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Altermagnets are a novel platform to realize exotic electromagnetic properties distinct from those of conventional ferromagnets and antiferromagnets. We report results of micro-focused angle-resolved photoemission spectroscopy (ARPES) on RuO2, of which altermagnetic nature has been under fierce debate. We have elucidated the band structure of the (100), (110) and (101) surfaces of a bulk single crystal. We found that, irrespective of the surface orientation, the experimental band structures obtained by ARPES commonly show a semi-quantitative agreement with the bulk-band calculation for the nonmagnetic phase, but display a severe disagreement with that for the antiferromagnetic phase. Moreover, spin-resolved ARPES signifies a negligible spin polarization for the bulk bands. These results suggest the absence of antiferromagnetism and altermagnetic spin splitting. Furthermore, we identified a flat surface band and a dispersive one near the Fermi level at the (100)/(110) and (101) surfaces, respectively, both of which are attributed to the topological surface states associated with the bulk Dirac nodal lines. The present ARPES results suggest that the crystal-orientation-dependent topological surface/interface states need to be taken into account to properly capture the transport and catalytic characteristics of RuO2., Comment: 29 pages, 9 figures

The helicity of 3D topological insulator surface states has drawn significant attention in spintronics owing to spin-momentum locking where the carriers' spin is oriented perpendicular to their momentum. This property can provide an efficient method to convert charge currents into spin currents, and vice-versa, through the Rashba-Edelstein effect. However, experimental signatures of these surface states to the spin-charge conversion are extremely difficult to disentangle from bulk state contributions. Here, we combine spin- and angle-resolved photo-emission spectroscopy, and time-resolved THz emission spectroscopy to categorically demonstrate that spin-charge conversion arises mainly from the surface state in Bi$_{1-x}$Sb$_x$ ultrathin films, down to few nanometers where confinement effects emerge. We correlate this large conversion efficiency, typically at the level of the bulk spin Hall effect from heavy metals, to the complex Fermi surface obtained from theoretical calculations of the inverse Rashba-Edelstein response. %We demonstrate this for film thickness down to a few nanometers, Both surface state robustness and sizeable conversion efficiency in epitaxial Bi$_{1-x}$Sb$_x$ thin films bring new perspectives for ultra-low power magnetic random-access memories and broadband THz generation., Comment: 23 pages, 3 figures

An anomalous $(2\times2)$ charge density wave (CDW) phase emerges in monolayer 1T-TiTe$_2$ which is absent for the bulk compound, and whose origin is still poorly understood. Here, we investigate the electronic band structure evolution across the CDW transition using temperature-dependent angle-resolved photoemission spectroscopy. Our study reveals an orbital-selective band hybridisation between the backfolded conduction and valence bands occurring at the CDW phase transition, which in turn leads to a significant electronic energy gain, underpinning the CDW transition. For the bulk compound, we show how this energy gain is almost completely suppressed due to the three-dimensionality of the electronic band structure, including via a $k_z$-dependent band inversion which switches the orbital character of the valence states. Our study thus sheds new light on how control of the electronic dimensionalilty can be used to trigger the emergence of new collective states in 2D materials.

In intermetallic compounds with zero-orbital momentum ($L=0$) the magnetic anisotropy and the electronic band structure are interconnected. Here, we investigate this connection on divalent Eu and trivalent Gd intermetallic compounds. We find by X-ray magnetic circular dichroism an out-of-plane easy magetization axis in 2D atom-thick EuAu$_2$. Angle-resolved photoemission and density-functional theory prove that this is due to strong $f-d$ band hybridization and Eu$^{2+}$ valence. In contrast, the easy in-plane magnetization of the structurally-equivalent GdAu$_2$ is ruled by spin-orbit-split $d$-bands, notably Weyl nodal lines, occupied in the Gd$^{3+}$ state. Regardless of the $L$ value, we predict a similar itinerant electron contribution to the anisotropy of analogous compounds., Comment: 9 pages, 4 figures; Supplemental Material 10 pages, 9 figures

Hybridization between $f$ electrons and conduction bands ($c$-$f$ hybridization) is a driving force for many unusual phenomena. To provide insight into it, systematic studies of CeCoIn$_5$ heavy fermion superconductor have been performed by angle-resolved photoemission spectroscopy (ARPES) in a large angular range at temperature of $T=6$ K. The used photon energy of 122 eV corresponds to Ce $4d$-$4f$ resonance. Calculations carried out with relativistic multiple scattering Korringa-Kohn-Rostoker method and one-step model of photoemission yielded realistic simulation of the ARPES spectra indicating that Ce-In surface termination prevails. Surface states, which have been identified in the calculations, contribute significantly to the spectra. Effects of the hybridization strongly depend on wave vector. They include a dispersion of heavy electrons and bands gaining $f$-electron character when approaching Fermi energy. We have also observed a considerable variation of $f$-electron spectral weight at $E_F$, which is normally determined by both matrix element effects and wave vector dependent $c$-$f$ hybridization. Fermi surface scans covering a few Brillouin zones revealed large matrix element effects. A symmetrization of experimental Fermi surface, which reduces matrix element contribution, yielded a specific variation of $4f$-electron enhanced spectral intensity at $E_F$ around $\bar{\Gamma}$ and $\bar{M}$ points. Tight-binding approximation calculations for Ce-In plane provided the same universal distribution of $4f$-electron density for a range of values of the parameters used in the model., Comment: 15 pages, 9 figures

Epitaxial bilayer silicon oxide is a transferable two-dimensional material predicted to be a wide band gap semiconductor, with potential applications for deep UV optoelectronics, or as a building block of van der Waals heterostructures. The prerequisite to any sort of such applications is the knowledge of the electronic band structure, which we unveil using angle-resolved photoemission spectroscopy and rationalise with the help of density functional theory calculations. We discover dispersing bands related to electronic delocalisation within the top and bottom planes of the material, with two linear crossings reminiscent of those predicted in bilayer AA-stacked graphene, and semi-flat bands stemming from the chemical bridges between the two planes. This band structure is robust against exposure to air, and can be controled by exposure to oxygen. We provide an experimental lower-estimate of the band gap size of 5 eV and predict a full gap of 7.36 eV using density functional theory calculations.

We report the observation of a two-dimensional electron system (2DES) at the $(110)$ surface of the transparent bulk insulator SnO$_2$, and the tunability of its carrier density by means of temperature or Eu deposition. The 2DES is insensitive to surface reconstructions and, surprisingly, it survives even after exposure to ambient conditions --an extraordinary fact recalling the well known catalytic properties SnO$_2$. Our data show that surface oxygen vacancies are at the origin of such 2DES, providing key information about the long-debated origin of $n$-type conductivity in SnO$_2$, at the basis of a wide range of applications. Furthermore, our study shows that the emergence of a 2DES in a given oxide depends on a delicate interplay between its crystal structure and the orbital character of its conduction band., Comment: 11 pages, 12 figures

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 time scale. Here, we use engineered Co2MnAlxSi1-x Heusler compounds to adjust the degree of spin polarization P from 60 to 100% and investigate how it correlates with the damping. We demonstrate experimentally that the damping decreases when increasing the spin polarization from 1.1 10-3 for Co2MnAl with 63% spin polarization to an ultra-low value of 4.10-4 for the half-metal magnet Co2MnSi. This allows us investigating 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, our high quality Heusler compounds allow controlling the band structure and therefore the channel for spin angular momentum dissipation.

Electronic band structures in solids stem from a periodic potential reflecting the structure of either the crystal lattice or an electronic order. In the stoichiometric ruthenate Ca$_3$Ru$_2$O$_7$, numerous Fermi surface sensitive probes indicate a low-temperature electronic reconstruction. Yet, the causality and the reconstructed band structure remain unsolved. Here, we show by angle-resolved photoemission spectroscopy, how in Ca$_3$Ru$_2$O$_7$ a $C_2$-symmetric massive Dirac semimetal is realized through a Brillouin-zone preserving electronic reconstruction. This Dirac semimetal emerges in a two-stage transition upon cooling. The Dirac point and band velocities are consistent with constraints set by quantum oscillation, thermodynamic, and transport experiments, suggesting that the complete Fermi surface is resolved. The reconstructed structure -- incompatible with translational-symmetry-breaking density waves -- serves as an important test for band structure calculations of correlated electron systems.

Band inversions are key to stabilising a variety of novel electronic states in solids, from topological surface states in inverted bulk band gaps of topological insulators to the formation of symmetry-protected three-dimensional Dirac and Weyl points and nodal-line semimetals. Here, we create a band inversion not of bulk states, but rather between manifolds of surface states. We realise this by aliovalent substitution of Nb for Zr and Sb for S in the ZrSiS family of nonsymmorphic semimetals. Using angle-resolved photoemission and density-functional theory, we show how two pairs of surface states, known from ZrSiS, are driven to intersect each other in the vicinity of the Fermi level in NbGeSb, as well as to develop pronounced spin-orbit mediated spin splittings. We demonstrate how mirror symmetry leads to protected crossing points in the resulting spin-orbital entangled surface band structure, thereby stabilising surface state analogues of three-dimensional Weyl points. More generally, our observations suggest new opportunities for engineering topologically and symmetry-protected states via band inversions of surface states., Comment: In press at Nature Communications. This is the originally submitted manuscript prior to changes during the review process. Contains 20+6 pages, including Supplementary Information

The prediction of ultra-low magnetic damping in Co 2 MnZ Heusler half-metal thin-film magnets is explored in this study and the damping response is shown to be linked to the underlying electronic properties. By substituting the Z elements in high crystalline quality films (Co 2 MnZ with Z=Si, Ge, Sn, Al, Ga, Sb), electronic properties such as the minority spin band gap, Fermi energy position in the gap and spin polarization can be tuned and the consequence on magnetization dynamics analyzed. The experimental results allow us to directly explore the interplay of spin polarization, spin gap, Fermi energy position and the magnetic damping obtained in these films, together with ab initio calculation predictions. The ultra-low magnetic damping coefficients measured in the range 4.1 10-4-9 10-4 for Co 2 MnSi, Ge, Sn, Sb are the lowest values obtained on a conductive layer and offers a clear experimental demonstration of theoretical predictions on Half-Metal Magnetic Heusler compounds and a pathway for future materials design.

Single crystalline bismuth (Bi) is known to have a peculiar electronic structure which is very close to the topological phase transition. The modification of the surface states of Bi depending on the temperature are revealed by angle-resolved photoelectron spectroscopy (ARPES). At low temperature, the upper branch of the surface state merged to the projected bulk conduction bands around the $\bar{M}$ point of the surface Brillouin zone (SBZ). In contrast, the same branch merged to the projected bulk valence bands at high temperature (400 K). Such behavior could be interpreted as a topological phase transition driven by the temperature, which might be applicable for future spin-thermoelectric devices. We discuss the possible mechanisms to cause such transition, such as the thermal lattice distortion and electron-phonon coupling., Comment: 15 pages with 6 figures (single column)

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 (2D) 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 sub-lattices defined by metal-oxygen-silicon bridges involving inequivalent substrate sites. We further discover four electronic bands below Fermi level, at high binding energies, two of them forming a Dirac cone at K point, and two others forming semi-flat 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., Comment: Main part : 31 pages, 6 figures / Supporting information : 13 pages, 11 figures

In Sr2IrO4 and Sr3Ir2O7, correlations, magnetism and spin-orbit coupling compete on similar energy scales, creating a new context to study metal-insulator transitions (MIT). We use here Angle-Resolved photoemission to investigate the MIT as a function of hole and electron doping in Sr3Ir2O7, obtained respectively by Ir/Rh and Sr/La substitutions. We show that there is a clear reduction as a function of doping of the gap between a lower and upper band on both sides of the Fermi level, from 0.2eV to 0.05eV. Although these two bands have a counterpart in band structure calculations, they are characterized by a very different degree of coherence. The upper band exhibits clear quasiparticle peaks, while the lower band is very broad and loses weight as a function of doping. Moreover, their ARPES spectral weights obey different periodicities, reinforcing the idea of their different nature. We argue that a very similar situation occurs in Sr2IrO4 and conclude that the physics of the two families is essentially the same.

The electronic structure of the reentrant superconductor Eu(Fe$_{0.86}$Ir$_{0.14}$)$_{2}$As$_{2}$ (T$_c$ = 22 K) with coexisting ferromagnetic order (T$_M$ = 18 K) is investigated using angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling spectroscopy (STS). We study the in-plane and out-of-plane band dispersions and Fermi surface (FS) of Eu(Fe$_{0.86}$Ir$_{0.14}$)$_{2}$As$_{2}$. The near E$_F$ Fe 3d-derived band dispersions near the $\Gamma$ and X high-symmetry points show changes due to Ir substitution, but the FS topology is preserved. From momentum dependent measurements of the superconducting gap measured at T = 5 K, we estimate an essentially isotropic s-wave gap ($\Delta\sim5.25\pm 0.25$ meV), indicative of strong-coupling superconductivity with 2$\Delta$/k$_{B}$T$_{c}\simeq$ 5.8. The gap gets closed at temperatures T $\geq$ 10 K, and this is attributed to the resistive phase which sets in at T$_M$ = 18 K due to the Eu$^{2+}$-derived magnetic order. The modifications of the FS with Ir substitution clearly indicates an effective hole doping with respect to the parent compound., Comment: 6 pages, 5 figures

We realize a two-dimensional electron system (2DES) in ZnO by simply depositing pure aluminum on its surface in ultra-high vacuum, and characterize its electronic structure using angle-resolved photoemission spectroscopy. The aluminum oxidizes into alumina by creating oxygen vacancies that dope the bulk conduction band of ZnO and confine the electrons near its surface. The electron density of the 2DES is up to two orders of magnitude higher than those obtained in ZnO heterostructures. The 2DES shows two $s$-type subbands, that we compare to the $d$-like 2DESs in titanates, with clear signatures of many-body interactions that we analyze through a self-consistent extraction of the system self-energy and a modeling as a coupling of a 2D Fermi liquid with a Debye distribution of phonons., Comment: Article + Supplementary Material, 12 pages, 3 main figures, 6 supplementary figures

In this paper we analyze in details the electronic properties of (Co/Ni) multilayers, a model system for spintronics devices. We use magneto-optical Kerr (MOKE), spin-polarized photoemission spectroscopy (SRPES), x-ray magnetic circular dichroism (XMCD) and anomalous surface diffraction experiments to investigate the electronic properties and perpendicular magnetic anisotropy (PMA) in [Co(x)/Ni(y)] single-crystalline stacks grown by molecular beam epitaxy., Comment: 11 pages, 11 figures, 1 Table

The organic spinterface describes the spin-polarized properties that develop, due to charge transfer, at the interface between a ferromagnetic metal (FM) and the molecules of an organic semiconductor. Yet, if the latter is also magnetic (e.g. molecular spin chains), the interfacial magnetic coupling can generate complexity within magnetotransport experiments. Also, assembling this interface may degrade the properties of its constituents (e.g. spin crossover or non-sublimable molecules). To circumvent these issues, one can separate the molecular and FM films using a less reactive nonmagnetic metal (NM). Spin-resolved photoemission spectroscopy measurements on the prototypical system Co(001)//Cu/Mnphthalocyanine (MnPc) reveal that the Cu/MnPc spinterface atop ferromagnetic Co is highly spin-polarized at room temperature, up to Cu spacer thicknesses of at least 10 monolayers. Ab-initio theory describes a spin polarization of the topmost Cu layer after molecular hybridization that can be accompanied by magnetic hardening effects. This spinterface's unexpected robustness paves the way for 1) integrating electronically fragile molecules within organic spinterfaces, and 2) manipulating molecular spin chains using the well-documented spin transfer torque properties of the FM/NM bilayer., Comment: 16 pages. Submitted

We report the electronic band structures and concomitant Fermi surfaces for a family of exfoliable tetradymite compounds with the formula $T_2$$Ch_2$$Pn$, obtained as a modification to the well-known topological insulator binaries Bi$_2$(Se,Te)$_3$ by replacing one chalcogen ($Ch$) with a pnictogen ($Pn$) and Bi with the tetravalent transition metals $T$ $=$ Ti, Zr, or Hf. This imbalances the electron count and results in layered metals characterized by relatively high carrier mobilities and bulk two-dimensional Fermi surfaces whose topography is well-described by first principles calculations. Intriguingly, slab electronic structure calculations predict Dirac-like surface states. In contrast to Bi$_2$Se$_3$, where the surface Dirac bands are at the $\Gamma-$point, for (Zr,Hf)$_2$Te$_2$(P,As) there are Dirac cones of strong topological character around both the $\bar {\Gamma}$- and $\bar {M}$-points which are above and below the Fermi energy, respectively. For Ti$_2$Te$_2$P the surface state is predicted to exist only around the $\bar {M}$-point. In agreement with these predictions, the surface states that are located below the Fermi energy are observed by angle resolved photoemission spectroscopy measurements, revealing that they coexist with the bulk metallic state. Thus, this family of materials provides a foundation upon which to develop novel phenomena that exploit both the bulk and surface states (e.g., topological superconductivity).

Germanium telluride features special spin-electric effects originating from spin-orbit coupling and symmetry breaking by the ferroelectric lattice polarization, which opens up many prospectives for electrically tunable and switchable spin electronic devices. By Mn doping of the {\alpha}-GeTe host lattice, the system becomes a multiferroic semiconductor possessing magnetoelectric properties in which the electric polarization, magnetization and spin texture are coupled to each other. Employing spin- and angle-resolved photoemission spectroscopy in bulk- and surface-sensitive energy ranges and by varying dipole transition matrix elements, we disentangle the bulk, surface and surface-resonance states of the electronic structure and determine the spin textures for selected parameters. From our results, we derive a comprehensive model of the {\alpha}-GeTe surface electronic structure which fits experimental data and first principle theoretical predictions and we discuss the unconventional evolution of the Rashba-type spin splitting upon manipulation by external B- and E-fields., Comment: 7 pages, 7 figures, 1 ancillary file

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 Fe$_{1+y}$Se$_x$Te$_{1-x}$ by tuning the Fermi energy, $\epsilon_F$, via chemical doping, which permits us to systematically change $\Delta / \epsilon_F$ from 0.16 to 0.5 were $\Delta$ 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.

One-dimensional (1D) electronic states were discovered on 1D surface atomic structure of Bi fabricated on semiconductor InSb(001) substrates by angle-resolved photoelectron spectroscopy (ARPES). The 1D state showed steep, Dirac-cone-like dispersion along the 1D atomic structure with a finite direct bandgap opening as large as 150 meV. Moreover, spin-resolved ARPES revealed the spin polarization of the 1D unoccupied states as well as that of the occupied states, the orientation of which inverted depending on the wave vector direction parallel to the 1D array on the surface. These results reveal that a spin-polarized quasi-1D carrier was realized on the surface of 1D Bi with highly efficient backscattering suppression, showing promise for use in future spintronic and energy-saving devices., Comment: 9 pages (4 figures for the main text, 7 for supplemental material). To be published in Physical Review Materials (Copyright is transferred to APS)

The interplay between electronic eigenstates, spin, and orbital degrees of freedom, combined with fundamental breaking of symmetries is currently one of the most exciting fields of research. Multiferroics such as (GeMn)Te fulfill these requirements providing unusual physical properties due to the coexistence and coupling between ferromagnetic and ferroelectric order in one and the same system. Here we show that multiferroic (GeMn)Te inherits from its parent ferroelectric {\alpha}-GeTe compound a giant Rashba splitting of three-dimensional bulk states which competes with the Zeeman spin splitting induced by the magnetic exchange interactions. The collinear alignment of ferroelectric and ferromagnetic polarization leads to an opening of a tunable Zeeman gap of up to 100 meV around the Dirac point of the Rashba bands, coupled with a change in spin texture by entanglement of magnetic and spin-orbit order. Through applications of magnetic fields, we demonstrate manipulation of spin- texture by spin resolved photoemission experiments, which is also expected for electric fields based on the multiferroic coupling. The control of spin helicity of the bands and its locking to ferromagnetic and ferroelectric order opens fascinating new avenues for highly multifunctional multiferroic Rashba devices suited for reprogrammable logic and/or nonvolatile memory applications., Comment: 10 pages, 4 figures

We study the effect of oxygen vacancies on the electronic structure of the model strongly correlated metal SrVO$_3$. By means of angle-resolved photoemission (ARPES) synchrotron experiments, we investigate the systematic effect of the UV dose on the measured spectra. We observe the onset of a spurious dose-dependent prominent peak at an energy range were the lower Hubbard band has been previously reported in this compound, raising questions on its previous interpretation. By a careful analysis of the dose dependent effects we succeed in disentangling the contributions coming from the oxygen vacancy states and from the lower Hubbard band. We obtain the intrinsic ARPES spectrum for the zero-vacancy limit, where a clear signal of a lower Hubbard band remains. We support our study by means of state-of-the-art ab initio calculations that include correlation effects and the presence of oxygen vacancies. Our results underscore the relevance of potential spurious states affecting ARPES experiments in correlated metals, which are associated to the ubiquitous oxygen vacancies as extensively reported in the context of a two-dimensional electron gas (2DEG) at the surface of insulating $d^0$ transition metal oxides., Comment: Manuscript + Supplemental Material, 12 pages, 9 figures

The electronic states of Au-induced atomic nanowires on Ge(001) (Au/Ge(001) NWs) have been investigated by angle-resolved photoelectron spectroscopy with linearly polarized light. We have found three electron pockets around $\bar{J}\bar{K}$, where the Fermi surfaces are closed in a surface Brillouin zone, indicating that the surface states of Au/Ge(001) NWs are two-dimensional whereas the atomic structure is one-dimensional. The two-dimensional metallic states exhibit remarkable suppression of the photoelectron intensity near a Fermi energy. This suppression can be explained by the correlation and localization effects in disordered metals, which is a deviation from a Fermi-liquid model., Comment: 5 pages, 4 figures

We present experimental results on the conversion of a spin current into a charge current by spin pumping into the Dirac cone with helical spin polarization of the elemental topological insulator (TI) {\alpha}-Sn[1-3]. By angle-resolved photoelectron spectroscopy (ARPES) we first confirm that the Dirac cone at the surface of {\alpha}-Sn (0 0 1) layers subsists after covering with Ag. Then we show that resonant spin pumping at room temperature from Fe through Ag into {\alpha}-Sn layers induces a lateral charge current that can be ascribed to the Inverse Edelstein Effect[4-5]. Our observation of an Inverse Edelstein Effect length[5-6] much longer than for Rashba interfaces[5-10] demonstrates the potential of the TI for 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 TI for spin to charge conversion and the conditions to reach it., Comment: 14 pages, 5 figures

We study the electronic structure of an ordered array of poly(para-phenylene) chains produced by surface-catalyzed dehalogenative polymerization of 1,4-dibromobenzene on copper (110). The quantization of unoccupied molecular states is measured as a function of oligomer length by scanning tunneling spectroscopy, with Fermi level crossings observed for chains longer than ten phenyl rings. Angle-resolved photoelectron spectroscopy reveals a graphene-like quasi one-dimensional valence band as well as a direct gap of 1.15 eV, as the conduction band is partially filled through adsorption on the surface. Tight-binding modelling and ab initio density functional theory calculations lead to a full description of the organic band-structure, including the k dispersion, the gap size and electron charge transfer mechanisms which drive the system into metallic behaviour. Therefore the entire band structure of a carbon-based conducting wire has been fully determined. This may be taken as a fingerprint of {\pi}-conjugation of surface organic frameworks., Comment: 20 pages, 5 figures

We report the existence of metallic two-dimensional electron gases (2DEGs) at the (001) and (101) surfaces of bulk-insulating TiO2 anatase due to local chemical doping by oxygen vacancies in the near-surface region. Using angle-resolved photoemission spectroscopy, we find that the electronic structure at both surfaces is composed of two occupied subbands of d_xy orbital character. While the Fermi surface observed at the (001) termination is isotropic, the 2DEG at the (101) termination is anisotropic and shows a charge carrier density three times larger than at the (001) surface. Moreover, we demonstrate that intense UV synchrotron radiation can alter the electronic structure and stoichiometry of the surface up to the complete disappearance of the 2DEG. These results open a route for the nano-engineering of confined electronic states, the control of their metallic or insulating nature, and the tailoring of their microscopic symmetry, using UV illumination at different surfaces of anatase., Comment: Article + Supplemental Material. See also the Synopsis @ Physics: http://physics.aps.org/synopsis-for/10.1103/PhysRevB.92.041106

We study with Angle Resolved PhotoElectron Spectroscopy (ARPES) the evolution of the electronic structure of Sr2IrO4, when holes or electrons are introduced, through Rh or La substitutions. At low dopings, the added carriers occupy the first available states, at bottom or top of the gap, revealing an anisotropic gap of 0.7eV in good agreement with STM measurements. At further doping, we observe a reduction of the gap and a transfer of spectral weight across the gap, although the quasiparticle weight remains very small. We discuss the origin of the in-gap spectral weight as a local distribution of gap values.

The research field of spintronics has sought, over the past 25 years and through several materials science tracks, a source of highly spin-polarized current at room temperature. Organic spinterfaces, which consist in an interface between a ferromagnetic metal and a molecule, represent the most promising track as demonstrated for a handful of interface candidates. How general is this effect? We deploy topographical and spectroscopic techniques to show that a strongly spin-polarized interface arises already between ferromagnetic cobalt and mere carbon atoms. Scanning tunneling microscopy and spectroscopy show how a dense semiconducting carbon film with a low band gap of about 0.4 eV is formed atop the metallic interface. Spin-resolved photoemission spectroscopy reveals a high degree of spin polarization at room temperature of carbon-induced interface states at the Fermi energy. From both our previous study of cobalt/phthalocyanine spinterfaces and present x-ray photoemission spectroscopy studies of the cobalt/carbon interface, we infer that these highly spin-polarized interface states arise mainly from sp2-bonded carbon atoms. We thus demonstrate the molecule-agnostic, generic nature of the spinterface formation.

We report the existence of confined electronic states at the (110) and (111) surfaces of SrTiO3. Using angle-resolved photoemission spectroscopy, we find that the corresponding Fermi surfaces, subband masses, and orbital ordering are different from the ones at the (001) surface of SrTiO3. This occurs because the crystallographic symmetries of the surface and sub-surface planes, and the electron effective masses along the confinement direction, influence the symmetry of the electronic structure and the orbital ordering of the t2g manifold. Remarkably, our analysis of the data also reveals that the carrier concentration and thickness are similar for all three surface orientations, despite their different polarities. The orientational tuning of the microscopic properties of two-dimensional electron states at the surface of SrTiO3 echoes the tailoring of macroscopic (e.g. transport) properties reported recently in LaAlO3/SrTiO3 (110) and (111) interfaces, and is promising for searching new types of 2D electronic states in correlated-electron oxides., Comment: Accepted for publication as a Letter in Physical Review Applied

We investigate with angle resolved photoelectron spectroscopy the change of the Fermi Surface (FS) and the main bands from the paramagnetic (PM) state to the antiferromagnetic (AFM) occurring below 72 K in Fe_{1.06}Te. The evolution is completely different from that observed in iron-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 PM state is very anomalous with a large pseudogap 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.

Using angle-resolved photoemission spectroscopy, we study the evolution of the number of carriers in Ba(Fe(1-x)Cox)2As2 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 at low Co contents and low temperatures 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.

We investigate the quasiperiodic crystal (LaS)1.196(VS2) by angle and time resolved photoemission spectroscopy. The dispersion of electronic states is in qualitative agreement with band structure calculated for the VS2 slab without the incommensurate distortion. Nonetheless, the spectra display a temperature dependent pseudogap instead of quasiparticles crossing. The sudden photoexcitation at 50 K induces a partial filling of the electronic pseudogap within less than 80 fs. The electronic energy flows into the lattice modes on a comparable timescale. We attribute this surprisingly short timescale to a very strong electron-phonon coupling to the incommensurate distortion. This result sheds light on the electronic localization arising in aperiodic structures and quasicrystals.

ARPES is a priori a technique of choice to measure the Fermi velocities vF in metals. In correlated systems, it is interesting to compare this experimental value to that obtained in band structure calculations, as deviations are usually taken as a good indicator of the presence of strong electronic correlations. Nevertheless, it is not always straightforward to extract vF from ARPES spectra. We study here the case of layered cobaltates, an interesting family of correlated metals. We compare the results obtained by standard methods, namely the fit of spectra at constant momentum k (energy distribution curve, EDC) or constant binding energy omega(momentum distribution curve, MDC). We find that the difference of vF between the two methods can be as large as a factor 2. The reliability of the 2 methods is intimately linked to the degree of k- and omega-dependence of the electronic self-energy. As the k-dependence is usually much smaller than the omega dependence for a correlated system, the MDC analysis is generally expected to give more reliable results. However, we review here several examples within cobaltates, where the MDC analysis apparently leads to unphysical results, while the EDC analysis appears coherent. We attribute the difference between the EDC and MDC analysis to a strong variation of the photoemission intensity with the momentum k. This distorts the MDC lineshapes but does not affect the EDC ones. Simulations including a k dependence of the intensity allow to reproduce the difference between MDC and EDC analysis very well. This momentum dependence could be of extrinsic or intrinsic. We argue that the latter is the most likely and actually contains valuable information on the nature of the correlations that would be interesting to extract further.

A blueprint for producing scalable digital graphene electronics has remained elusive. Current methods to produce semiconducting-metallic graphene networks all suffer from either stringent lithographic demands that prevent reproducibility, process-induced disorder in the graphene, or scalability issues. Using angle resolved photoemission, we have discovered a unique one dimensional metallic-semiconducting-metallic junction made entirely from graphene, and produced without chemical functionalization or finite size patterning. The junction is produced by taking advantage of the inherent, atomically ordered, substrate-graphene interaction when it is grown on SiC, in this case when graphene is forced to grow over patterned SiC steps. This scalable bottomup approach allows us to produce a semiconducting graphene strip whose width is precisely defined within a few graphene lattice constants, a level of precision entirely outside modern lithographic limits. The architecture demonstrated in this work is so robust that variations in the average electronic band structure of thousands of these patterned ribbons have little variation over length scales tens of microns long. The semiconducting graphene has a topologically defined few nanometer wide region with an energy gap greater than 0.5 eV in an otherwise continuous metallic graphene sheet. This work demonstrates how the graphene-substrate interaction can be used as a powerful tool to scalably modify graphene's electronic structure and opens a new direction in graphene electronics research., Comment: 11 pages, 7 figures

The design of large-scale electronic circuits that are entirely spintronics-driven requires a current source that is highly spin-polarised at and beyond room temperature, cheap to build, efficient at the nanoscale and straightforward to integrate with semiconductors. Yet despite research within several subfields spanning nearly two decades, this key building block is still lacking. We experimentally and theoretically show how the interface between Co and phthalocyanine molecules constitutes a promising candidate. 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 molecules's nitrogen pi orbitals, which substantiates an ab-initio theoretical description of highly spin-polarised charge conduction across the interface due to differing spinterface formation mechanims 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.

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 (SO) spitting. These strong deviations from the Rashba-like coupling cannot be treated in $\textbf{k}\cdot \textbf{p}$ perturbation theory. Instead, first principle calculations could accurately reproduce the experimental dispersion of the electronic states. Our analysis shows that the giant anisotropy of the SO splitting is due to a large out-of plane buckling of the spin and orbital texture., Comment: 5 pages, 4 figures

In all iron pnictides, the positions of the ligand alternatively above and below the Fe plane create 2 inequivalent Fe sites. This results in 10 Fe 3d bands in the electronic structure. However, they do not all have the same status for an ARPES experiment. There are interference effects between the 2 Fe that modulate strongly the intensity of the bands and that can even switch their parity. We give a simple description of these effects, notably showing that ARPES polarization selection rules in these systems cannot be applied by reference to a single Fe ion. We show that ARPES data for the electron pockets in Ba(Fe0.92Co0.08)2As2 are in excellent agreement with this model. We observe both the total suppression of some bands and the parity switching of some other bands. Once these effects are properly taken into account, the structure of the electron pockets, as measured by ARPES, becomes very clear and simple. By combining ARPES measurements in different experimental configurations, we clearly isolate each band forming one of the electron pockets. We identify a deep electron band along one ellipse axis with the dxy orbital and a shallow electron band along the perpendicular axis with the dxz/dyz orbitals, in good agreement with band structure calculations. We show that the electron pockets are warped as a function of kz as expected theoretically, but that they are much smaller than predicted by the calculation.

Gold intercalation between the buffer layer and a graphene monolayer of epitaxial graphene on SiC(0001) leads to the formation of quasi free standing small aggregates of clusters. Angle Resolved Photoemission Spectroscopy measurements reveal that these clusters preserve the linear dispersion of the graphene quasiparticles and surprisingly increase their Fermi velocity. They also strongly modify the band structure of graphene around the Van Hove singularities (VHs) by a strong extension without charge transfer. This result gives a new insight on the role of the intercalant in the renormalization of the bare electronic band structure of graphene usually observed in Graphite and Graphene Intercalation Compounds.

In this work we use LEEM, XPEEM and XPS to study how the excess Si at the graphene-vacuum interface reorders itself at high temperatures. We show that silicon deposited at room temperature onto multilayer graphene films grown on the SiC(000[`1]) rapidly diffuses to the graphene-SiC interface when heated to temperatures above 1020. In a sequence of depositions, we have been able to intercalate ~ 6 ML of Si into the graphene-SiC interface., Comment: 6 pages, 8 figures, submitted to PRB

We present a detailed comparison of the electronic structure of BaFe2As2 in its paramagnetic and antiferromagnetic (AFM) phases, through angle-resolved photoemission studies. Using different experimental geometries, we resolve the full elliptic shape of the electron pockets, including parts of dxy symmetry along its major axis that are usually missing. This allows us to define precisely how the hole and electron pockets are nested and how the different orbitals evolve at the transition. We conclude that the imperfect nesting between hole and electron pockets explains rather well the formation of gaps and residual metallic droplets in the AFM phase, provided the relative parity of the different bands is taken into account. Beyond this nesting picture, we observe shifts and splittings of numerous bands at the transition. We show that the splittings are surface sensitive and probably not a reliable signature of the magnetic order. On the other hand, the shifts indicate a significant redistribution of the orbital occupations at the transition, especially within the dxz/dyz system, which we discuss.

Despite many ARPES investigations of iron pnictides, the structure of the electron pockets is still poorly understood. By combining ARPES measurements in different experimental configurations, we clearly resolve their elliptic shape. Comparison with band calculation identify a deep electron band with the dxy orbital and a shallow electron band along the perpendicular ellipse axis with the dxz/dyz orbitals. We find that, for both electron and hole bands, the lifetimes associated with dxy are longer than for dxz/dyz. This suggests that the two types of orbitals play different roles in the electronic properties and that their relative weight is a key parameter to determine the ground state.

Graphene stacked in a Bernal configuration (60 degrees relative rotations between sheets) differs electronically from isolated graphene due to the broken symmetry introduced by interlayer bonds forming between only one of the two graphene unit cell atoms. A variety of experiments have shown that non-Bernal rotations restore this broken symmetry; consequently, these stacking varieties have been the subject of intensive theoretical interest. Most theories predict substantial changes in the band structure ranging from the development of a Van Hove singularity and an angle dependent electron localization that causes the Fermi velocity to go to zero as the relative rotation angle between sheets goes to zero. In this work we show by direct measurement that non-Bernal rotations preserve the graphene symmetry with only a small perturbation due to weak effective interlayer coupling. We detect neither a Van Hove singularity nor any significant change in the Fermi velocity. These results suggest significant problems in our current theoretical understanding of the origins of the band structure of this material., Comment: 7 pages, 6 figures, submitted to PRB

Similar to silicon that is the basis of conventional electronics, strontium titanate (SrTiO3) is the bedrock of the emerging field of oxide electronics. SrTiO3 is the preferred template to create exotic two-dimensional (2D) phases of electron matter at oxide interfaces, exhibiting metal-insulator transitions, superconductivity, or large negative magnetoresistance. However, the physical nature of the electronic structure underlying these 2D electron gases (2DEGs) remains elusive, although its determination is crucial to understand their remarkable properties. Here we show, using angle-resolved photoemission spectroscopy (ARPES), that there is a highly metallic universal 2DEG at the vacuum-cleaved surface of SrTiO3, independent of bulk carrier densities over more than seven decades, including the undoped insulating material. This 2DEG is confined within a region of ~5 unit cells with a sheet carrier density of ~0.35 electrons per a^2 (a is the cubic lattice parameter). We unveil a remarkable electronic structure consisting on multiple subbands of heavy and light electrons. The similarity of this 2DEG with those reported in SrTiO3-based heterostructures and field-effect transistors suggests that different forms of electron confinement at the surface of SrTiO3 lead to essentially the same 2DEG. Our discovery provides a model system for the study of the electronic structure of 2DEGs in SrTiO3-based devices, and a novel route to generate 2DEGs at surfaces of transition-metal oxides., Comment: 28 pages, 9 figures

We study with ARPES the electronic structure of CoO2 slabs, stacked with rock-salt (RS) layers exhibiting a different (misfit) periodicity. Fermi Surfaces (FS) in phases with different doping and/or periodicities reveal the influence of the RS potential on the electronic structure. We show that these RS potentials are well ordered, even in incommensurate phases, where STM images reveal broad stripes with width as large as 80\AA. The anomalous evolution of the FS area at low dopings is consistent with the localization of a fraction of the electrons. We propose that this is a new form of electronic ordering, induced by the potential of the stacked layers (RS or Na in NaxCoO2) when the FS becomes smaller than the Brillouin Zone of the stacked structure.

Previous ARPES 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 the quasiparticle weight Z, which turns out to be very small 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.

We present a detailed investigation of Ba(Fe0.65Ru0.35)2As2 by transport measurements and Angle Resolved photoemission spectroscopy. We observe that Fe and Ru orbitals hybridize to form a coherent electronic structure and that Ru does not induce doping. The number of holes and electrons, deduced from the area of the Fermi Surface pockets, are both about twice larger than in BaFe2As2. The contribution of both carriers to the transport is evidenced by a change of sign of the Hall coefficient with decreasing temperature. Fermi velocities increase significantly with respect to BaFe2As2, suggesting a significant reduction of correlation effects. This may be a key to understand the appearance of superconductivity at the expense of magnetism in undoped iron pnictides.