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F. Y. Bruno

Publications and source records attributed to F. Y. Bruno.

At least 19 recordsLinked to original sources

Fermi surface and pseudogap in highly doped Sr$_{2}$IrO$_{4}$

The fate of the Fermi surface in bulk electron-doped Sr$_{2}$IrO$_{4}$ remains elusive, as does the origin and extension of its pseudogap phase. Here, we use high-resolution angle-resolved photoelectron spectroscopy (ARPES) to investigate the electronic structure of Sr$_{2-x}$La$_{x}$IrO$_{4}$ up to $x=0.2$, a factor of two higher than in previous work. We find that the antinodal pseudogap persists up to the highest doping level, and thus beyond the sharp increase in Hall carrier density to $\simeq 1+x$ recently observed above $x^{*}\simeq 0.16$ [Y.-T. Hsu et al., Nature Physics 20, 1593 (2024)]. This suggests that doped iridates host a unique phase of matter in which a large Hall density coexists with an anisotropic pseudogap, breaking up the Fermi surface into disconnected arcs. The temperature boundary of the pseudogap is $T^{*}\simeq 200$ K for $x=0.2$, comparable to cuprates and to the energy scale of short range antiferromagnetic correlations in cuprates and iridates.

cond-mat.str-el

KTaO3(001) Preparation Methods in Vacuum: Effects on Surface Stoichiometry, Crystallography, and in-gap States

KTaO3 single crystals with different orientations are used as substrates for the epitaxial growth of thin films and/or as hosts for two-dimensional electron gases. Due to the polar nature of the KTaO3(001) surface, one can expect difficulties and challenges to arise in its preparation. Maintaining good insulating characteristics without adding undesirable in-gap electronic states, obtaining good crystalline order up to the top surface layer, a sufficiently flat surface, and complete cleanliness of the surface (without water, C or OH contaminants), are in general difficult conditions to accomplish simultaneously. Cleaving in vacuum is likely the best option for obtaining a clean surface. However, since KTaO3 is cubic and lacks a well-defined cleavage plane, this method is notsuitable for sample growth or reproducible device fabrication. Here, we systematically evaluate the effect of typical preparation methods applied on the surfaces of KTaO3(001) single crystals. In particular, we used annealing in vacuum at different temperatures, light sputtering with Ar+ ions at low energy (500 eV) followed by annealing, heavy Ar+ ion bombardment and annealing, and grazing Ar+ ion bombardment under continuous azimuthal rotation combined with both annealing in vacuum and in O2 atmosphere. Possible side effects after each treatment are evaluated by a combination of techniques, including low-energy ion scattering at forward angles, Auger electron spectroscopy, low-energy electron energy loss, X-ray photoelectron spectroscopy, low-energy electron diffraction, and time of flightsecondary ion mass spectrometry. Advantages and shortcomings of each preparation method are discussed in detail.

cond-mat.mtrl-sci

High stability 2D electron gases formed in Si3N4/Al//KTaO3 heterostructures: synthesis and in-depth interfacial characterization

The two-dimensional electron gas (2DEG) found in KTaO3-based interfaces has garnered attention due to its remarkable electronic properties. In this study, we investigated the conducting system embedded at the Si3N4/Al//KTO(110) heterostructure. We demonstrate that the Al/KTO interface supports a conducting system, with the Si3N4 passivation layer acting as a barrier to oxygen diffusion, enabling ex-situ characterization. Our findings reveal that the mobility and carrier density of the system can be tuned by varying the Al layer thickness. Using scanning transmission electron microscopy, electron energy-loss spectroscopy, X-ray photoemission spectroscopy, and time-of-flight secondary ion mass spectrometry, we characterized the structural and chemical composition of the interface. We found that the Al layer fully oxidizes into AlOx, drawing oxygen from the KTaO3 substrate. The oxygen depletion zone extends 3-5 nm into the substrate and correlates to the Al thickness. Heterostructures with thicker Al layers exhibit higher carrier densities but lower mobilities, likely due to interactions with the oxygen vacancies that act as scattering centers. These findings highlight the importance of considering the effect and extent of the oxygen depletion zone when designing and modeling two-dimensional electron systems in complex oxides.

cond-mat.mtrl-sci

Anisotropic Electronic Structure of the Two-Dimensional Electron Gas at the AlOx/KTaO3(110) interface

Oxide-based two-dimensional electron gases (2DEGs) have generated significant interest due to their potential for discovering novel physical properties. Among these, 2DEGs formed in KTaO3 stand out due to the recently discovered crystal face-dependent superconductivity and large Rashba splitting, both of which hold potential for future oxide electronics devices. In this work, angle-resolved photoemission spectroscopy is used to study the electronic structure of the 2DEG formed at the (110) surface of KTaO3 after deposition of a thin Al layer. Our experiments revealed a remarkable anisotropy in the orbital character of the electron-like dispersive bands, which form a Fermi surface consisting of two elliptical contours with their major axes perpendicular to each other. The measured electronic structure is used to constrain the modeling parameters of self-consistent tight-binding slab calculations of the band structure. In these calculations, an anisotropic Rashba splitting is found with a value as large as 4 meV at the Fermi level along the [-110] crystallographic direction. This large unconventional and anisotropic Rashba splitting is rationalized based on the orbital angular momentum formulation. These findings provide insights into the interpretation of spin-orbitronics experiments and help to constrain models for superconductivity in the KTO(110)-2DEG system.

cond-mat.mtrl-sci

Electronic structure of the highly conductive perovskite oxide SrMoO$_3$

We use angle-resolved photoemission to map the Fermi surface and quasiparticle dispersion of bulk-like thin films of SrMoO$_3$ grown by pulsed laser deposition. The electronic self-energy deduced from our data reveals weak to moderate correlations in SrMoO$_3$, consistent with our observation of well-defined electronic states over the entire occupied band width. We further introduce spectral function calculations that combine dynamical mean-field theory with an unfolding procedure of density functional calculations and demonstrate good agreement of this approach with our experiments.

cond-mat.str-el

Bulk and surface electronic structure of the dual-topology semimetal Pt2HgSe3

We report high-resolution angle resolved photoemission measurements on single crystals of Pt2HgSe3 grown by high-pressure synthesis. Our data reveal a gapped Dirac nodal line whose (001)-projection separates the surface Brillouin zone in topological and trivial areas. In the non-trivial $k$-space range we find surface states with multiple saddle-points in the dispersion resulting in two van Hove singularities in the surface density of states. Based on density functional theory calculations, we identify these surface states as signatures of a topological crystalline state which coexists with a weak topological phase.

cond-mat.mtrl-sci

High-resolution photoemission on Sr2RuO4 reveals correlation-enhanced effective spin-orbit coupling and dominantly local self-energies

We explore the interplay of electron-electron correlations and spin-orbit coupling in the model Fermi liquid Sr2RuO4 using laser-based angle-resolved photoemission spectroscopy. Our precise measurement of the Fermi surface confirms the importance of spin-orbit coupling in this material and reveals that its effective value is enhanced by a factor of about two, due to electronic correlations. The self-energies for the $β$ and $γ$ sheets are found to display significant angular dependence. By taking into account the multi-orbital composition of quasiparticle states, we determine self-energies associated with each orbital component directly from the experimental data. This analysis demonstrates that the perceived angular dependence does not imply momentum-dependent many-body effects, but arises from a substantial orbital mixing induced by spin-orbit coupling. A comparison to single-site dynamical mean-field theory further supports the notion of dominantly local orbital self-energies, and provides strong evidence for an electronic origin of the observed non-linear frequency dependence of the self-energies, leading to `kinks' in the quasiparticle dispersion of Sr2RuO4.

cond-mat.str-el

Band Structure and Spin-Orbital Texture of the (111)-KTaO3 Two-Dimensional Electron Gas

Two-dimensional electron gases (2DEGs) in oxides show great potential for discovering new physical phenomena and at the same time hold promise for electronic applications. In this work we use angle resolved photoemission to determine the electronic structure of a 2DEG stabilized in the (111)-oriented surface of the strong spin orbit coupling material KTaO3. Our measurements reveal multiple sub-bands that emerge as a consequence of quantum confinement and form a six-fold symmetric Fermi surface. This electronic structure is well reproduced by self-consistent tight-binding supercell calculations. Based on these calculations we determine the spin and orbital texture of the 2DEG. We show that the 2DEG Fermi surface is derived from bulk J = 3/2 states and exhibits an unconventional anisotropic Rashba-like lifting of the spin-degeneracy. Spin-momentum locking holds only for high symmetry directions and a strong out-of-plane spin component renders the spin-texture three-fold symmetric. We find that the average spin-splitting on the Fermi surface is an order of magnitude larger than in SrTiO3, which should translate into an enhancement in the spin-orbitronic response of (111)-KTaO3 2DEG based devices.

cond-mat.mtrl-sci

In-situ strain-tuning of the metal-insulator-transition of Ca$_{2}$RuO$_{4}$ in angle-resolved photoemission experiments

We report the evolution of the $k$-space electronic structure of lightly doped bulk Ca$_{2}$RuO$_{4}$ with uniaxial strain. Using ultrathin plate-like crystals, we achieve strain levels up to $-4.1\%$, sufficient to suppress the Mott phase and access the previously unexplored metallic state at low temperature. Angle-resolved photoemission experiments performed while tuning the uniaxial strain reveal that metallicity emerges from a marked redistribution of charge within the Ru $t_{2g}$ shell, accompanied by a sudden collapse of the spectral weight in the lower Hubbard band and the emergence of a well defined Fermi surface which is devoid of pseudogaps. Our results highlight the profound roles of lattice energetics and of the multiorbital nature of Ca$_{2}$RuO$_{4}$ in this archetypal Mott transition and open new perspectives for spectroscopic measurements.

cond-mat.str-el

Observation of out-of-plane spin texture in a SrTiO3 (111) two-dimensional electron gas

We explore the second order bilinear magnetoelectric resistance (BMER) effect in the d-electron-based two-dimensional electron gas (2DEG) at the SrTiO3 (111) surface. We find an evidence of a spin-split band structure with the archetypal spin-momentum locking of the Rashba effect for the in-plane component. Under an out-of-plane magnetic field, we find a BMER signal that breaks the six-fold symmetry of the electronic dispersion, which is a fingerprint for the presence of a momentum dependent out-of-plane spin component. Relativistic electronic structure calculations reproduce this spin-texture and indicate that the out-of-plane component is a ubiquitous property of oxide 2DEGs arising from strong crystal field effects. We further show that the BMER response of the SrTiO3 (111) 2DEG is tunable and unexpectedly large.

cond-mat.mes-hall

Structural, magnetic, and electronic properties of GdTiO3 Mott insulator thin films grown by pulsed laser deposition

We report on the optimization process to synthesize epitaxial thin films of GdTiO3 on SrLaGaO4 substrates by pulsed laser deposition. Optimized films are free of impurity phases and are fully strained. They possess a magnetic Curie temperature TC = 31.8 K with a saturation magnetization of 4.2 muB per formula unit at 10 K. Transport measurements reveal an insulating response, as expected. Optical spectroscopy indicates a band gap of 0.7 eV, comparable to the bulk value. Our work adds ferrimagnetic orthotitanates to the palette of perovskite materials for the design of emergent strongly correlated states at oxide interfaces using a versatile growth technique such as pulsed laser deposition.

cond-mat.str-el

Atomically precise lateral modulation of a two-dimensional electron liquid in anatase TiO2 thin films

Engineering the electronic band structure of two-dimensional electron liquids (2DELs) confined at the surface or interface of transition metal oxides is key to unlocking their full potential. Here we describe a new approach to tailoring the electronic structure of an oxide surface 2DEL demonstrating the lateral modulation of electronic states with atomic scale precision on an unprecedented length scale comparable to the Fermi wavelength. To this end, we use pulsed laser deposition to grow anatase TiO2 films terminated by a (1 x 4) in-plane surface reconstruction. Employing photo-stimulated chemical surface doping we induce 2DELs with tunable carrier densities that are confined within a few TiO2 layers below the surface. Subsequent in-situ angle resolved photoemission experiments demonstrate that the (1 x 4) surface reconstruction provides a periodic lateral perturbation of the electron liquid. This causes strong backfolding of the electronic bands, opening of unidirectional gaps and a saddle point singularity in the density of states near the chemical potential.

cond-mat.str-el

ARPES Studies of Two-Dimensional Electron Gases at Transition Metal Oxide Surfaces

High mobility two-dimensional electron gases (2DEGs) underpin today's silicon based devices and are of fundamental importance for the emerging field of oxide electronics. Such 2DEGs are usually created by engineering band offsets and charge transfer at heterointerfaces. However, in 2011 it was shown that highly itinerant 2DEGs can also be induced at bare surfaces of different transition metal oxides where they are far more accessible to high resolution angle resolved photoemission (ARPES) experiments. Here we review work from this nascent field which has led to a systematic understanding of the subband structure arising from quantum confinement of highly anisotropic transition metal d-states along different crystallographic directions. We further discuss the role of different surface preparations and the origin of surface 2DEGs, the understanding of which has permitted control over 2DEG carrier densities. Finally, we discuss signatures of strong many-body interactions and how spectroscopic data from surface 2DEGs may be related to the transport properties of interface 2DEGs in the same host materials.

cond-mat.str-el

Electronic structure of buried LaNiO3 layers in (111)-oriented LaNiO3/LaMnO3 superlattices probed by soft x-ray ARPES

Taking advantage of the large electron escape depth of soft x-ray angle resolved photoemission spectroscopy we report electronic structure measurements of (111)-oriented [LaNiO3/LaMnO3] superlattices and LaNiO3 epitaxial films. For thin films we observe a 3D Fermi surface with an electron pocket at the Brillouin zone center and hole pockets at the zone vertices. Superlattices with thick nickelate layers present a similar electronic structure. However, as the thickness of the LaNiO3 is reduced the superlattices become insulating. These heterostructures do not show a marked redistribution of spectral weight in momentum space but exhibit a pseudogap of 50 meV.

cond-mat.mtrl-sci

Observation of Large Topologically Trivial Fermi-Arcs in the Candidate Type-II Weyl Semimetal WTe2

We report angle-resolved photoemission experiments resolving the distinct electronic structure of the inequivalent top and bottom (001) surfaces of WTe2. On both surfaces, we identify a surface state that forms a large Fermi-arc emerging out of the bulk electron pocket. Using surface electronic structure calculations, we show that these Fermi arcs are topologically trivial and that their existence is independent of the presence of type-II Weyl points in the bulk band structure. This implies that the observation of surface Fermi arcs alone does not allow the identification of WTe2 as a topological Weyl semimetal. We further use the identification of the two different surfaces to clarify the number of Fermi surface sheets in WTe2.

cond-mat.mtrl-sci

Fermi arcs and their topological character in the candidate type-II Weyl semimetal MoTe2

We report a combined experimental and theoretical study of the candidate type-II Weyl semimetal MoTe2. Using laser-based angle-resolved photoemission we resolve multiple distinct Fermi arcs on the inequivalent top and bottom (001) surfaces. All surface states observed experimentally are reproduced by an electronic structure calculation for the experimental crystal structure that predicts a topological Weyl semimetal state with 8 type-II Weyl points. We further use systematic electronic structure calculations simulating different Weyl point arrangements to discuss the robustness of the identified Weyl semimetal state and the topological character of Fermi arcs in MoTe2.

cond-mat.mtrl-sci

Absence of Giant Spin Splitting in the Two-Dimensional Electron Liquid at the Surface of SrTiO$_3$ (001)

We reinvestigate the putative giant spin splitting at the surface of SrTiO$_3$ reported by Santander-Syro $et~al.$ [Nature Mat. 13, 1085 (2014)]. Our spin- and angle-resolved photoemission experiments on (001) oriented surfaces supporting a two-dimensional electron liquid with high carrier density show no detectable spin polarization in the photocurrent. We demonstrate that this result excludes a giant spin splitting while it is fully consistent with the unconventional Rashba-like splitting seen in band structure calculations that reproduce the experimentally observed ladder of quantum confined subbands.

cond-mat.str-el

Tailoring the nature and strength of electron-phonon interactions in the SrTiO$_3$(001) two-dimensional electron liquid

Surfaces and interfaces offer new possibilities for tailoring the many-body interactions that dominate the electrical and thermal properties of transition metal oxides. Here, we use the prototypical two-dimensional electron liquid (2DEL) at the SrTiO$_3$(001) surface to reveal a remarkably complex evolution of electron-phonon coupling with the tunable carrier density of this system. At low density, where superconductivity is found in the analogous 2DEL at the LaAlO$_3$/SrTiO$_3$ interface, our angle-resolved photoemission data show replica bands separated by 100\,meV from the main bands. This is a hallmark of a coherent polaronic liquid and implies strong long-range coupling to a single longitudinal optical phonon mode. In the overdoped regime the preferential coupling to this mode decreases and the 2DEL undergoes a crossover to a more conventional metallic state with weaker short-range electron-phonon interaction. These results place constraints on the theoretical description of superconductivity and allow for a unified understanding of the transport properties in SrTiO$_3$-based 2DELs.

cond-mat.str-el