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F. Fortuna

Publications and source records attributed to F. Fortuna.

At least 19 recordsLinked to original sources

Dimensional control of the band-gap crossover in layered lead iodide

Before assessing the suitability of a semiconductor for specific applications, the first question to ask is whether it possesses a direct or indirect band gap. This distinction is fundamental, as the operation of devices such as light-emitting diodes, solar cells, and photodetectors is closely tied to the band-gap nature. Semiconductors that exhibit a band-gap crossover, from indirect to direct or vice versa, offer enhanced versatility for optoelectronic applications. Prominent examples include transition metal dichalcogenides and the subject of this study, PbI2. The nature of the band gap, and its crossover, can only be directly determined in reciprocal space by tracking the valence-band maximum and conduction-band minimum. Here, we directly visualize the thickness-dependent crossover of PbI2 from an indirect to a direct band gap using angle-resolved photoemission spectroscopy. Our measurements reveal a shift of the valence-band maximum toward the Brillouin-zone center as the film thickness exceeds a monolayer. Supported by density functional theory calculations, our results show that this crossover is driven by interlayer interactions and the hybridization of iodine pz orbitals. These findings demonstrate the tunable electronic structure of PbI2 and its potential for optoelectronic applications.

cond-mat.mtrl-sci

Correlated Structural and Optical Characterization during Van der Waals Epitaxy of PbI2 on Graphene

Van der Waals heterostructures of 2D layered materials have gained much attention due to their flexible electronic properties, which make them promising candidates for energy, sensing, catalytic, and biomedical applications. Lead iodide (PbI2), a 2D layered semiconductor material belonging to the metal halide family, shows a thickness-dependent band gap with an indirect-to-direct transition above one monolayer. It has emerged as an excellent candidate for photodetectors and is a key component in metal halide perovskites solar cells. In the current work, we investigated the growth dynamics and the real-time correlation between structural and optical properties of PbI2 layers deposited on graphene/SiC(0001) by Molecular Beam Epitaxy. The structural and optical properties are probed respectively by Grazing Incidence Fast Atom Diffraction and Surface Differential Reflectance Spectroscopy. The growth proceeds layer-by-layer in a van der Waals-like epitaxy, with the zigzag direction of PbI2 parallel to the armchair direction of graphene. Both techniques bring evidence of significant modifications of the structural, electronic, and optical properties of the first PbI2 monolayer, characterized by a 1% tensile strain that relaxes over 3 to 5 monolayers. For a single monolayer, Angle-Resolved Photoemission Spectroscopy reveals a charge transfer from graphene to PbI2, demonstrated by an energy shift of the order of 50 meV in the graphene band structure.

cond-mat.mes-hall

Metallic layered materials with magnetic frustration: An ARPES view of the SmAuAl$_4$Ge$_2$ and TbAuAl$_4$Ge$_2$

Compounds of the new materials class LnTAl$_4$X$_2$ (Ln = lanthanide, X = tetrel, T = transition metal) host exotic magnetic phenomena due to geometric frustration induced by their triangular lattice. Complex spin arrangements, magnetic fluctuations and double magnetic transitions have been well observed by means of magneto-transport. Nevertheless, the experimental electronic structure of this family of materials has been poorly studied. We have investigated the experimental electronic structure of two members of this class of materials: SmAuAl$_4$Ge$_2$ and TbAuAl$_4$Ge$_2$. By means of Angle-Resolved PhotoEmission Spectroscopy (ARPES) accompanied by Density Functional Theory calculations (DFT), we reveal common trends and features, the important effect of localized spin moments on the electronic structure, the presence of surface-localized electronic states and the nature of the surface termination layer. Low-dimensionality, exchange interaction, and spin-orbit coupling are all important ingredients of the electronic structure.

cond-mat.str-el

Electronic structure dimensionality of the quantum-critical ferromagnet YbNi$_4$P$_2$

YbNi$_4$P$_2$ is the first known ferromagnetic metal showing a second-order quantum phase transition. Current theoretical understanding rules out second order ferromagnetic quantum criticality in centrosymmetric 2D and 3D metals. Thus, studying the electronic structure of YbNi$_4$P$_2$ is of prime fundamental importance. Using angle-resolved photoemission spectroscopy, we experimentally prove the existence of 1D Fermi surface contours. In addition, our results demonstrate that part of the electronic structure of YbNi$_4$P$_2$ is made of states of higher dimensionality, thereby bringing into question the fact that ferromagnetic quantum criticality in centrosymmetric crystals, is exclusively found in 1D systems. Our experimental data show that the electronic structure of YbNi$_4$P$_2$ is a playground of mixed dimensionality, electron correlations, strong hybridization and spin-orbit coupling, all of them providing new insights in understanding the origin of ferromagnetic quantum criticality.

cond-mat.str-el

Experimental observation of metallic states with different dimensionality in a quasi-1D charge density wave compound

TaTe$_4$ is a quasi-1D tetrachalcogenide that exhibits a CDW instability caused by a periodic lattice distortion. Recently, pressure-induced superconductivity has been achieved in this compound, revealing a competition between these different ground states and making TaTe$_4$ very interesting for fundamental studies. Although TaTe$_4$ exhibits CDW ordering below 475 K, transport experiments have reported metallic behavior with a resistivity plateau at temperatures lower than 10 K. In this paper, we study the electronic structure of TaTe$_4$ using a combination of high-resolution angle-resolved photoemission spectroscopy and density functional calculations. Our results reveal the existence of the long-sought metallic states. These states exhibit mixed dimensionality, while some of them might have potential topological properties.

cond-mat.str-el

Long-lived Andreev states as evidence for protected hinge modes in a bismuth nanoring Josephson junction

Second-order topological insulators are characterized by helical, non-spin-degenerate, one-dimensional states running along opposite crystal hinges, with no backscattering. Injecting superconducting pairs therefore entails splitting Cooper pairs into two families of helical Andreev states of opposite helicity, one at each hinge. Here we provide evidence for such separation via the measurement and analysis of switching supercurrent statistics of a crystalline nanoring of bismuth. Using a phenomenological model of two helical Andreev hinge modes, we find that pairs relax at a rate comparable to individual quasiparticles, in contrast with the much faster pair relaxation of non-topological systems. This constitutes a unique tell-tale sign of the spatial separation of topological helical hinges.

cond-mat.mes-hall

Experimental observation and spin texture of Dirac node arcs in tetradymite topological metals

We report the observation of a non-trivial spin texture in Dirac node arcs, novel topological objects formed when Dirac cones of massless particles extend along an open one-dimensional line in momentum space. We find that such states are present in all the compounds of the tetradymite M$_2$Te$_2$X family (M$=$Ti, Zr or Hf and X$=$P or As), regardless of the weak or strong character of the topological invariant. The Dirac node arcs in tetradymites are thus the simplest possible, textbook example, of a type-I Dirac system with a single spin-polarized node arc.

cond-mat.mes-hall

Quantum interference effects of out-of-plane confinement on two-dimensional electron systems in oxides

It was recently discovered that a conductive, metallic state is formed on the surface of some insulating oxides. Firstly observed on SrTiO$_3$(001), it was then found in other compounds as diverse as anatase TiO$_2$, KTaO$_3$, BaTiO$_3$, ZnO, and also on different surfaces of SrTiO$_3$ (or other oxides) with different symmetries. The spatial extension of the wave function of this electronic state is of only a few atomic layers. Experiments indicate its existence is related to the presence of oxygen vacancies induced at or near the surface of the oxide. In this article we present a simplified model aimed at describing the effect of its small spatial extension on measurements of its 3D electronic structure by angular resolved photoemission spectroscopy (ARPES). For the sake of clarity, we base our discussion on a simple tight binding scheme plus a confining potential that is assumed to be induced by the oxygen vacancies. Our model parameters are, nevertheless, obtained from density functional calculations. With this methodology we can explain from a very simple concept of selective interference the "wobbling", i.e., the photoemission intensity modulation and/or apparent dispersion of the Fermi surface and spectra along the out-of-plane ($k_z$) direction, and the "mixed 2D/3D" characteristics observed in some experiments. We conclude that the critical model parameters for such an effect are the relative strength of the electronic hopping of each band and the height/width aspect ratio of the surface confining potential. By considering recent photoemission measurements under the light of our findings, we can get relevant information on the electronic wave functions and of the nature of the confining potential.

cond-mat.str-el

Tunable two-dimensional electron system at the (110) surface of SnO$_2$

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.

cond-mat.mtrl-sci

Computed stereo lensless X-ray imaging

The ability to gain insights into the 3D properties of artificial or biological systems is often critical. However, 3D structures are difficult to retrieve at low dose and with extremely fast processing, as most techniques are based on acquiring and computing hundreds of 2D angular projections. This is even more challenging with ultrashort X-rays which allow realizing nanometre scale studies and ultrafast time resolved 2D movies. Here we show that computer stereo vision concepts can be transposed to X-rays. We demonstrate nanoscale three-dimensional reconstruction from a single ultrafast acquisition. Two diffraction patterns are recorded simultaneously on a single CCD camera and after phase retrieval two stereo images are reconstructed. A 3D representation of the sample is then computed from quantitative disparity maps with about 130x130x380nm3 voxel resolution in a snapshot of 20 femtoseconds. We extend our demonstration to phase contrast X-ray stereo imaging and reveal hidden 3D features of a sample. Computed phase stereo imaging will find scientific applications at X-ray free electron lasers, synchrotrons and laser-based sources, but also in fast industrial and medical 3D diagnostics.

eess.IV

Tailoring Vanadium Dioxide Film Orientation using Nanosheets: A Combined Microscopy, Diffraction, Transport and Soft X-ray in Transmission Study

VO2 is a much-discussed material for oxide electronics and neuromorphic computing applications. Here, heteroepitaxy of vanadium dioxide (VO2) was realized on top of oxide nanosheets that cover either the amorphous silicon dioxide surfaces of Si substrates or X-ray transparent silicon nitride membranes. The out-of-plane orientation of the VO2 thin films was controlled at will between (011)M1/(110)R and (-402)M1/(002)R by coating the bulk substrates with Ti0.87O2 and NbWO6 nanosheets, respectively, prior to VO2 growth. Temperature dependent X-ray diffraction and automated crystal orientation mapping in microprobe TEM mode (ACOM-TEM) characterized the high phase purity, the crystallographic and orientational properties of the VO2 films. Transport measurements and soft X-ray absorption in transmission are used to probe the VO2 metal-insulator transition, showing results of a quality equal to those from epitaxial films on bulk single-crystal substrates. Successful local manipulation of two different VO2 orientations on a single substrate is demonstrated using VO2 grown on lithographically-patterned lines of Ti0.87O2 and NbWO6 nanosheets investigated by electron backscatter diffraction. Finally, the excellent suitability of these nanosheet-templated VO2 films for advanced lensless imaging of the metal-insulator transition using coherent soft X-rays is discussed.

cond-mat.mtrl-sci

High-density two-dimensional electron system induced by oxygen vacancies in ZnO

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.

cond-mat.mtrl-sci

Converting topological insulators into topological metals within the tetradymite family

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 $Γ-$point, for (Zr,Hf)$_2$Te$_2$(P,As) there are Dirac cones of strong topological character around both the $\bar Γ$- 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).

cond-mat.str-el

Magnetization dynamics of weak stripe domains in Fe-N thin films: a multi-technique complementary approach

The resonant eigenmodes of a nitrogen-implanted iron α'-FeN characterized by weak stripe domains are investigated by Brillouin light scattering and broadband ferromagnetic resonance experiments, assisted by micromagnetic simulations. The spectrum of the dynamic eigenmodes in the presence of the weak stripes is very rich and two different families of modes can be selectively detected using different techniques or different experimental configurations. Attention is paid to the evolution of the mode frequencies and spatial profiles under the application of an external magnetic field, of variable intensity, in the direction parallel or transverse to the stripes. The different evolution of the modes with the external magnetic field is accompanied by a distinctive spatial localization in specific regions, such as the closure domains at the surface of the stripes and the bulk domains localized in the inner part of the stripes. The complementarity of BLS and FMR techniques, based on different selection rules, is found to be a fruitful tool for the study of the wealth of localized mag-netic excitations generally found in nanostructures.

cond-mat.mes-hall

Hubbard band or oxygen vacancy states in the correlated electron metal SrVO$_3$?

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.

cond-mat.str-el

Engineering two-dimensional electron gases at the (001) and (101) surfaces of TiO2 anatase using light

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.

cond-mat.mtrl-sci

Superconducting nanowires by electron-beam-induced deposition

Superconducting nanowires can be fabricated by decomposition of an organometallic gas using a focused beam of Ga ions. However, physical damage and unintentional doping often results from the exposure to the ion beam, motivating the search for a means to achieve similar structures with a beam of electrons instead of ions. This has so far remained an experimental challenge. We report the fabrication of superconducting tungsten nanowires by electron-beam-induced-deposition, with critical temperature of 2.0 K and critical magnetic field of 3.7 T, and compare them with superconducting wires made with ions. This work opens up new possibilities for the realization of nanoscale superconducting devices, without the requirement of an ion beam column.

cond-mat.mes-hall

Magnetic field resistant quantum interferences in bismuth nanowires based Josephson junctions

We investigate proximity induced superconductivity in micrometer-long bismuth nanowires con- nected to superconducting electrodes with a high critical field. At low temperature we measure a supercurrent that persists in magnetic fields as high as the critical field of the electrodes (above 11 T). The critical current is also strongly modulated by the magnetic field. In certain samples we find regular, rapid SQUID-like periodic oscillations occurring up to high fields. Other samples ex- hibit less periodic but full modulations of the critical current on Tesla field scales, with field-caused extinctions of the supercurrent. These findings indicate the existence of low dimensionally, phase coherent, interfering conducting regions through the samples, with a subtle interplay between orbital and spin contributions. We relate these surprising results to the electronic properties of the surface states of bismuth, strong Rashba spin-orbit coupling, large effective g factors, and their effect on the induced superconducting correlations.

cond-mat.mes-hall