effects.

Experimental study of the incoherent spectral weight in the photoemission spectra of the misfit cobaltate [Bi_{2}Ba{2}O{4}][CoO{2}]{2}.

Previous angle-resolved photoemission spectroscopy experiments in NaxCoO2 reported both a strongly renormalized bandwidth near the Fermi level and moderately renormalized Fermi velocities, leaving it unclear whether the correlations are weak or strong and how they could be quantified. We explain why this situation occurs and solve the problem by extracting clearly the coherent and incoherent parts of the band crossing the Fermi level. We show that one can use their relative weight to estimate self-consistently a quasiparticle weight Z=0.15+/-0.05. We suggest this method could be a reliable way to study the evolution of correlations in cobaltates and for comparison with other strongly correlated systems.