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Mo$_8$O$_{23}$ is a low-dimensional chemically robust transition metal oxide coming from a prospective family of functional materials, MoO$_{3-x}$, ranging from a wide gap insulator $(x=0)$ to a metal $(x=1)$. The large number of stoichometric compounds with intermediate $x$ have widely different properties. In Mo$_8$O$_{23}$, an unusual charge density wave transition has been suggested to occur above room temperature, but its low temperature behaviour is particularly enigmatic. We present a comprehensive experimental study of the electronic structure associated with various ordering phenomena in this compound, complemented by theory. Density-functional theory (DFT) calculations reveal a cross-over from a semi-metal with vanishing band overlap to narrow-gap semiconductor behaviour with decreasing temperature. A buried Dirac crossing at the zone boundary is confirmed by angle-resolved photoemission spectroscopy (ARPES). Tunnelling spectroscopy (STS) reveals a gradual gap opening corresponding to a metal-to-insulator transition at 343 K in resistivity, consistent with CDW formation and DFT results, but with large non-thermal smearing of the spectra implying strong carrier scattering. At low temperatures, the CDW picture is negated by the observation of a metallic Hall contribution, a non-trivial gap structure in STS below $\sim 170$ K and ARPES spectra, that together represent evidence for the onset of the correlated state at $70$ K and the rapid increase of gap size below $\sim 30$ K. The intricate interplay between electronic correlations and the presence of multiple narrow bands near the Fermi level set the stage for metastability and suggest suitability for memristor applications., Comment: 13 pages, 6 figures, pre-print of an article published in Scientific Reports. The final authenticated version is available online at http://dx.doi.org/10.1038/s41598-019-52231-4

Trigonal tellurium, a small-gap semiconductor with pronounced magneto-electric and magneto-optical responses, is among the simplest realizations of a chiral crystal. We have studied by spin- and angle-resolved photoelectron spectroscopy its unconventional electronic structure and unique spin texture. We identify Kramers-Weyl, composite, and accordionlike Weyl fermions, so far only predicted by theory, and show that the spin polarization is parallel to the wave vector along the lines in k space connecting high-symmetry points. Our results clarify the symmetries that enforce such spin texture in a chiral crystal, thus bringing new insight in the formation of a spin vectorial field more complex than the previously proposed hedgehog configuration. Our findings thus pave the way to a classification scheme for these exotic spin textures and their search in chiral crystals.

Metal monochalcogenides $(MX)$ have recently been rediscovered as two-dimensional materials with electronic properties highly dependent on the number of layers. Although some intriguing properties appear in the few-layer regime, the carrier mobility of $MX$ compounds increases with the number of layers, motivating the interest in multilayered heterostructures or bulk materials. By means of angle-resolved photoemission spectroscopy (ARPES) measurements and density functional theory calculations, we compare the electronic band structure of bulk $\ensuremath{\epsilon}\text{\ensuremath{-}}\mathrm{GaSe}$ and $\ensuremath{\epsilon}$-InSe semiconductors. We focus our attention on the top valence band of the two compounds along main symmetry directions, discussing the effect of spin-orbit coupling and contributions from post-transition-metal (Ga or In) and Se atoms. Our results show that the top valence band at $\mathrm{\ensuremath{\Gamma}}$ point is dominated by Se ${p}_{z}$ states, while the main effect of Ga or In appears more deeply in binding energy, at the Brillouin zone corners, and in the conduction band. These findings explain also the experimental observation of a hole effective mass rather insensitive to the post-transition metal. Finally, by means of spin-resolved ARPES and surface band structure calculations we describe Rashba-Bychkov spin splitting of surface states in $\ensuremath{\epsilon}\text{\ensuremath{-}}\mathrm{InSe}$.

In nodal-line semimetals linearly dispersing states form Dirac loops in the reciprocal space, with high degree of electron-hole symmetry and almost-vanishing density of states near the Fermi level. The result is reduced electronic screening and enhanced correlations between Dirac quasiparticles. Here we investigate the electronic structure of ZrSiSe, by combining time- and angle-resolved photoelectron spectroscopy with ab initio density functional theory (DFT) complemented by an extended Hubbard model (DFT +U +V). We show that electronic correlations are reduced on an ultrashort timescale by optical excitation of high-energy electrons-hole pairs, which transiently screen the Coulomb interaction. Our findings demonstrate an all-optical method for engineering the band structure of a quantum material., Comment: 6 pages, 3 figures

Anatase TiO2 is among the most studied materials for light-energy conversion applications, but the nature of its fundamental charge excitations is still unknown. Yet it is crucial to establish whether light absorption creates uncorrelated electron-hole pairs or bound excitons and, in the latter case, to determine their character. Here, by combining steady-state angle-resolved photoemission spectroscopy and spectroscopic ellipsometry with state-of-the-art ab initio calculations, we demonstrate that the direct optical gap of single crystals is dominated by a strongly bound exciton rising over the continuum of indirect interband transitions. This exciton possesses an intermediate character between the Wannier-Mott and Frenkel regimes and displays a peculiar two-dimensional wavefunction in the three-dimensional lattice. The nature of the higher-energy excitations is also identified. The universal validity of our results is confirmed up to room temperature by observing the same elementary excitations in defect-rich samples (doped single crystals and nanoparticles) via ultrafast two-dimensional deep-ultraviolet spectroscopy.Here the authors combine steady-state angle-resolved photoemission spectroscopy, ellipsometry and ultrafast two-dimensional ultraviolet spectroscopy to examine the role of many-body correlations in anatase TiO2, revealing the existence of strongly bound excitons in single crystals and nanoparticles.

We present a comprehensive angle-resolved photoemission spectroscopy study of Ca1.8Sr0.2RuO4. Four distinct bands are revealed and along the Ru-O bond direction their orbital characters are identif ...

In materials with nearly commensurate band filling the electron liquid may spontaneously separate into components with distinct properties, yielding complex intra- and interunit cell ordering patterns and a reduced dimensionality. Polarization-dependent angle-resolved photoemission data with submicron spatial resolution demonstrate such an electronic self-organization in NbSe3, a compound considered to be a paradigm of charge order. The new data indicate the emergence of a novel order, and reveal the one-dimensional (1D) physics hidden in a material which naively could be considered the most three dimensional of all columnar chalcogenides. The 1D physics is evidenced by a new selection rule—in two polarizations we observe two strikingly different dispersions each closely resembling apparently contradicting results of previous studies of this material., The work at Lausanne and Geneva is supported by the Swiss NSF. M.A.V. acknowledges financial support from Spanish MICIN Postdoctoral Mobility Program. S.P. acknowledges C’NANO Ile-de-France, DIM NanoK, for the support of the Nanospecs project. Work in Spain was supported by a MINECO (Grants FIS2015-64886-C5-4-P and CTQ2015-64579-C3-3-P), Generalitat de Catalunya (2017SGR1506 and 2017SGR1289), and XRQTC. E.C. acknowledges support from MINECO through the Severo Ochoa Centers of Excellence Program under Grant No. SEV-2015-0496. ICN2 is funded by the CERCA Program/ Generalitat de Catalunya, and supported by the Severo Ochoa program from Spanish MINECO (Grant No. SEV- 2017-0706). P.A. acknowledges support from the Maria de Maeztu Units of Excellence Program under Grant MDM- 2017-0767. S.C. gratefully acknowledges the Becas Chile program (CONICYT PAI/INDUSTRIA 72090772) for a doctoral grant at the Universitat de Barcelona. Synchrotron SOLEIL is supported by the Centre National de la Recherche Scientifique (CNRS) and the Commissariat à l’Energie Atomique et aux energies Alternatives (CEA).

BaTiO${}_{3}$ (BTO) is one of the most important ferroelectric oxides. Its most common source of uncontrolled doping, the oxygen vacancy, releases free electrons that confine in a two-dimensional electron gas (2DEG) at the surface. This 2DEG can be readily monitored by angle-resolved photoemission, and be used to measure the defect dynamics in ultrathin BTO films. The authors reveal two remarkable properties: first, oxygen defects close to the thin film surface are preferably in a charge state of 2+, which limits charge carrier trapping. Second, these defects migrate even below room temperature, fostering significant surface charge carrier density fluctuations that ultimately quench the 2DEG.

Resonant inelastic X-ray scattering (RIXS) experiments performed at the oxygen-$K$ edge on the iridate perovskites {\SIOS} and {\SION} reveal a sequence of well-defined dispersive modes over the energy range up to $\sim 0.8$ eV. The momentum dependence of these modes and their variation with the experimental geometry allows us to assign each of them to specific collective magnetic and/or electronic excitation processes, including single and bi-magnons, and spin-orbit and electron-hole excitons. We thus demonstrated that dispersive magnetic and electronic excitations are observable at the O-$K$ edge in the presence of the strong spin-orbit coupling in the $5d$ shell of iridium and strong hybridization between Ir $5d$ and O $2p$ orbitals, which confirm and expand theoretical expectations. More generally, our results establish the utility of O-$K$ edge RIXS for studying the collective excitations in a range of $5d$ materials that are attracting increasing attention due to their novel magnetic and electronic properties. Especially, the strong RIXS response at O-$K$ edge opens up the opportunity for investigating collective excitations in thin films and heterostructures fabricated from these materials., Comment: 6 pages, 4 figures with supplementary material. Accepted by PRB Rapid Communications

We present a study of the resonant inelastic scattering response of \ybin\ excited at the tender Yb $M_5$ X-ray edge. In the high-temperature, paramagnetic phase, we observe a multiplet structure which can be understood at an ionic level. Upon cooling through the valence transition at $T_v\sim$ 40$K$, we observe a strong renormalization of the low-energy spectra, indicating a sensitivity to the formation of an intermediate valence phase at low temperatures. Similar spectrum renormalization has been observed in the optical conductivity, which suggests that the low-energy electronic structure possesses both mixed conduction and localized character., 8 pages, 5 figures; submitted, Phys. Rev. B

We use resonant inelastic x-ray scattering (RIXS) at the Cu L3 edge to measure the charge and spin excitations in the “half-stuffed” Cu-O planes of the cuprate antiferromagnet Ba2Cu3O4Cl2. The RIXS line shape reveals distinct contributions to the dd excitations from the two structurally inequivalent Cu sites, which have different out-of-plane coordinations. The low-energy response exhibits magnetic excitations. We find a spin-wave branch whose dispersion follows the symmetry of a CuO2 sublattice, similar to the case of the “fully stuffed” planes of tetragonal CuO (T-CuO). Its bandwidth is closer to that of a typical cuprate material, such as Sr2CuO2Cl2, than it is to that of T-CuO. We interpret this result as arising from the absence of the effective four-spin inter-sublattice interactions that act to reduce the bandwidth in T-CuO.

The prediction of Weyl fermions in the low-temperature noncentrosymmetric $1{T}^{\ensuremath{'}}$ phase of ${\mathrm{MoTe}}_{2}$ still awaits clear experimental confirmation. Here, we report angle-resolved photoemission (ARPES) data and ab initio calculations that reveal a surface state arc dispersing between the valence and the conduction band, as expected for a Weyl semimetal. However, we find that the arc survives in the high-temperature centrosymmetric $1{T}^{\ensuremath{'}\ensuremath{'}}$ phase. Therefore, a surface Fermi arc is not an unambiguous fingerprint of a topologically nontrivial phase. We have also investigated the surface state spin texture of the $1{T}^{\ensuremath{'}}$ phase by spin-resolved ARPES, and identified additional topologically trivial spin-split states within the projected band gap at higher binding energies.

A paradigmatic case of multi-band Mott physics including spin-orbit and Hund's coupling is realized in Ca2RuO4. Progress in understanding the nature of this Mott insulating phase has been impeded by the lack of knowledge about the low-energy electronic structure. Here we provide—using angle-resolved photoemission electron spectroscopy—the band structure of the paramagnetic insulating phase of Ca2RuO4 and show how it features several distinct energy scales. Comparison to a simple analysis of atomic multiplets provides a quantitative estimate of the Hund's coupling J=0.4 eV. Furthermore, the experimental spectra are in good agreement with electronic structure calculations performed with Dynamical Mean-Field Theory. The crystal field stabilization of the dxy orbital due to c-axis contraction is shown to be essential to explain the insulating phase. These results underscore the importance of multi-band physics, Coulomb interaction and Hund's coupling that together generate the Mott insulating state of Ca2RuO4., Detailed knowledge of the low-energy electronic structure is required to understand the Mott insulating phase of Ca2RuO4. Here, Sutter et al. provide directly the experimental band structure of the paramagnetic insulating phase of Ca2RuO4 and unveil the electronic origin of its Mott phase.

Physical review / B 96(24), 241408 (2017). doi:10.1103/PhysRevB.96.241408, $MoTe_2$ has recently been shown to realize in its low-temperature phase the type-II Weyl semimetal (WSM). We investigated by time- and angle- resolved photoelectron spectroscopy (tr-ARPES) the possible influence of the Weyl points on the electron dynamics above the Fermi level $E_F$, by comparing the ultrafast response of $MoTe_2$in the trivial and topological phases. In the low-temperature WSM phase, we report an enhanced relaxation rate of electrons optically excited to the conduction band, which we interpret as a fingerprint of the local gap closure when Weyl points form. By contrast, we find that the electron dynamics of the related compound $WTe_2$is slower and temperature independent, consistent with a topologically trivial nature of this material. Our results shows that tr-ARPES is sensitive to the small modifications of the unoccupied band structure accompanying the structural and topological phase transition of $MoTe_2$., Published by Inst., Woodbury, NY

The manipulation of the electronic properties of solids by light is an exciting goal, which requires knowledge of the electronic structure with energy, momentum and temporal resolution. Time- and angle-resolved photoemission spectroscopy (tr-ARPES) is the most direct probe of the effects of an optical excitation on the band structure of a material. In particular, tr-ARPES in the extreme ultraviolet (VUV) range gives access to the ultrafast dynamics over the entire Brillouin zone. VUV tr-ARPES experiments can now be performed at the ASTRA (ARPES Spectrometer for Time-Resolved Applications) end station of Harmonium, at LACUS. Its capabilities are illustrated by measurements of the ultrafast electronic response of ZrSiTe, a novel topological semimetal characterized by linearly dispersing states located at the Brillouin zone boundary.

With its tunable band-gap and its unique optical and electronic properties black phosphorus (BP) opens exciting opportunities for optoelectronic nanotechnology. The band-gap extends from the visible to the mid-infrared spectral range, as a function of sample thickness and external parameters such as electric field and pressure. This, combined with the saturable absorption and in-plane anisotropic optical properties, makes BP a versatile platform for realizing polarization-sensitive photodetectors and absorbers. Although its near-equilibrium properties have been intensively studied, the development of efficient ultrafast optical devices requires detailed knowledge of the temporal dynamics of the photoexcited hot-carriers. Here we address the electronic response of BP to an ultrafast laser excitation, by means of time-and angle-resolved photoelectron spectroscopy. Following the optical excitation, we directly observe a shift of the valence band (VB) position, indicative of band-gap renormalization (BGR). Our data also show that the hole population in the VB relaxes with a characteristic time tau(VB) = 10.2 +/- 1.0 ps, while the lifetime of the electrons accumulated at the minimum of the conduction band is tau(CB) = 1.9 +/- 0.2 ps. The experimental results are well reproduced by ab initio calculations of the out-of-equilibrium electronic properties. Our study sets the reference for the ultrafast carrier dynamics in BP and demonstrates the material's ultrafast BGR, which is promising for optoelectronic switches.

Long known for its peculiar resistivity, showing a thus far unexplained anomalous peak as a function of temperature, ZrTe5 has recently received rising attention in a somewhat different context. While both theoretical and experimental results seem to point to a nontrivial topology of the low-energy electronic states, there is no agreement on the nature of their topological character. Here, by an angle-resolved photoemission study of the evolution of the band structure with temperature and surface doping, we show that (i) the material presents a van Hove singularity close to the Fermi level, and (ii) no surface states exist at the (010) surface. These findings reconcile band structure measurements with transport results and establish the topology of this puzzling compound.

Bilayer graphene is a highly promising material for electronic and optoelectronic applications since it is supporting massive Dirac fermions with a tuneable band gap. However, no consistent picture of the gap's effect on the optical and transport behavior has emerged so far, and it has been proposed that the insulating nature of the gap could be compromised by unavoidable structural defects, by topological in-gap states, or that the electronic structure could be altogether changed by many-body effects. Here we directly follow the excited carriers in bilayer graphene on a femtosecond time scale, using ultrafast time- and angle-resolved photoemission. We find a behavior consistent with a single-particle band gap. Compared to monolayer graphene, the existence of this band gap leads to an increased carrier lifetime in the minimum of the lowest conduction band. This is in sharp contrast to the second sub-state of the conduction band, in which the excited electrons decay through fast, phonon-assisted inter-band transitions., Comment: 5 pages, 4 figures

We measured high resolution Cu $L_3$ edge resonant inelastic x-ray scattering (RIXS) of the undoped cuprates La$_2$CuO$_4$, Sr$_2$CuO$_2$Cl$_2$, CaCuO$_2$ and NdBa$_2$Cu$_3$O$_6$. The dominant spectral features were assigned to $dd$ excitations and we extensively studied their polarization and scattering geometry dependence. In a pure ionic picture, we calculated the theoretical cross sections for those excitations and used them to fit the experimental data with excellent agreement. By doing so, we were able to determine the energy and symmetry of Cu-3$d$ states for the four systems with unprecedented accuracy and confidence. The values of the effective parameters could be obtained for the single ion crystal field model but not for a simple two-dimensional cluster model. The firm experimental assessment of $dd$ excitation energies carries important consequences for the physics of high $T_c$ superconductors. On one hand, having found that the minimum energy of orbital excitation is always $\geq 1.4$ eV, i.e., well above the mid-infrared spectral range, leaves to magnetic excitations (up to 300 meV) a major role in Cooper pairing in cuprates. On the other hand, it has become possible to study quantitatively the effective influence of $dd$ excitations on the superconducting gap in cuprates., 22 pages, 11 figures, 1 table

We discuss two different approaches for tuning the giant spin-orbit splitting of a BiAg2 surface alloy. The first approach consists of electron doping by alkaline metal deposition in order to shift the energy position of the spin-split surface states, while the second is based on the novel Si(1 1 1)-Ag-BiAg2 trilayer system. In both cases the spin-polarized structure near the Fermi level can be controlled by an external parameter, while the second approach permits coupling the concept of giant spin-splitting with a semiconducting substrate. (C) 2010 Elsevier B.V. All rights reserved.

Resonant inelastic x-ray scattering in the soft x-ray regime has been profiting much from technical advances that have lowered considerably the instru- mental linewidth. At the ADRESS beam line of the Swiss Light Source the SAXES spectrometer can be used to measure RIXS spectra at the L edges of the 3d transition metals with unprecedented energy resolution, of the order of 100 meV for Mn, Ni and Cu. We present here some preliminary spectra on CuO, malachite, NiO, NiCl2, MnO and LaMnO3. The dd excitations are very well resolved allowing accurate experimental evaluation of 3d state energy splitting. The low energy scale becomes accessible opening the way to the study of collective excitations in strongly correlated electron systems, like magnons and orbitons.

We present Angle-Resolved Photoelectron Spectroscopy (ARPES) data on spin-orbit split states in two XAg2 surface alloys grown on an Ag(111) substrate, and of the Si(111)-AgBiAg2 trilayer system. We briefly discuss the origin of the unusually large energy and momentum splitting, and the possibility of tuning by surface engineering the spin polarization at the Fermi level. [DOI: 10.1380/ejssnt.2009.264]

We report an investigation of the structural and electronic properties of a Pb monolayer (ML) grown on Ag(1 0 0), by combining x-ray photoelectron diffraction (XPD) and angle resolved photoelectron spectroscopy (ARPES). The Pb atoms are found to arrange in a pseudo-hexagonal adlayer commensurate to the underlying square Ag substrate, resulting in a coincidence cell with c( ##IMG## [http://ej.iop.org/images/0953-8984/27/45/455502/cmaa0562ieqn001.gif] $6times 2$ ) periodicity. The electronic structure of the Pb ML in proximity of the Fermi level consists in three p -derived bands, which show different degrees of hybridization with the substrate for their different orbital characters. In particular, we report that the p xy states disperse without forming energy gap, in contrast to previous ARPES studies of the Pb ML on different metallic substrates. We attribute the absence of energy gap to the commensurability between substrate and adlayer, resulting in a higher two-dimensionality of the Pb ML.

The dynamics of excited electrons and holes in single layer (SL) MoS$_2$ have so far been difficult to disentangle from the excitons that dominate the optical response of this material. Here, we use time- and angle-resolved photoemission spectroscopy for a SL of MoS$_2$ on a metallic substrate to directly measure the excited free carriers. This allows us to ascertain a direct quasiparticle band gap of 1.95 eV and determine an ultrafast (50 fs) extraction of excited free carriers via the metal in contact with the SL MoS$_2$. This process is of key importance for optoelectronic applications that rely on separated free carriers rather than excitons., 15 pages, 4 Figures. To appear in Nano Letters, 2015

We investigate the polaronic ground state of anatase TiO2 by bulk-sensitive resonant inelastic x-ray spectroscopy (RIXS) at the Ti L3 edge. We find that the formation of the polaron cloud involves a single 95 meV phonon along the c axis, in addition to the 108 meV ab-plane mode previously identified by photoemission. The coupling strength to both modes is the same within error bars, and it is unaffected by the carrier density. These data establish RIXS as a directional bulk-sensitive probe of electron-phonon coupling in solids.

We investigate the composition and temperature (10-450 K) dependence of the Yb valence in YbMn6Ge6-xSnx (x = 0.0, 3.8, 4.2, 4.4, and 5.5) using resonant inelastic x-ray scattering (RIXS). The observed change in the Yb valence with composition (from v similar to 3 for x = 0 to v similar to 2.7 for x = 5.5) is likely driven by negative chemical pressure effects due to the Sn for Ge substitution. While Yb is nonmagnetic in YbMn6Ge0.5Sn5.5, intermediate valent Yb magnetically orders at unexpectedly high temperature (up to 90 K) in the alloys with x = 3.8, 4.2, and 4.4. The three latter alloys further exhibit an increase in the Yb valence upon cooling, which is opposite to the usual behavior. Interactions with the magnetically ordered Mn sublattice are invoked to account for these unprecedented phenomena through a simplified model based on an Anderson Hamiltonian with a Zeeman term mimicking the Mn-Yb exchange interactions. We further show that the Yb magnetic behavior in this series can be interpreted based on Doniach's picture. Compared with standard intermediate valent materials where Yb is embedded in a nonmagnetic matrix, the strong Mn-Yb exchange interaction enhances the intermediate valent Yb magnetic ordering temperature and allows for extending the stability domain of the Yb magnetic order towards lower Yb valence.

The ultrafast dynamics of excited carriers in graphene is closely linked to the Dirac spectrum and playsa central role for many electronic and optoelectronic applications. Harvesting energy from excitedelectron-hole pairs, for instance, is only possible if these pairs can be separated before they lose energyto vibrations, merely heating the lattice. Until now, the hot carrier dynamics in graphene could only beaccessed indirectly. Here, we present a dynamical view on the Dirac cone by time- and angle-resolvedphotoemission spectroscopy. This allows us to show the quasi-instant thermalization of the electron gas toa temperature of 2000 K, to determine the time-resolved carrier density, and to disentangle the subsequentdecay into excitations of optical phonons and acoustic phonons (directly and via supercollisions).

We investigate the evolution of both the occupied and unoccupied electronic structure in representative compounds of the infinitely adaptive superlattice series (Sb2)m−Sb2Te3 (m=0–3) by means of angle-resolved photoemission spectroscopy and time-delayed two-photon photoemission, combined with first-principles band-structure calculations. We discover that the topological nature of the surface states and their spin texture are robust, with dispersions evolving from linear (Dirac-like) to parabolic (Rashba-like) along the series, as the materials evolve from semiconductors to semimetals. Our findings provide a promising strategy for engineering the topological states with the desired flexibility needed for realizing different quantum phenomena and spintronics applications.

High-resolution resonant inelastic x-ray scattering (RIXS) at the oxygen K edge has been used to study the orbital excitations of Ca2RuO4 and Sr2RuO4. In combination with linear dichroism x-ray absorption spectroscopy, the ruthenium 4d-orbital occupation and excitations were probed through their hybridization with the oxygen p orbitals. These results are described within a minimal model, taking into account crystal field splitting and a spin-orbit coupling λso=200 meV. The effects of spin-orbit interaction on the electronic structure and implications for the Mott and superconducting ground states of (Ca,Sr)2RuO4 are discussed.

The prospect of optically inducing and controlling a spin-polarized current in spintronic devices has generated wide interest in the out-of-equilibrium electronic and spin structure of topological insulators. In this Letter we show that only measuring the spin intensity signal over several orders of magnitude by spin-, time-, and angle-resolved photoemission spectroscopy can provide a comprehensive description of the optically excited electronic states in Bi2Se3. Our experiments reveal the existence of a surface resonance state in the second bulk band gap that is benchmarked by fully relativistic ab initio spin- resolved photoemission calculations. We propose that the newly reported state plays a major role in the ultrafast dynamics of the system, acting as a bottleneck for the interaction between the topologically protected surface state and the bulk conduction band. In fact, the spin- polarization dynamics in momentum space show that these states display macroscopically different temperatures and, more importantly, different cooling rates over several picoseconds.

Time- and angle-resolved photoemission measurements on two doped graphene samples displaying different doping levels reveal remarkable differences in the ultrafast dynamics of the hot carriers in the Dirac cone. In the more strongly ($n$-)doped graphene, we observe larger carrier multiplication factors ($>$ 3) and a significantly faster phonon-mediated cooling of the carriers back to equilibrium compared to in the less ($p$-)doped graphene. These results suggest that a careful tuning of the doping level allows for an effective manipulation of graphene's dynamical response to a photoexcitation., 17 pages, 3 figures

We present an overview of the new family of semiconductors BiTeX (X = I, Br, Cl) from the perspective of angle resolved photoemission spectroscopy. The strong band bending occurring at the surface potentially endows them with a large flexibility, as they are capable of hosting both hole and electron conduction, and can be modified by inclusion or adsorption of foreign atoms. In addition, their trigonal crystal structure lacks a center of symmetry and allows for both bulk and surface spin-split bands at the Fermi level. We elucidate analogies and differences among the three materials, also in the light of recent theoretical and experimental work.

We present ultraviolet photoelectron spectroscopy studies on alkali metal-intercalated thin films of electroluminescent p-sexiphenyl (6P) and the organic hole transporting material N,N'-bis-(1-naphthyl)-N,N'-diphenyll-1,1-biphenyl1-4,4'-diamine (alpha-NPD). The formation of new occupied electronic states in the otherwise empty energy gap of 6P and alpha-NPD is observed, accompanied by a significant shift of the Fermi-level. Depending on the work function phi of the substrate used for the organic thin films, we observe two different scenarios at low intercalation levels: the new electronic states are observed at (and even above) E-F for high phi substrates, whereas they are observed below E-F for low phi substrates. At high intercalation levels, all the states are observed below E-F. The observation of states at and above E-F is attributed to a lack of thermodynamic equilibrium across the organic thin film. (c) 2005 Elsevier B.V. All rights reserved.

We discuss the spectral signatures of strong electronic correlations and electron-phonon interactions in two representative low-dimensional systems. In the 2D compound 1T-TaSe2 a charge-density-wave (CDW) induces a narrowing of the conduction band, which triggers a surface metal-insulator (M-I) transition and the disappearance of the quasiparticle (QP) features. In the 1D blue bronze K0.3MoO3 strong interaction with the lattice lead to pseudogapped polaronic lineshapes, and the large mass renormalization masks the signatures of electronic correlations. (C) 2004 Elsevier B.V All rights reserved.

With the advent of the very intense 3rd generation synchrotron sources of X rays, new powerful spectroscopic techniques, requiring the detection of very low cross section phenomena, have come of age. Among them Resonant Inelastic X-Ray Scattering (RIXS) is rapidly becoming a major probe of the electronic structure of solids. RIXS measures the decay radiation that follows the excitation of core electrons into states located in a narrow region above the Fermi level. It shares with other core-level spectroscopies a remarkable chemical sensitivity and provides specific information on selected elements in a compound. Since photons are used to excite the process and photons are detected, truly bulk-sensitive information can be obtained. RIXS is sensitive to the nature of the ground state and of the characteristic excitations of a material, and can separately measure their energies, because exciting atoms with different atomic configuration leaves the solid in final states of different total energy. Therefore, it can discriminate different chemical environments and valence states of the same element. In this paper, we outline the basic principles of RIXS, with special emphasis on electronic excitations, and discuss the relevance of this information for studies of hybridization and valence in materials science, by referring to recent experiments.

We exploited angle-resolved photoemission (ARPES) to investigate the nature of the elementary quasiparticle (QP) excitations in selected low-dimensional compounds. In the model quasi two-dimensional conductor TiTe2, we observe spectral lineshapes which are consistent with a Fermi liquid (FL) scenario, and the usual QP scattering mechanisms. In contrast, in typical quasi one-dimensional Peierls systems like TTF-TCNQ, (TaSe4)(2)I and K0.3MoO3 we find clear non-FL lineshapes. We briefly discuss the possible origins of these unusual properties. (C) 2002 Elsevier Science B.V. All rights reserved.

Intermediate valence is one of the typical phenomena of systems with strong electronic correlation. The Anderson impurity model predicts a scaling of the valence with the reduced temperature T/T(K), which is difficult to observe by traditional surface-sensitive electronic spectroscopies. This paper presents results obtained by resonant inelastic X-ray scattering (RIXS), a bulk-sensitive configuration- and chemical-specific technique. The temperature dependence of the valence of YbInCu(4) and YbAgCu(4) was measured by tuning the incident energy to the resonance of the Yb(2+) spectral component. In the case of YbInCu(4) a sharp valence transition, as known from thermodynamical measurements, has been found. The valence of YbAgCu(4) reveals a smooth dependence consistent with a Kondo temperature T(K) = 70 K. These findings establish RIXS as a powerful tool for measuring bulk electronic properties of solids.

The influence of dimensionality on the electronic properties of layered perovskite materials remains an outstanding issue. We address it here for Sr3Ir2O7, the bilayer compound of the iridate Srn+1IrnO3n+1 series. By angle-resolved photoemission spectroscopy we show that in this material the interlayer coupling is large and that the intercell coupling is, conversely, negligible. From a detailed mapping of the bilayer splitting, and from the intensity modulation of the bonding and antibonding bands with photon energy, we establish differences and similarities with the prominent case of the bilayer superconducting cuprates.

Nodal angle-resolved photoemission spectra taken on overdoped La1.77Sr0.23CuO4 are presented and analyzed. It is proven that the low-energy excitations are true Landau Fermi-liquid quasiparticles. We show that momentum and energy distribution curves can be analyzed self-consistently without quantitative knowledge of the bare band dispersion. Finally, by imposing Kramers-Kronig consistency on the self-energy Sigma, insight into the quasiparticle residue is gained. We conclude by comparing our results to quasiparticle properties extracted from thermodynamic, magnetoresistance, and high-field quantum oscillation experiments on overdoped Tl2Ba2CuO6+delta.

Bulk Rashba systems BiTeX (X = I, Br, Cl) are emerging as important candidates for developing spintronics devices because of the coexistence of spin-split bulk and surface states, along with the ambipolar character of the surface charge carriers. The need to study the spin texture of strongly spin-orbit-coupled materials has recently promoted circular dichroic angular resolved photoelectron spectroscopy (CD-ARPES) as an indirect tool to measure the spin and the angular degrees of freedom. Here we report a detailed photon-energy-dependent study of the CD-ARPES spectra in BiTeX (X = I, Br, Cl). Our work reveals a large variation in the magnitude and sign of the dichroism. Interestingly, we find that the dichroic signal modulates differently for the three compounds and for the different spin-split states. These findings show a momentum and photon-energy dependence for the CD-ARPES signals in the bulk Rashba semiconductor BiTeX (X = I, Br, Cl). Finally, the outcome of our experiment indicates the important relation between the modulation of the dichroism and the phase differences between the wave functions involved in the photoemission process. This phase difference can be due to initial- or final-state effects. In the former case the phase difference results in possible interference effects among the photoelectrons emitted from different atomic layers and characterized by entangled spin-orbital polarized bands. In the latter case the phase difference results from the relative phases of the expansion of the final state in different outgoing partial waves.

We investigate the consequences of broken translational symmetry in the superconductor FeSexTe1�x using angle-resolved photoemission spectroscopy. We find that the intensity does not follow the periodicity dictated by the crystal structure, owing to the form of the perturbing potential and the symmetries of the Fe d orbitals. Their interplay leads to substantial differences in the orbital character and spectral features observed at nominally equivalent locations in the reciprocal space. Such differences cannot be accounted for by the usual dipole matrix element effects and are due instead to the structure factor, which must be explicitly considered whenever more than one atom is present in the unit cell.