A Kondo lattice is often electrically insulating at low temperatures. However, several recent experiments have detected signatures of bulk metallicity within this Kondo insulating phase. In this study, we visualized the real-space charge landscape within a Kondo lattice with atomic resolution using a scanning tunneling microscope. We discovered nanometer-scale puddles of metallic conduction electrons centered around uranium-site substitutions in the heavy-fermion compound uranium ruthenium silicide (URu2Si2) and around samarium-site defects in the topological Kondo insulator samarium hexaboride (SmB6). These defects disturbed the Kondo screening cloud, leaving behind a fingerprint of the metallic parent state. Our results suggest that the three-dimensional quantum oscillations measured in SmB6 arise from Kondo-lattice defects, although we cannot exclude other explanations. Our imaging technique could enable the development of atomic-scale charge sensors using heavy-fermion probes.
Doped Mott insulators are the starting point for interesting physics such as high temperature superconductivity and quantum spin liquids. For multi-band Mott insulators, orbital selective ground states have been envisioned. However, orbital selective metals and Mott insulators have been difficult to realize experimentally. Here we demonstrate by photoemission spectroscopy how Ca 2 RuO 4 , upon alkali-metal surface doping, develops a single-band metal skin. Our dynamical mean field theory calculations reveal that homogeneous electron doping of Ca 2 RuO 4 results in a multi-band metal. All together, our results provide evidence for an orbital-selective Mott insulator breakdown, which is unachievable via simple electron doping. Supported by a cluster model and cluster perturbation theory calculations, we demonstrate a type of skin metal-insulator transition induced by surface dopants that orbital-selectively hybridize with the bulk Mott state and in turn produce coherent in-gap states.
CeBi has an intricate magnetic phase diagram whose fully-polarized state has recently been suggested as a Weyl semimetal, though the role of $f$ states in promoting strong interactions has remained elusive. Here we focus on the less-studied, but also time-reversal symmetry-breaking ferrimagnetic phase of CeBi, where our density functional theory (DFT) calculations predict additional Weyl nodes near the Fermi level $E_\mathrm{F}$. We use spin-polarized scanning tunneling microscopy and spectroscopy to image the surface ferrimagnetic order on the itinerant Bi $p$ states, indicating their orbital hybridization with localized Ce $f$ states. We observe suppression of this spin-polarized signature at $E_\mathrm{F}$, coincident with a Fano line shape in the conductance spectra, suggesting the Bi $p$ states partially Kondo screen the $f$ magnetic moments, and this $p-f$ hybridization causes strong Fermi-level band renormalization. The $p$ band flattening is supported by our quasiparticle interference (QPI) measurements, which also show band splitting in agreement with DFT, painting a consistent picture of a strongly interacting magnetic Weyl semimetal.
Monolayer FeSe on SrTiO3 superconducts with reported Tc as high as 100 K, but the dramatic interfacial Tc enhancement remains poorly understood. Oxygen vacancies in SrTiO3 are known to enhance the interfacial electron doping, electron-phonon coupling, and superconducting gap, but the detailed mechanism is unclear. Here we apply scanning transmission electron microscopy (STEM) and electron energy loss spectroscopy (EELS) to FeSe/SrTiO3 to image the diffusion of selenium into SrTiO3 to an unexpected depth of several unit cells, consistent with the simultaneously observed depth profile of oxygen vacancies. Our density functional theory (DFT) calculations support the crucial role of oxygen vacancies in facilitating the thermally driven Se diffusion. In contrast to excess Se in the FeSe monolayer or FeSe/SrTiO3 interface that is typically removed during post-growth annealing, the diffused Se remains in the top few unit cells of the SrTiO3 bulk after the extended post-growth annealing that is necessary to achieve superconductivity. Thus the unexpected Se in SrTiO3 may contribute to the interfacial electron doping and electron-phonon coupling that enhance Tc, suggesting another important role for oxygen vacancies as facilitators of Se diffusion.
We have carried out a comprehensive high-resolution angle-resolved photoemission spectroscopy (ARPES) study of the pseudogap interplay with superconductivity in La-based cuprates. The three systems La$_{2-x}$Sr$_x$CuO$_4$, La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$, and La$_{1.8-x}$Eu$_{0.2}$Sr$_x$CuO$_4$ display slightly different pseudogap critical points in the temperature versus doping phase diagram. We have studied the pseudogap evolution into the superconducting state for doping concentrations just below the critical point. In this setting, near optimal doping for superconductivity and in the presence of the weakest possible pseudogap, we uncover how the pseudogap is partially suppressed inside the superconducting state. This conclusion is based on the direct observation of a reduced pseudogap energy scale and re-emergence of spectral weight suppressed by the pseudogap. Altogether these observations suggest that the pseudogap phenomenon in La-based cuprates is in competition with superconductivity for anti-nodal spectral weight.
The interplay between structural and electronic phases in iron-based superconductors is a central theme in the search for the superconducting pairing mechanism. While electronic nematicity is competing with superconductivity, the effect of purely structural orthorhombic order is unexplored. Here, using x-ray diffraction and angle-resolved photoemission spectroscopy, we reveal a structural orthorhombic phase in the electrondoped iron-pnictide superconductor Pr4Fe2As2Te0.88O4 (T-c = 25 K), which is distinct from orthorhombicity in the nematic phase in underdoped pnictides. Despite the high electron doping we find an exceptionally high orthorhombic onset temperature (T-ort similar to 250 K), no signatures of phase competition with superconductivity, and absence of electronic nematic order as the driving mechanism for orthorhombicity. Combined, our results establish a high-temperature phase in the phase diagram of iron-pnictide superconductors and impose strong constraints for the modeling of their superconducting pairing mechanism.
Angle-resolved photoemission spectroscopy, visualizing the superconducting gap in k -space, plays a pivotal role in research on cuprates and other high- T c superconducting materials. However, there has always been an imminent doubt whether this technique truly represents the intrinsic bulk spectral function, whose response can be distorted by energy- and k -dependence of the photoexcitation matrix element, and by a small photoelectron escape depth of few surface atomic layers. Here, we address this fundamental question with soft-X-ray photoemission measurements of the superconducting gap in the paradigm high- T c cuprate Bi 2 Sr 2 CaCu 2 O 8 . We vary the matrix element by spanning a dense k -space grid, formed by the lattice superstructure, and the probing depth by changing the emission angle. The measured gap appears independent of the matrix element effects, probing depth or photoexcitation energy. This fact proves the relevance of photoemission studies for the bulk superconductivity in Bi 2 Sr 2 CaCu 2 O 8 , and calls for similar verification experiments on other high- T c compounds, in particular more three-dimensional ones. Bi 2 Sr 2 CaCu 2 O 8 shows an anomalously fast decay of the coherent spectral weight with photon energy, tracing back to strong electron–phonon interaction or relaxation of the lattice coherence.
We present a combined soft x-ray and high-resolution vacuum-ultraviolet angle-resolved photoemission spectroscopy study of the electron-overdoped cuprate Pr1.3-xLa0.7CexCuO4 (PLCCO). Demonstration of its highly two-dimensional band structure enabled precise determination of the in-plane self-energy dominated by electron-electron scattering. Through analysis of this self-energy and the Fermi liquid cut-off energy scale, we find-in contrast to hole-doped cuprates-a momentum isotropic and comparatively weak electron correlation in PLCCO. Yet, the self-energies extracted from multiple oxide systems combine to demonstrate a logarithmic divergent relation between the quasiparticle scattering rate and mass. This constitutes a spectroscopic version of the Kadowaki-Woods relation with an important merit-the demonstration of Fermi liquid quasiparticle lifetime and mass being set by a single energy scale.
We predict that CeBi in the ferromagnetic state is a Weyl semimetal. Our calculations within density functional theory show the existence of two pairs of Weyl nodes on the momentum path $(0, 0, k_z)$ at $15$ meV} above and $100$ meV below the Fermi level. Two corresponding Fermi arcs are obtained on surfaces of mirror-symmetric (010)-oriented slabs at $E=15$ meV and both arcs are interrupted into three segments due to hybridization with a set of trivial surface bands. By studying the spin texture of surface states, we find the two Fermi arcs are strongly spin-polarized but in opposite directions, which can be detected by spin-polarized ARPES measurements. Our theoretical study of quasiparticle interference (QPI) for a nonmagnetic impurity at the Bi site also reveals several features related to the Fermi arcs. Specifically, we predict that the spin polarization of the Fermi arcs leads to a bifurcation-shaped feature only in the spin-dependent QPI spectrum, serving as a fingerprint of the Weyl nodes.
We use resonant inelastic x-ray scattering to investigate charge-stripe correlations in La_1.675Eu_0.2Sr_0.125CuO_4. By differentiating elastic from inelastic scattering, it is demonstrated that charge-stripe correlations precede both the structural low-temperature tetragonal phase and the transport-defined pseudogap onset. The scattering peak amplitude from charge stripes decays approximately as T^-2 towards our detection limit. The in-plane integrated intensity, however, remains roughly temperature independent. Therefore, although the incommensurability shows a remarkably large increase at high temperature, our results are interpreted via a single scattering constituent. In fact, direct comparison to other stripe-ordered compounds (La_1.875Ba_0.125CuO_4, La_1.475Nd_0.4Sr_0.125CuO_4 and La_1.875Sr_0.125CuO_4) suggests a roughly constant integrated scattering intensity across all these compounds. Our results therefore provide a unifying picture for the charge-stripe ordering in La-based cuprates. As charge correlations in La_1.675Eu_0.2Sr_0.125CuO_4 extend beyond the low-temperature tetragonal and pseudogap phase, their emergence heralds a spontaneous symmetry breaking in this compound.
We predict that CeBi in the ferromagnetic state is a Weyl semimetal. Our calculations within density functional theory show the existence of two pairs of Weyl nodes on the momentum path (0, 0, k(z)) at 15 meV above and 100 meV below the Fermi level. Two corresponding Fermi arcs are obtained on surfaces of mirror-symmetric (010)-oriented slabs at E = 15 meV and both arcs are interrupted into three segments due to hybridization with a set of trivial surface bands. By studying the spin texture of surface states, we find the two Fermi arcs are strongly spin polarized but in opposite directions, which can be detected by spin-polarized ARPES measurements. Our theoretical study of quasiparticle interference (QPI) for a nonmagnetic impurity at the Bi site also reveals several features related to the Fermi arcs. Specifically, we predict that the spin polarization of the Fermi arcs leads to a bifurcation-shaped feature only in the spin-dependent QPI spectrum, serving as a fingerprint of the Weyl nodes.
The Kondo insulator ${\mathrm{SmB}}_{6}$ has emerged as a primary candidate for exotic quantum phases, due to the predicted formation of strongly correlated, low-velocity topological surface states and corresponding high Fermi-level density of states. However, measurements of the surface-state velocity in ${\mathrm{SmB}}_{6}$ differ by orders of magnitude, depending on the experimental technique used. Here we reconcile two techniques, scanning tunneling microscopy (STM) and angle-resolved photoemission spectroscopy (ARPES), by accounting for surface band bending on polar terminations. Using spatially resolved scanning tunneling spectroscopy, we measure a band shift of $\ensuremath{\sim}20$ meV between full-Sm and half-Sm terminations, in qualitative agreement with our density-functional theory calculations of the surface charge density. Furthermore, we reproduce the apparent high-velocity surface states reported by ARPES by simulating their observed spectral function as an equal-weight average over the two band-shifted domains that we image by STM. Our results highlight the necessity of local measurements to address inhomogeneously terminated surfaces or fabrication techniques to achieve uniform termination for meaningful large-area surface measurements of polar crystals such as ${\mathrm{SmB}}_{6}$.
A comprehensive angle-resolved photoemission spectroscopy study of the band structure in singlelayer cuprates is presented with the aim of uncovering universal trends across different materials. Five different hole-and electron-overdoped cuprate superconductors (La1.59Eu0.2Sr0.21CuO4, La1.77Sr0.23CuO4, Bi1.74Pb0.38Sr1.88CuO6+delta, Tl2Ba2CuO6+delta, and Pr1.15La0.7Ce0.15CuO4) have been studied with special focus on the bands with a predominately d-orbital character. Using a light polarization analysis, the e(g) and t(2g) bands are identified across these materials. A clear correlation between the d(3z2-r2) band energy and the apical oxygen distance d(A) is demonstrated. Moreover, the compound dependence of the d(x2-y2) band bottom and the t(2g) band top is revealed. A direct comparison to density functional theory (DFT) calculations employing hybrid exchange-correlation functionals demonstrates excellent agreement. We thus conclude that the DFT methodology can be used to describe the global band structure of overdoped single-layer cuprates on both the hole-and electron-doped side.