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A. Damascelli

Publications and source records attributed to A. Damascelli.

At least 55 records · Page 3Linked to original sources

Bond-Order and the Role of Ligand States in Stripe-Modulated IrTe2

The coupled electronic-structural modulations of the ligand states in IrTe$_2$ have been studied by x-ray absorption spectroscopy (XAS) and resonant elastic x-ray scattering (REXS). Distinctive pre-edge structures are observed at the Te-$M_{4,5}$ (3$d$ $\rightarrow$ 5$p$) absorption edge, indicating the presence of a Te 5$p$-Ir 5$d$ covalent state near the Fermi level. An enhancement of the REXS signal near the Te 3$d$ $\rightarrow$ 5$p$ resonance at the $Q\!=\!(1/5,0,-1/5)$ superlattice reflection is observed below the structural transition temperature $T_s\sim$ 280 K. The analysis of the energy-dependent REXS lineshape reveals the key role played by the spatial modulation of the covalent Te 5$p$-Ir 5$d$ bond-density in driving the stripe-like order in IrTe$_2$, and uncovers its coupling with the charge and/or orbital order at the Ir sites. The similarity between these findings and the charge-ordering phenomenology observed in the high-T$_c$ superconducting cuprates suggests that the iridates may harbor similar exotic phases.

cond-mat.str-el↗

Sign inversion in the superconducting order parameter of LiFeAs inferred from Bogoliubov quasiparticle interference

Quasiparticle interference (QPI) by means of scanning tunneling microscopy/spectroscopy (STM/STS), angle resolved photoemission spectroscopy (ARPES), and multi-orbital tight bind- ing calculations are used to investigate the band structure and superconducting order parameter of LiFeAs. Using this combination we identify intra- and interband scattering vectors between the hole (h) and electron (e) bands in the QPI maps. Discrepancies in the band dispersions inferred from previous ARPES and STM/STS are reconciled by recognizing a difference in the $k_z$ sensitivity for the two probes. The observation of both h-h and e-h scattering is exploited using phase-sensitive scattering selection rules for Bogoliubov quasiparticles. From this we infer an s$_\pm$ gap structure, where a sign change occurs in the superconducting order parameter between the e and h bands.

cond-mat.supr-con↗

Photoelectron spin-polarization-control in the topological insulator Bi2Se3

We study the manipulation of the photoelectron spin-polarization in Bi$_2$Se$_3$ by spin- and angle-resolved photoemission spectroscopy. General rules are established that enable controlling the spin-polarization of photoemitted electrons via light polarization, sample orientation, and photon energy. We demonstrate the $\pm$100% reversal of a single component of the measured spin-polarization vector upon the rotation of light polarization, as well as a full three-dimensional manipulation by varying experimental configuration and photon energy. While a material-specific density-functional theory analysis is needed for the quantitative description, a minimal two-atomic-layer model qualitatively accounts for the spin response based on the interplay of optical selection rules, photoelectron interference, and topological surface-state complex structure. It follows that photoelectron spin-polarization control is generically achievable in systems with a layer-dependent, entangled spin-orbital texture.

cond-mat.mtrl-sci↗

Breakdown of singlets and triplets in Sr2RuO4 revealed by spin-resolved ARPES

Spin-orbit coupling has been conjectured to play a key role in the low-energy electronic structure of Sr2RuO4. Using circularly polarized light combined with spin- and angle-resolved photoemission spectroscopy, we directly measure the value of the effective spin-orbit coupling to be 130 +/- 30 meV. This is even larger than theoretically predicted and comparable to the energy splitting of the dxy and dxz,yz orbitals around the Fermi surface, resulting in a strongly momentum-dependent entanglement of spin and orbital character. As demonstrated by the spin expectation value obtained for a pair of electrons with zero total momentum, the classification of the Cooper pairs in terms of pure singlets or triplets fundamentally breaks down, necessitating a description of the unconventional superconducting state of Sr2RuO4 in terms of these newly found spin-orbital entangled eigenstates.

cond-mat.supr-con↗

Charge order driven by Fermi-arc instability in Bi2201

The understanding of the origin of superconductivity in cuprates has been hindered by the apparent diversity of intertwining electronic orders in these materials. We combined resonant x-ray scattering (REXS), scanning-tunneling microscopy (STM), and angle-resolved photoemission spectroscopy (ARPES) to observe a charge order that appears consistently in surface and bulk, and in momentum and real space within one cuprate family, Bi2201. The observed wave vectors rule out simple antinodal nesting in the single-particle limit but match well with a phenomenological model of a many-body instability of the Fermi arcs. Combined with earlier observations of electronic order in other cuprate families, these findings suggest the existence of a generic charge-ordered state in underdoped cuprates and uncover its intimate connection to the pseudogap regime.

cond-mat.supr-con↗

Polarity-driven surface metallicity in SmB$_6$

By a combined angle-resolved photoemission spectroscopy and density functional theory study, we discover that the surface metallicity is polarity-driven in SmB$_6$. Two surface states, not accounted for by the bulk band structure, are reproduced by slab calculations for coexisting B$_6$ and Sm surface terminations. Our analysis reveals that a metallic surface state stems from an unusual property, generic to the (001) termination of all hexaborides: the presence of boron $2p$ dangling bonds, on a polar surface. The discovery of polarity-driven surface metallicity sheds new light on the 40-year old conundrum of the low-temperature residual conductivity of SmB$_6$, and raises a fundamental question in the field of topological Kondo insulators regarding the interplay between polarity and nontrivial topological properties.

cond-mat.mtrl-sci↗

Electronic superlattice revealed by resonant scattering from random impurities in Sr3Ru2O7

Resonant elastic x-ray scattering (REXS) is an exquisite element-sensitive tool for the study of subtle charge, orbital, and spin superlattice orders driven by the valence electrons, which therefore escape detection in conventional x-ray diffraction (XRD). Although the power of REXS has been demonstrated by numerous studies of complex oxides performed in the soft x-ray regime, the cross section and photon wavelength of the material-specific elemental absorption edges ultimately set the limit to the smallest superlattice amplitude and periodicity one can probe. Here we show -- with simulations and REXS on Mn-substituted Sr$_3$Ru$_2$O$_7$ -- that these limitations can be overcome by performing resonant scattering experiments at the absorption edge of a suitably-chosen, dilute impurity. This establishes that -- in analogy with impurity-based methods used in electron-spin-resonance, nuclear-magnetic resonance, and Mössbauer spectroscopy -- randomly distributed impurities can serve as a non-invasive, but now momentum-dependent probe, greatly extending the applicability of resonant x-ray scattering techniques.

cond-mat.str-el↗

Layer-by-layer entangled spin-orbital texture of the topological surface state in Bi2Se3

We study Bi2Se3 by polarization-dependent angle-resolved photoemission spectroscopy (ARPES) and density-functional theory slab calculations. We find that the surface state Dirac fermions are characterized by a layer-dependent entangled spin-orbital texture, which becomes apparent through quantum interference effects. This explains the discrepancy between the spin polarization from spin-resovled ARPES - ranging from 20 to 85% - and the 100% value assumed in phenomenological models. It also suggests a way to probe the intrinsic spin texture of topological insulators, and to continuously manipulate the spin polarization of photoelectrons and photocurrents all the way from 0 to +/-100% by an appropriate choice of photon energy, linear polarization, and angle of incidence.

cond-mat.mtrl-sci↗

Surface-enhanced charge-density-wave instability in underdoped Bi2201

Neutron and x-ray scattering experiments have provided mounting evidence for spin and charge ordering phenomena in underdoped cuprates. These range from early work on stripe correlations in Nd-LSCO to the latest discovery of charge-density-waves in YBCO. Both phenomena are characterized by a pronounced dependence on doping, temperature, and an externally applied magnetic field. Here we show that these electron-lattice instabilities exhibit also a previously unrecognized bulk-surface dichotomy. Surface-sensitive electronic and structural probes uncover a temperature-dependent evolution of the CuO2 plane band dispersion and apparent Fermi pockets in underdoped Bi2201, which is directly associated with an hitherto-undetected strong temperature dependence of the incommensurate superstructure periodicity below 130K. In stark contrast, the structural modulation revealed by bulk-sensitive probes is temperature independent. These findings point to a surface-enhanced incipient charge-density-wave instability, driven by Fermi surface nesting. This discovery is of critical importance in the interpretation of single-particle spectroscopy data and establishes the surface of cuprates and other complex oxides as a rich playground for the study of electronically soft phases.

cond-mat.supr-con↗

Determining the Surface-To-Bulk Progression in the Normal-State Electronic Structure of Sr2RuO4 by Angle-Resolved Photoemission and Density Functional Theory

In search of the potential realization of novel normal-state phases on the surface of Sr2RuO4 - those stemming from either topological bulk properties or the interplay between spin-orbit coupling (SO) and the broken symmetry of the surface - we revisit the electronic structure of the top-most layers by ARPES with improved data quality as well as ab-initio LDA slab calculations. We find that the current model of a single surface layer (\surd2x\surd2)R45° reconstruction does not explain all detected features. The observed depth-dependent signal degradation, together with the close quantitative agreement with LDA+SO slab calculations based on the LEED-determined surface crystal structure, reveal that (at a minimum) the sub-surface layer also undergoes a similar although weaker reconstruction. This points to a surface-to-bulk progression of the electronic states driven by structural instabilities, with no evidence for Dirac and Rashba-type states or surface magnetism.

cond-mat.str-el↗

Competition between the Pseudogap and Superconducting States of Bi$_{2}$Sr$_{2}$Ca$_{0.92}$Y$_{0.08}$Cu$_{2}$O$_{8+δ}$ Single Crystals Revealed by Ultrafast Broadband Optical Reflectivity

Ultrafast broadband transient reflectivity experiments are performed to study the interplay between the non-equilibrium dynamics of the pseudogap and the superconducting phases in Bi$_{2}$Sr$_{2}$Ca$_{0.92}$Y$_{0.08}$Cu$_{2}$O$_{8+δ}$. Once superconductivity is established the relaxation of the pseudogap proceeds $\sim$ 2 times faster than in the normal state, and the corresponding transient reflectivity variation changes sign after $\sim$ 0.5 ps. The results can be described by a set of coupled differential equations for the pseudogap and for the superconducting order parameter. The sign and strength of the coupling term suggest a remarkably weak competition between the two phases, allowing their coexistence.

cond-mat.str-el↗

Na2IrO3 as a spin-orbit-assisted antiferromagnetic insulator with a 340 meV gap

We study Na2IrO3 by ARPES, optics, and band structure calculations in the local-density approximation (LDA). The weak dispersion of the Ir 5d-t2g manifold highlights the importance of structural distortions and spin-orbit coupling (SO) in driving the system closer to a Mott transition. We detect an insulating gap Δ_gap = 340 meV which, at variance with a Slater-type description, is already open at 300 K and does not show significant temperature dependence even across T_N ~ 15 K. An LDA analysis with the inclusion of SO and Coulomb repulsion U reveals that, while the prodromes of an underlying insulating state are already found in LDA+SO, the correct gap magnitude can only be reproduced by LDA+SO+U, with U = 3 eV. This establishes Na2IrO3 as a novel type of Mott-like correlated insulator in which Coulomb and relativistic effects have to be treated on an equal footing.

cond-mat.str-el↗

Mott versus Slater-type metal-insulator transition in Mn-substituted Sr3Ru2O7

We present a temperature-dependent x-ray absorption (XAS) and resonant elastic x-ray scattering (REXS) study of the metal-insulator transition (MIT) in Sr3(Ru1-xMnx)2O7. The XAS results reveal that the MIT drives the onset of local antiferromagnetic correlations around the Mn impurities, a precursor of the long-range antiferromagnetism detected by REXS at T_order<T_MIT. This establishes that the MIT is of the Mott-type (electronic correlations) as opposed to Slater-type (magnetic order). While this behavior is induced by Mn impurities, the (1/4,1/4,0) order exists for a wide range of Mn concentrations, and points to an inherent instability of the parent compound.

cond-mat.str-el↗

NO-assisted molecular-beam epitaxial growth of nitrogen substituted EuO

We have investigated a method for substituting oxygen with nitrogen in EuO thin films, which is based on molecular beam epitaxy distillation with NO gas as the oxidizer. By varying the NO gas pressure, we produce crystalline, epitaxial EuO_(1-x)N_x films with good control over the films' nitrogen concentration. In-situ x-ray photoemission spectroscopy reveals that nitrogen substitution is connected to the formation Eu3+ 4f6 and a corresponding decrease in the number of Eu2+ 4f7, indicating that nitrogen is being incorporated in its 3- oxidation state. While small amounts of Eu3+ in over-oxidized Eu_(1-delta)O thin films lead to a drastic suppression of the ferromagnetism, the formation of Eu3+ in EuO_(1-x)N_x still allows the ferromagnetic phase to exist with an unaffected Tc, thus providing an ideal model system to study the interplay between the magnetic f7 (J=7/2) and the non-magnetic f6 (J=0) states close to the Fermi level.

cond-mat.mtrl-sci↗

Probing the role of Co substitution in the electronic structure of iron-pnictides

The role of Co substitution in the low-energy electronic structure of Ca(Fe$_{0.944}$Co$_{0.056}$)$_2$As$_2$ is investigated by resonant photoemission spectroscopy and density functional theory. The Co 3d-state center-of-mass is observed at 250 meV higher binding energy than Fe's, indicating that Co posses one extra valence electron, and that Fe and Co are in the same 2+ oxidation state. Yet, significant Co character is detected for the Bloch wavefunctions at the chemical potential, revealing that the Co 3d electrons are part of the Fermi sea determining the Fermi surface. This establishes the complex role of Co substitution in CaFe2As2, and the inadequacy of a rigid-band shift description.

cond-mat.supr-con↗

A spectral function tour of electron-phonon coupling outside the Migdal limit

We simulate spectral functions for electron-phonon coupling in a filled band system - far from the asymptotic limit often assumed where the phonon energy is very small compared to the Fermi energy in a parabolic band and the Migdal theorem predicting 1+lambda quasiparticle renormalizations is valid. These spectral functions are examined over a wide range of parameter space through techniques often used in angle-resolved photoemission spectroscopy (ARPES). Analyzing over 1200 simulations we consider variations of the microscopic coupling strength, phonon energy and dimensionality for two models: a momentum-independent Holstein model, and momentum-dependent coupling to a breathing mode phonon. In this limit we find that any `effective coupling', lambda_eff, inferred from the quasiparticle renormalizations differs from the microscopic dimensionless coupling characterizing these Hamiltonians, lambda, and could drastically either over- or under-estimate it depending on the particular parameters and model. In contrast, we show that perturbation theory retains good predictive power for low coupling and small momenta, and that the momentum-dependence of the self-energy can be revealed via the relationship between velocity renormalization and quasiparticle strength. Additionally we find that (although not strictly valid) it is often possible to infer the self-energy and bare electronic structure through a self-consistent Kramers-Kronig bare-band fitting; and also that through lineshape alone, when Lorentzian, it is possible to reliably extract the shape of the imaginary part of a momentum-dependent self-energy without reference to the bare-band.

cond-mat.str-el↗

Rashba spin-splitting control at the surface of the topological insulator Bi2Se3

The electronic structure of Bi2Se3 is studied by angle-resolved photoemission and density functional theory. We show that the instability of the surface electronic properties, observed even in ultra-high-vacuum conditions, can be overcome via in-situ potassium deposition. In addition to accurately setting the carrier concentration, new Rashba-like spin-polarized states are induced, with a tunable, reversible, and highly stable spin splitting. Ab-initio slab calculations reveal that these Rashba state are derived from the 5QL quantum-well states. While the K-induced potential gradient enhances the spin splitting, this might be already present for pristine surfaces due to the symmetry breaking of the vacuum-solid interface.

cond-mat.str-el↗