SearcharxivSearch

arXiv subjects

Marco Grioni

Publications and source records attributed to Marco Grioni.

At least 19 recordsLinked to original sources

Photostationary Lifshitz transition in High Tc superconductor Bi2Sr2CaCu2O8+{\delta}

To date, controlling the steady-state electronic band structure in high-Tc cuprate superconductors has been achieved primarily through chemical doping or magnetic fields. Here, we present that ultrafast optical excitation can instead drive the electronic band structure of Bi2Sr2CaCu2O8+{\delta} into a photostationary, long-lived excited state. At sufficiently high pump fluences, this state undergoes a Lifshitz transition of the Fermi surface, characterized by a change in topology from hole-like to electron-like. Time- and angle-resolved photoemission spectroscopy, supported by single-band tight-binding calculations, reveals that 1.6 eV photoexcitation induces band-structure evolutions closely analogous to those produced by chemical doping. These results point to an efficient photodoping mechanism involving cooperative effects, including charge transfer, renormalization of effective electronic correlations, and defect-assisted charge trapping. Our findings raise fundamental questions regarding thermalization processes occurring on timescales comparable to the laser repetition period in cuprates. More broadly, ultrafast optical control enables access to otherwise inaccessible regions of the phase diagram by tuning the pump fluence.

cond-mat.str-el

High-resolution MHz time- and angle-resolved photoemission spectroscopy based on a tunable vacuum ultraviolet source

Time and angle-resolved photoemission spectroscopy (trARPES) allows direct mapping of the electronic band structure and its dynamic response on femtosecond timescales. Here, we present a new ARPES system, powered by a new fiber-based femtosecond light source in the vacuum ultraviolet (VUV) range, accessing the complete first Brillouin zone for most materials. We present trARPES data on Au(111), polycrystalline Au, Bi2Se3 and TaTe2, demonstrating an energy resolution of 21 meV with a time resolution of <360 fs, at a high repetition rate of 1 MHz. The system is integrated with an extreme ultraviolet (EUV) high harmonic generation (HHG) beamline, enabling excellent tunability of the time-bandwidth resolution.

physics.ins-det

Unveiling the electronic transformations in the semi-metallic correlated-electron transitional oxide Mo$_8$O$_{23}$

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.

cond-mat.str-el

Orbitally selective breakdown of Fermi liquid quasiparticles in Ca$_{1.8}$Sr$_{0.2}$RuO$_4$

We present a comprehensive angle-resolved photoemission spectroscopy study of Ca$_{1.8}$Sr$_{0.2}$RuO$_4$. Four distinct bands are revealed and along the Ru-O bond direction their orbital characters are identified through a light polarization analysis and comparison to dynamical mean-field theory calculations. Bands assigned to $d_{xz}, d_{yz}$ orbitals display Fermi liquid behavior with fourfold quasiparticle mass renormalization. Extremely heavy fermions - associated with a predominantly $d_{xy}$ band character - are shown to display non-Fermi-liquid behavior. We thus demonstrate that Ca$_{1.8}$Sr$_{0.2}$RuO$_4$ is a hybrid metal with an orbitally selective Fermi liquid quasiparticle breakdown.

cond-mat.str-el

Dispersive Magnetic and Electronic Excitations in Iridate Perovskites Probed with Oxygen $K$-Edge Resonant Inelastic X-ray Scattering

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.

cond-mat.str-el

Kondo lattice excitation observed using resonant inelastic X-ray scattering at the Yb $M_5$ edge

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.

cond-mat.str-el

Strongly bound excitons in anatase TiO2 single crystals and nanoparticles

Anatase TiO$_2$ 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.

cond-mat.mtrl-sci

A Novel Quasi-One-Dimensional Topological Insulator in Bismuth Iodide $β$-Bi$_4$I$_4$

Recent progress in the field of topological states of matter(1,2) has largely been initiated by the discovery of bismuth and antimony chalcogenide bulk topological insulators (TIs)(3-6), followed by closely related ternary compounds(7-16) and predictions of several weak TIs(17-19). However, both the conceptual richness of Z$_2$ classification of TIs as well as their structural and compositional diversity are far from being fully exploited. Here, a new Z$_2$ topological insulator is theoretically predicted and experimentally confirmed in the $β$-phase of quasi-one-dimensional bismuth iodide Bi$_4$I$_4$. The electronic structure of $β$-Bi$_4$I$_4$, characterized by Z$_2$ invariants (1;110), is in proximity of both the weak TI phase (0;001) and the trivial insulator phase (0;000). Our angle-resolved photoemission spectroscopy measurements on the (001) surface reveal a highly anisotropic band-crossing feature located at the point of the surface Brillouin zone and showing no dispersion with the photon energy, thus being fully consistent with the theoretical prediction.

cond-mat.mtrl-sci

Ultrafast Electron Dynamics in Epitaxial Graphene Investigated with Time- and Angle-Resolved Photoemission Spectroscopy

In order to exploit the intriguing optical properties of graphene it is essential to gain a better understanding of the light-matter interaction in the material on ultrashort timescales. Exciting the Dirac fermions with intense ultrafast laser pulses triggers a series of processes involving interactions between electrons, phonons and impurities. Here we study these interactions in epitaxial graphene supported on silicon carbide (semiconducting) and iridium (metallic) substrates using ultrafast time- and angle-resolved photoemission spectroscopy (TR-ARPES) based on high harmonic generation. For the semiconducting substrate we reveal a complex hot carrier dynamics that manifests itself in an elevated electronic temperature and an increase in linewidth of the $π$ band. By analyzing these effects we are able to disentangle electron relaxation channels in graphene. On the metal substrate this hot carrier dynamics is found to be severely perturbed by the presence of the metal, and we find that the electronic system is much harder to heat up than on the semiconductor due to screening of the laser field by the metal.

cond-mat.str-el

Tunable Carrier Multiplication and Cooling in Graphene

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.

cond-mat.mtrl-sci

Observation of Ultrafast Free Carrier Dynamics in Single Layer MoS$_2$

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.

cond-mat.mtrl-sci

Ramifications of Optical Pumping on the Interpretation of Time-Resolved Photoemission Experiments on Graphene

In pump-probe time and angle-resolved photoemission spectroscopy (TR-ARPES) experiments the presence of the pump pulse adds a new level of complexity to the photoemission process in comparison to conventional ARPES. This is evidenced by pump-induced vacuum space-charge effects and surface photovoltages, as well as multiple pump excitations due to internal reflections in the sample-substrate system. These processes can severely affect a correct interpretation of the data by masking the out-of-equilibrium electron dynamics intrinsic to the sample. In this study, we show that such effects indeed influence TR-ARPES data of graphene on a silicon carbide (SiC) substrate. In particular, we find a time- and laser fluence-dependent spectral shift and broadening of the acquired spectra, and unambiguously show the presence of a double pump excitation. The dynamics of these effects is slower than the electron dynamics in the graphene sample, thereby permitting us to deconvolve the signals in the time domain. Our results demonstrate that complex pump-related processes should always be considered in the experimental setup and data analysis.

cond-mat.str-el

Ultrafast Dynamics of Massive Dirac Fermions in Bilayer Graphene

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.

cond-mat.mes-hall

Extracting the Temperature of Hot Carriers in Time- and Angle-Resolved Photoemission

The interaction of light with a material's electronic system creates an out-of-equilibrium (non-thermal) distribution of optically excited electrons. Non-equilibrium dynamics relaxes this distribution on an ultrafast timescale to a hot Fermi-Dirac distribution with a well-defined temperature. The advent of time- and angle-resolved photoemission spectroscopy (TR-ARPES) experiments has made it possible to track the decay of the temperature of the excited hot electrons in selected states in the Brillouin zone, and to reveal their cooling in unprecedented detail in a variety of emerging materials. It is, however, not a straightforward task to determine the temperature with high accuracy. This is mainly attributable to an a priori unknown position of the Fermi level and the fact that the shape of the Fermi edge can be severely perturbed when the state in question is crossing the Fermi energy. Here, we introduce a method that circumvents these difficulties and accurately extracts both the temperature and the position of the Fermi level for a hot carrier distribution by tracking the occupation statistics of the carriers measured in a TR-ARPES experiment.

cond-mat.str-el

Combined large spin-splitting and one dimensional confinement in surface alloys

We have found and characterized by angle-resolved photoelectron spectroscopy (ARPES) quasi-one dimensional spin-split states in chain-like surface alloys formed by large Z elements (Bi and Pb) at the Cu(110) surface. The ARPES results are supported by first-principles relativistic calculations, which also confirm the spin polarization of these states, characteristic of the Rashba-Bychkov effect. The Fermi surface contours are open, but warped, as a result of the interaction with the bulk Cu conduction band. This interaction introduces a k dependence of the spin splitting perpendicular to the chains direction. We have also investigated the influence of the atomic spin-orbit parameter in substitutional isostructural Bi_{1-x}Pb_{x} overlayers, and found that the magnitude of the spin splitting can be continuously tuned as a function of stoichiometry.

cond-mat.mes-hall

Direct view on the ultrafast carrier dynamics in graphene

The ultrafast dynamics of excited carriers in graphene is closely linked to the Dirac spectrum and plays a central role for many electronic and optoelectronic applications. Harvesting energy from excited electron-hole pairs, for instance, is only possible if these pairs can be separated before they lose energy to vibrations, merely heating the lattice. While the hot carrier dynamics in graphene could so far only be accessed indirectly, we here present a direct time-resolved view on the Dirac cone by angle-resolved photoemission (ARPES). This allows us to show the quasi-instant thermalisation of the electron gas to a temperature of more than 2000 K; to determine the time-resolved carrier density; to disentangle the subsequent decay into excitations of optical phonons and acoustic phonons (directly and via supercollisions); and to show how the presence of the hot carrier distribution affects the lifetime of the states far below the Fermi energy.

cond-mat.mes-hall

Two Distinct Phases of Bilayer Graphene Films on Ru(0001)

By combining angle-resolved photoemission spectroscopy and scanning tunneling microscopy we reveal the structural and electronic properties of multilayer graphene on Ru(0001). We prove that large ethylene exposure allows to synthesize two distinct phases of bilayer graphene with different properties. The first phase has Bernal AB stacking with respect to the first graphene layer, displays weak vertical interaction and electron doping. The long-range ordered moiré pattern modulates the crystal potential and induces replicas of the Dirac cone and minigaps. The second phase has AA stacking sequence with respect to the first layer, displays weak structural and electronic modulation and p-doping. The linearly dispersing Dirac state reveals the nearly-freestanding character of this novel second layer phase.

cond-mat.mes-hall

Anisotropic spin gaps in BiAg$_2$-Ag/Si(111)

We present a detailed analysis of the band structure of the BiAg$_2$/Ag/Si(111) trilayer system by means of high resolution Angle Resolved Photoemission Spectroscopy (ARPES). BiAg2/Ag/Si(111) exhibits a complex spin polarized electronic structure due to giant spin-orbit interactions. We show that a complete set of constant energy ARPES maps, supplemented by a modified nearly free electron calculation, provides a unique insight into the structure of the spin polarized bands and spin gaps. We also show that the complex gap structure can be continuously tuned in energy by a controlled deposition of an alkali metal.

cond-mat.mtrl-sci