The theory for time-resolved photoemission spectroscopy as applied to pump-probe experiments is developed and solved for the generic case of a strongly correlated material. The formal development incorporates all of the nonequilibrium effects of the pump pulse and the finite time width of the probe pulse. While our formal development is completely general, in our numerical illustration for the Hubbard model, we assume the pump pulse drives the electrons into a nonequilibrium configuration, which rapidly thermalizes to create a hot (quasi-equilibrium) electronic system, and we then study the effects of windowing that arise from the finite width of the probe pulse. We find sharp features in the spectra are broadened, particularly the quasiparticle peak of strongly correlated metals at low temperature.
Nonequilibrium calculations in the presence of an electric field are usually performed in a gauge, and need to be transformed to reveal the gauge-invariant observables. In this work, we discuss the issue of gauge invariance in the context of time-resolved angle-resolved pump/probe photoemission. If the probe is applied while the pump is still on, one must ensure that the calculations of the observed photocurrent are gauge invariant. We also discuss the requirement of the photoemission signal to be positive and the relationship of this constraint to gauge invariance. We end by discussing some t…
The sudden photohole of least energy created in the photoemission process is a vibrationally excited state of a small polaron. Therefore the photoemission spectrum in LaMnO3 is predicted to have multiple Franck-Condon vibrational sidebands. This generates an intrinsic line broadening approximately 0.5 eV. The photoemission spectral function has two peaks whose central energies disperse with band width approximately 1.2 eV. Signatures of these phenomena are predicted to appear in angle-resolved photoemission spectra.
In this work, we theoretically examine recent pump/probe photoemission experiments on the strongly correlated charge-density-wave insulator TaS\_2. We describe the general nonequilibrium many-body formulation of time-resolved photoemission in the sudden approximation, and then solve the problem using dynamical mean-field theory with the numerical renormalization group and a bare density of states calculated from density functional theory including the charge-density-wave distortion of the ion cores and spin-orbit coupling We find a number of interesting results: (i) the bare band structure act…
The implications of the angle-resolved photoemission spectroscopy (ARPES) on the issue of spin-charge separation are discussed from the viewpoint of slave-particle RVB theories. It is pointed out that the non-local phase string is essential to reproduce the two-peak structure experimentally observed in SrCuO_2. The comparison between 1D and 2D cases is also made.
We describe different approximations associated with employing a constant matrix element for the coupling of light to multiband electrons in the context of time-resolved angle-resolved photoemission spectroscopy (TR-ARPES). In particular, we demonstrate that the constant matrix approximation only holds for one of the coordinate representations, and changing to other bases, requires including nonconstant corrections to the matrix element. We also discuss some simplifying approximations, where a constant matrix element is employed in multiple bases, and the consequences of this further approxima…
Distinct amplitude mode dynamics upon resonant and off-resonant excitation across the charge density wave energy gap in LaTe3 investigated by time- and angle-resolved photoemission spectroscopy
Time-resolved photoemission experiments can reveal fascinating quantum dynamics of correlated electrons. However, the thermalization of the electronic system is typically so fast that very short probe pulses are necessary to resolve the time evolution of the quantum state, and this leads to poor energy resolution due to the energy-time uncertainty relation. Although the photoemission intensity can be calculated from the nonequilibrium electronic Green functions, the converse procedure is therefore difficult. We analyze a hypothetical time-resolved photoemission experiment on a correlated elect…
The connection between the Fermi surface and charge-density wave (CDW) order is revisited in 2H-TaSe2. Using angle-resolved photoemission spectroscopy, ab initio band structure calculations, and an accurate tight-binding model, we develop the empirical k-resolved susceptibility function, which we use to highlight states that contribute to the susceptibility for a particular q-vector. We show that although the Fermi surface is involved in the peaks in the susceptibility associated with CDW order, it is not through conventional Fermi surface nesting, but rather through finite energy transitions …
Polarization-controlled synchrotron radiation was used to map the electronic structure of buried conducting interfaces of LaAlO$_3$/SrTiO$_3$ in a resonant angle-resolved photoemission experiment. A strong dependence on the light polarization of the Fermi surface and band dispersions is demonstrated, highlighting the distinct Ti 3d orbitals involved in 2D conduction. Samples with different 2D doping levels were prepared and measured by photoemission, revealing different band occupancies and Fermi surface shapes. A direct comparison between the photoemission measurements and advanced first-prin…
We use angle-resolved photoemission spectroscopy to study heavy fermion superconductor Ce2RhIn8. The Fermi surface is rather complicated and consists of several hole and electron pock- ets. We do not observe kz dispersion of Fermi sheets, which is consistent with 2D character of the electronic structure. Comparison of the ARPES data and band structure calculations points to a localized picture of f electrons. Our findings pave the way for understanding the transport and thermodynamical properties of this material.
Spin- and angle-resolved resonant (Ce $4d\to4f$) photoemission spectra of a monolayer Ce on Fe(110) reveal spin-dependent changes of the Fermi-level peak intensities. That indicate a spin-dependence of $4f$ hybridization and, thus, of $4f$ occupancy and local moment. The phenomenon is described in the framework of the periodic Anderson model by $4f$ electron hopping into the exchange split Fe 3d derived bands that form a spin-gap at the Fermi energy around the $\barΓ$ point of the surface Brillouin zone.
Electronic Coulomb correlations lead to characteristic signatures in the spectroscopy of transition metal pnictides and chalcogenides: quasi-particle renormalizations, lifetime effects or incoherent badly metallic behavior above relatively low coherence temperatures are measures of many-body effects due to local Hubbard and Hund's couplings. We review and compare the results of angle-resolved photoemission spectroscopy experiments (ARPES) and of combined density functional dynamical mean field theory (DFT+DMFT) calculations. We emphasize the doping-dependence of the quasi-particle mass renorma…
In connection with the experiment on oxygen isotope effect of Bi2Sr2CaCu2O8 with the angle-resolved photoemission spectroscopy (ARPES), we theoretically study the isotope-induced band shift in ARPES by the Hartree-Fork and quantum Monte Carlo methods. We find that this band shift can be clarified based on a quadratically coupled electron-phonon (e-ph) model. The large ratio of band shift versus phonon energy change is connected with the softening effect of phonon, and the positive-negative sign change is due to the momentum dependence of the e-ph coupling.
We report the electronic structure of a prototypical valence fluctuation system, YbAl2, using angle-resolved photoemission spectroscopy. The observed band dispersions and Fermi surfaces are well described in terms of band structure calculations based on local density approximation. Strong hybridization between the conduction and 4f bands is identified on the basis of the periodic Anderson model. The evaluated small mass enhancement factor and the high Kondo temperature qualitatively agree with those obtained from thermodynamic measurements. Such findings suggest that the strong hybridization s…
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 …
We have performed a high-resolution angle resolved Ce 4$d-4f$ resonant photoemission experiment on the heavy fermion superconductor CeIrIn$_5$. We have observed a quasi-particle band which has an energy dispersion of $\sim 30$ meV in the Ce 4$f$ on-resonance spectra. The result suggests that although the 4$f$ spectra are dominated by the localized/correlated character, the small itinerant component is responsible for the superconductivity in this compound.
We propose angle-resolved two-photon photoemission spectroscopy (AR-2PPES) as a technique to detect the location of the bottom of the upper Hubbard band (UHB) in two-dimensional insulating cuprates. The AR-2PPES spectra are numerically calculated for small Hubbard clusters. When the pump photon excites an electron from the lower Hubbard band, the bottom of the UHB is less clear, but when an electron in the nonbonding oxygen band is excited, the bottom of the UHB can be identified clearly, accompanied with additional spectra originated from the spin-wave excitation at half filling.
In time-resolved photoemission experiments, more than one electron can be emitted from the solid by a single ultra-short pulse. We theoretically demonstrate how correlations between the momenta of outgoing electrons relate to time-dependent two-particle correlations in the solid. This can extend the scope of time- and angular-resolved photoemission spectroscopy to probe superconducting and charge density fluctuations in systems without long-range order, and to reveal their dynamics independent of the electronic gap and thus unrestricted by the energy-time uncertainty. The proposal is illustrat…
The low-energy electronic structure of the J_{eff}=1/2 spin-orbit insulator Sr3Ir2O7 has been studied by means of angle-resolved photoemission spectroscopy. A comparison of the results for bilayer Sr3Ir2O7 with available literature data for the related single-layer compound Sr2IrO4 reveals qualitative similarities and similar J_{eff}=1/2 bandwidths for the two materials, but also pronounced differences in the distribution of the spectral weight. In particuar, photoemission from the J_{eff}=1/2 states appears to be suppressed. Yet, it is found that the Sr3Ir2O7 data are in overall better agreem…
We have investigated the electronic structure of A-site ordered CaCu$_3$Ti$_4$O$_{12}$ as a function of temperature by using angle-integrated and -resolved photoemission spectroscopies. Intrinsic changes of the electronic structure have been successfully observed in the valence band region by the careful consideration of charging effects. The obtained photoemission results have revealed that the intensity of the nearly non-dispersive Cu 3$d$-O 2$p$ hybridized bands at the binding energy of $\sim$2 eV increases with decreasing temperature from 300 to 120 K. This suggests that the density of the…
We have performed an angle-resolved photoemission study of the three-dimensional perovskite-type SrVO$_3$. Observed spectral weight distribution of the coherent part in the momentum space shows cylindrical Fermi surfaces consisting of the V 3$d$ $t_{2g}$ orbitals as predicted by local-density-approximation (LDA) band-structure calculation. The observed energy dispersion shows a moderately enhanced effective mass compared to the LDA results, corresponding to the effective mass enhancement seen in the thermodynamic properties. Contributions from the bulk and surface electronic structures to the …
High resolution spin-resolved photoemission is used to probe the properties of a Gd(0001) surface state. The state shows both a spin-mixing behavior reflecting the exchange of magnons with the local moments and a reduction of the exchange splitting with increasing temperature. The surface state polarization at low T suggests that the surface layer has an enhanced Tc of 365K or greater. Measurements of the photoemission linewidths show that at low temperatures, the lifetime of a majority spin photohole is predominantly limited by electron-phonon scattering and that of a minority spin photohole …
Numerous angle resolved photoemission spectroscopy (ARPES) studies of a wide class of low-density metallic systems, ranging from doped transition metal oxides to quasi two-dimensional interfaces between insulators, exhibit phonon sidebands below the quasi-particle peak as a unique hallmark of polaronic correlations. Here, we single out properties of ARPES spectra that can provide a robust estimate of the effective range (screening length) of the electron-phonon interaction, regardless of the limited experimental resolution, dimensionality and particular features of the electronic structure, fa…
In a high-resolution photoemission study of a Mo(110) surface state various contributions to the measured width and energy of the quasiparticle peak are investigated. Electron-phonon coupling, electron-electron interactions and scattering from defects are all identified mechanisms responsible for the finite lifetime of a valence photo-hole. The electron-phonon induced mass enhancement and rapid change of the photo-hole lifetime near the Fermi level are observed for the first time.
We have performed angle-resolved photoemission spectroscopy (ARPES) experiments on paramagnetic UFeGa5 using soft X-ray synchrotron radiation (hn=500eV) and derived the bulk- and U 5f-sensitive electronic structure of UFeGa5. Although the agreement between the experimental band structure and the LDA calculation treating U 5f electrons as being itinerant is qualitative, the morphology of the Fermi surface is well explained by the calculation, suggesting that the U 5f states can be essentially understood within the itinerant-electron model.
We investigate the temporal evolution of electronic states in strontium iridate Sr$_2$IrO$_4$. The time resolved photoemission spectra of intrinsic, electron doped and the hole doped samples are monitored in identical experimental conditions. Our data on intrinsic and electron doped samples, show that primary doublon-holon pairs relax near to the chemical potential on a timescale shorter than $70$ fs. The subsequent cooling of low energy excitations takes place in two step: a rapid dynamics of $\cong120$ fs is followed by a slower decay of $\cong 1$ ps. The reported timescales endorse the anal…
We have made an angle-resolved photoemission study of a one-dimensional (1D) Mott-Hubbard insulator Na_{0.96}V_{2}O_{5} and found that the spectra of the V 3d lower Hubbard band are strongly dependent on the temperature. We have calculated the one-particle spectral function of the one-dimensional t-J model at finite temperatures by exact diagonalization and compared them with the experimental results. Good overall agreement is obtained between experiment and theory. The strong finite temperature effects are discussed in terms of the existence of the ``Fermi surface'' of the spinon band.
With the current interest in the rare-earth tellurides as high temperature charge density wave materials, a greater understanding of the physics of these systems is needed, particularly in the case of the ditellurides. We report a detailed study of the band structure of LaTe_2 in the charge density wave state using high-resolution angle resolved photoemission spectroscopy (ARPES). From this work we hope to provide insights into the successes and weaknesses of past theoretical study as well as helping to clear up prior ambiguities by providing an experimental basis for future work in the tellur…
Using angle resolved photoemission spectroscopy (ARPES) we report the first band dispersions and distinct features of the bulk Fermi surface (FS) in the paramagnetic metallic phase of the prototypical metal-insulator transition material V$_2$O$_3$. Along the $c$-axis we observe both an electron pocket and a triangular hole-like FS topology, showing that both V 3$d$ $a_{1g}$ and $e_g^π$ states contribute to the FS. These results challenge the existing correlation-enhanced crystal field splitting theoretical explanation for the transition mechanism and pave the way for the solution of this myste…
We have investigated charge dynamics and electronic structures for single crystals of metallic layered nickelates, R2-xSrxNiO4 (R=Nd, Eu), isostructural to La2-xSrxCuO4. Angle-resolved photoemission spectroscopy on the barely-metallic Eu0.9Sr1.1NiO4 (R=Eu, x=1.1) has revealed a large hole surface of x2-y2 character with a high-energy pseudogap of the same symmetry and comparable magnitude with those of underdoped (x<0.1) cuprates, although the antiferromagnetic interactions are one order of magnitude smaller. This finding strongly indicates that the momentum-dependent pseudogap feature in the …
We report the electronic structure of YbB6, a recently predicted moderately correlated topological insulator, measured by angle-resolved photoemission spectroscopy. We directly observed linearly dispersive bands around the time-reversal invariant momenta Γ and X with negligible kz dependence, consistent with odd number of surface states crossing the Fermi level in a Z2 topological insulator. Circular dichroism photoemission spectra suggest that these in-gap states possess chirality of orbital angular momentum, which is related to the chiral spin texture, further indicative of their topological…
The energy-time uncertainty is an intrinsic limit for time-resolved experiments imposing a tradeoff between the duration of the light pulses used in experiments and their frequency content. In standard time-resolved photoemission, this limitation maps directly onto a tradeoff between the time resolution of the experiment and the energy resolution that can be achieved on the electronic spectral function. Here we propose a protocol to disentangle the energy and time resolutions in photoemission. We demonstrate that dynamical information on all time scales can be retrieved from time-resolved phot…
Material line defects are one-dimensional structures but the search and proof of electron behaviour consistent with the reduced dimension of such defects has been so far unsuccessful. Here we show using angle resolved photoemission spectroscopy that twin-grain boundaries in the layered semiconductor MoSe2 exhibit parabolic metallic bands. The one-dimensional nature is evident from a charge density wave transition, whose periodicity is given by kF/π, consistent with scanning tunneling microscopy and angle resolved photoemission measurements. Most importantly, we provide evidence for spin- and c…
We present the first direct study of charge density wave (CDW) formation in quasi-2D single layer LaTe_2 using high-resolution angle resolved photoemission spectroscopy (ARPES) and low energy electron diffraction (LEED). CDW formation is driven by Fermi surface (FS) nesting, however characterized by a surprisingly smaller gap (50meV) than seen in the double layer RTe_3 compounds, extending over the entire FS. This establishes LaTe_2 as the first reported semiconducting 2D CDW system where the CDW phase is FS nesting driven. In addition, the layer dependence of this phase in the tellurides and …
Recent studies suggest that an exemplary Kondo insulator SmB6 belongs to a new class of topological insulators (TIs), in which non-trivial spin-polarized metallic states emerge on surface upon the formation of Kondo hybridization gap in the bulk. Remarkably, the bulk resistivity reaches more than 20 Ohm cm at 4 K, making SmB6 a candidate for a so-called bulk-insulating TI. We here investigate optical-pulse responses of SmB6 by pump-and-probe photoemission spectroscopy. Surface photovoltage effect is observed below ~90 K. This indicates that an optically-active band bending region develops bene…
A first principles approach for spin and angle resolved resonant photoemission is developed within multiple scattering theory and applied to a Cr(110) surface at the 2$p$-3$d$ resonance. The resonant photocurrent from this non ferromagnetic system is found to be strongly spin polarized by circularly polarized light, in agreement with experiments on antiferromagnetic and magnetically disordered systems. By comparing the antiferromagnetic and Pauli-paramagnetic phases of Cr, we explicitly show that the spin polarization of the photocurrent is independent of the existence of local magnetic moment…
A novel method for mapping the local spin and orbital nature of the ground state of a system via corresponding flip excitations in both sectors is proposed based on angle resolved resonant photoemission and related diffraction patterns, presented here for the first time via an ab-initio modified one-step theory of photoemission. The analysis is done on the paradigmatic weak itinerant ferromagnet bcc Fe, whose magnetism, seen as a correlation phenomenon given by the coexistence of localized moments and itinerant electrons, and the non-Fermi liquid behaviour at ambient and extreme conditions bot…
We have performed soft-X-ray angle resolved photoemission for metallic V$_2$O$_3$. Combining a micro focus beam (40 x 65 $μ$m$^2$) and micro positioning techniques with a long working distance microscope, we have succeeded in observing band dispersions from tiny cleavage surfaces with typical size of the several tens of $μ$m. The photoemission spectra show a clear position dependence reflecting the morphology of the cleaved sample surface. By selecting high quality flat regions on the sample surface, we have succeeded in band mapping using both photon-energy and polar-angle dependences, openin…
Recently, the time-reversal violation predicted for the pseudogap phase of the cuprates, which was observed by dichroism experiments using Angle-Resolved Photoemission has also been observed by polarized neutron diffraction. Earlier derivation of dichroism in angle resolved photoemission due to time-reversal violation relied on existence of mirror planes in the crystal. Here the theory of the effect is generalized to the case that mirror plane symmetry is weakly violated due to perturbing potentials such as a superstructure.
The consistency of angle-resolved photoemission and optical conductivity experiments on high temperature superconductors is examined. In the limit (apparently consistent with angle-resolved photoemission data) of an electron self energy with a weak momentum dependence and a strong frequency dependence formulae are derived which directly related quantities measured in the two experiments. Application of the formuale to optimally and overdoped $Bi_{2}Ca_{2}SrCu_{2}O_{8+δ}$ shows that the total self energy inferred from photoemission measurements cannot be interpreted as a transport scattering ra…
High-$T_c$ cuprate superconductors are characterized by a strong momentum-dependent anisotropy between the low energy excitations along the Brillouin zone diagonal (nodal direction) and those along the Brillouin zone face (antinodal direction). Most obvious is the d-wave superconducting gap, with the largest magnitude found in the antinodal direction and no gap in the nodal direction. Additionally, while antinodal quasiparticle excitations appear only below $T_c$, superconductivity is thought to be indifferent to nodal excitations as they are regarded robust and insensitive to $T_c$. Here we r…
Present-day angle-resolved photoemission spectroscopy (ARPES) has offered a tremendous advance in the understanding of electron energy spectra in cuprate superconductors and some related compounds. However, in high magnetic field, magnetic quantum oscillations at low temperatures indicate the existence of small electron (hole) Fermi pockets seemingly missing in ARPES of hole (electron) doped cuprates. Here ARPES and quantum oscillations are reconciled in the framework of an impurity band in the charge-transfer Mott-Hubbard insulator.
In a recent preprint Campuzano et al.(cond-mat/0309402), have questioned the validity of our ARPES results (cond-mat/0305179) contradicting the interpretation of earlier photoemission experiments in terms of the time-reversal symmetry breaking in Bi2212. Here we highlight the principal results of our study and refute all the criticism.
Angle-resolved photoemission spectra present two challenges for the d-density wave (DDW) theory of the pseudogap state of the cuprates: (1) hole pockets near $(π/2,π/2)$ are not observed, in apparent contradiction with the assumption of translational symmetry breaking, and (2) there are no well-defined quasiparticles at the {\it antinodal} points, in contradiction with the predictions of mean-field theory of this broken symmetry state. Here, we show how these puzzles can be resolved.
Time-Resolved Photoemission Spectroscopy of Quantum Materials Using High Harmonic Generation: Probing Electron-Phonon Interactions and Non-Equilibrium Dynamics
This paper summarizes experimental results presented at the international conference honoring Prof. C.N. Yang's 80th birthday. I show seven examples that illustrate how one can use angle-resolved photoemission spectroscopy to gain insights into the many-body physics responsible for the rich phase diagram of cuprate superconductors. I hope to give the reader a snapshot of the evolution of this experimental technique from a tool to study chemical bonds and band structure to an essential many-body spectroscopy for one of the most important physics problems of our time.
Superconducting excitations -- Bogoliubov quasiparticles -- are the quantum mechanical mixture of negatively charged electron (-e) and positively charged hole (+e). We propose a new observable for Angular Resolved Photoemission Spectroscopy (ARPES) studies that is the manifestation of the particle-hole entanglement of the superconducting quasiparticles. We call this observable a {\em Bogoliubov angle}. This angle measures the relative weight of particle and hole amplitude in the superconducting (Bogoliubov) quasiparticle. We show how this quantity can be measured by comparing the ratio of spec…
We amend ab initio strongly-correlated band structures by taking into account the band-tailing phenomenon in doped charge-transfer Mott-Hubbard insulators. We show that the photoemission from band tails accounts for sharp "quasi-particle" peaks, rapid loss of their intensities in some directions of the Brillouin zone ("Fermi-arcs") and high-energy "waterfall" anomalies as a consequence of matrix-element effects of disorder-localised states in the charge-transfer gap of doped cuprates.
Time- and angle-resolved photoemission spectroscopy has played an important role in revealing the non-equilibrium electronic structures of solid-state materials. The implementation of high harmonic generation to obtain a higher photon energy also allows us to investigate the wide Brillouin zone on a time scale below 100 fs. In this article, we review our recent studies using high-harmonic-generation-laser-based time- and angle-resolved photoemission spectroscopy to study a variety of quantum materials. We reveal many unprecedented phenomena in each system and highlight some representative resu…
Techniques in time- and angle-resolved photoemission spectroscopy have facilitated a number of recent advances in the study of quantum materials. We review developments in this field related to the study of incoherent nonequilibrium electron dynamics, the analysis of interactions between electrons and collective excitations, the exploration of dressed-state physics, and the illumination of unoccupied band structure. Future prospects are also discussed.
We develop a novel self-consistent approach for studying the angle resolved photoemission spectra (ARPES) of a hole in the t-J-Holstein model giving perfect agreement with numerically exact Diagrammatic Monte Carlo data at zero temperature for all regimes of electron-phonon coupling. Generalizing the approach to finite temperatures we find that the anomalous temperature dependence of the ARPES in undoped cuprates is explained by cooperative interplay of coupling of the hole to magnetic fluctuations and strong electron-phonon interaction.
In order to determine the orbital characters on the various Fermi surface pockets of the Fe-based superconductors Ba$_{0.6}$K$_{0.4}$Fe$_{2}$As$_{2}$ and FeSe$_{0.45}$Te$_{0.55}$, we introduce a method to calculate photoemission matrix elements. We compare our simulations to experimental data obtained with various experimental configurations of beam orientation and light polarization. We show that the photoemission intensity patterns revealed from angle-resolved photoemission spectroscopy measurements of Fermi surface mappings and energy-momentum plots along high-symmetry lines exhibit asymmet…
We develop a path-integral theory to study the angle-resolved photoemission spectra (ARPES) of high-T_c superconductors based on a two-dimensional model for the CuO2 conduction plane, including both electron-electron (e-e) and electron-phonon (e-ph) interactions. Comparing our result with the experimental one of Bi2Sr2CaCu2O8, we find that the experimentally observed isotopic band shift in ARPES is due to the off-diagonal quadratic e-ph coupling, whereas the presence of e-e repulsion partially suppresses this effect.
A recent letter by Xue et al. (PRL v.83, 1235 ('99)) reports a Fermi-Liquid (FL) angle resolved photoemission (ARPES) lineshape for quasi one-dimensional Li0.9Mo6O17, contradicting our report (PRL v.82, 2540 ('99)) of a non-FL lineshape in this material. Xue et al. attributed the difference to the improved angle resolution. In this comment, we point out that this reasoning is flawed. Rather, we find that their data have fundamental differences from other ARPES results and also band theory.
