Deconstruction of Resolution Effects in Angle-Resolved Photoemission

We study how the energy and momentum resolution of angle-resolved photoemission spectroscopy (ARPES) affects the linewidth, Fermi crossing, velocity, and curvature of the measured band structure. Based on the fact that the resolution smooths out the spectra, acting as a low-pass filter, we develop an iterative simulation scheme that compensates for resolution effects and allows the fundamental physical parameters to be accurately extracted. By simulating a parabolic band structure of Fermi-liquid quasiparticles, we show that this method works for an energy resolution up to 100 meV and a momentum resolution equal to twice the energy resolution scaled by the Fermi velocity. Our analysis acquires particular relevance in the hard and soft x-ray regimes, where a degraded resolution limits the accuracy of the extracted physical parameters, making it possible to study how the electronic excitations are modified when the ARPES probing depth increases beyond the surface.Comment: A high-resolution version can be found at: http://www.phas.ubc.ca/~quantmat/ARPES/PUBLICATIONS/Articles/ARPES_resolution.pd

Low temperature ellipsometry of NaV2O5

The dielectric function of alpha'NaV2O5 was measured with electric field along the a and b axes in the photon energy range 0.8-4.5 eV for temperatures down to 4K. We observe a pronounced decrease of the intensity of the 1 eV peak upon increasing temperature with an activation energy of about 25meV, indicating that a finite fraction of the rungs becomes occupied with two electrons while others are emptied as temperature increases. No appreciable shifts of peaks were found s in the valence state of individual V atoms at the phase transition is very small. A remarkable inflection of this temperature dependence at the phase transition at 34 K indicates that charge ordering is associated with the low temperature phase.Comment: Revisions in style and order of presentation. One new figure. In press in Physical Review B. REVTeX, 4 pages with 4 postscript figure

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{\deg} 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.Comment: 4 pages, 4 figures, 1 table. Further information and PDF available at: http://www.phas.ubc.ca/~quantmat/ARPES/PUBLICATIONS/articles.htm

Suppressed reflectivity due to spin-controlled localization in a magnetic semiconductor

The narrow gap semiconductor FeSi owes its strong paramagnetism to electron-correlation effects. Partial Co substitution for Fe produces a spin-polarized doped semiconductor. The spin-polarization causes suppression of the metallic reflectivity and increased scattering of charge carriers, in contrast to what happens in other magnetic semiconductors, where magnetic order reduces the scattering. The loss of metallicity continues progressively even into the fully polarized state, and entails as much as a 25% reduction in average mean-free path. We attribute the observed effect to a deepening of the potential wells presented by the randomly distributed Co atoms to the majority spin carriers. This mechanism inverts the sequence of steps for dealing with disorder and interactions from that in the classic Al'tshuler Aronov approach - where disorder amplifies the Coulomb interaction between carriers - in that here, the Coulomb interaction leads to spin polarization which in turn amplifies the disorder-induced scattering.Comment: 6 figures Submitted to PR

Dirac dispersion and non-trivial Berry's phase in three-dimensional semimetal RhSb3

We report observations of magnetoresistance, quantum oscillations and angle-resolved photoemission in RhSb$_3$, a unfilled skutterudite semimetal with low carrier density. The calculated electronic band structure of RhSb$_3$ entails a $Z_2$ quantum number $\nu_0=0,\nu_1=\nu_2=\nu_3=1$ in analogy to strong topological insulators, and inverted linear valence/conduction bands that touch at discrete points close to the Fermi level, in agreement with angle-resolved photoemission results. Transport experiments reveal an unsaturated linear magnetoresistance that approaches a factor of 200 at 60 T magnetic fields, and quantum oscillations observable up to 150~K that are consistent with a large Fermi velocity ($\sim 1.3\times 10^6$ ms$^{-1}$), high carrier mobility ($\sim 14$ $m^2$/Vs), and small three dimensional hole pockets with nontrivial Berry phase. A very small, sample-dependent effective mass that falls as low as $0.015(7)$ bare masses scales with Fermi velocity, suggesting RhSb$_3$ is a new class of zero-gap three-dimensional Dirac semimetal.Comment: 9 pages, 4 figure

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 {\Delta}_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.Comment: Accepted in Physical Review Letters. Auxiliary and related material can be found at: http://www.phas.ubc.ca/~quantmat/ARPES/PUBLICATIONS/articles.htm

Doping dependent charge order correlations in electron-doped cuprates

Understanding the interplay between charge order (CO) and other phenomena (e.g. pseudogap, antiferromagnetism, and superconductivity) is one of the central questions in the cuprate high-temperature superconductors. The discovery that similar forms of CO exist in both hole- and electron-doped cuprates opened a path to determine what subset of the CO phenomenology is universal to all the cuprates. Here, we use resonant x-ray scattering to measure the charge order correlations in electron-doped cuprates (La2-xCexCuO4 and Nd2-xCexCuO4) and their relationship to antiferromagnetism, pseudogap, and superconductivity. Detailed measurements of Nd2-xCexCuO4 show that CO is present in the x = 0.059 to 0.166 range, and that its doping dependent wavevector is consistent with the separation between straight segments of the Fermi surface. The CO onset temperature is highest between x = 0.106 and 0.166, but decreases at lower doping levels, indicating that it is not tied to the appearance of antiferromagnetic correlations or the pseudogap. Near optimal doping, where the CO wavevector is also consistent with a previously observed phonon anomaly, measurements of the CO below and above the superconducting transition temperature, or in a magnetic field, show that the CO is insensitive to superconductivity. Overall these findings indicate that, while verified in the electron-doped cuprates, material-dependent details determine whether the CO correlations acquire sufficient strength to compete for the ground state of the cuprates.Comment: Supplementary information available upon reques

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 M\"ossbauer 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

Neel Order and Electron Spectral Functions in the Two-Dimensional Hubbard Model: a Spin-Charge Rotating Frame Approach

Using recently developed quantum SU(2)xU(1) rotor approach, that provides a self-consistent treatment of the antiferromagnetic state we have performed electronic spectral function calculations for the Hubbard model on the square lattice. The collective variables for charge and spin are isolated in the form of the space-time fluctuating U(1) phase field and rotating spin quantization axis governed by the SU(2) symmetry, respectively. As a result interacting electrons appear as composite objects consisting of bare fermions with attached U(1) and SU(2) gauge fields. This allows us to write the fermion Green's function in the space-time domain as the product CP^1 propagator resulting from the SU(2) gauge fields, U(1) phase propagator and the pseudo-fermion correlation function. As a result the problem of calculating the spectral line shapes now becomes one of performing the convolution of spin, charge and pseudo-fermion Green's functions. The collective spin and charge fluctuations are governed by the effective actions that are derived from the Hubbard model for any value of the Coulomb interaction. The emergence of a sharp peak in the electron spectral function in the antiferromagnetic state indicates the decay of the electron into separate spin and charge carrying particle excitations.Comment: 16 pages, 5 figures, submitted to Phys. Rev.

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.Comment: A high-resolution version can be found at http://www.physics.ubc.ca/~quantmat/ARPES/PUBLICATIONS/Articles/BiSe_K.pd