Search

The cuprate high-temperature superconductors exhibit many unexplained electronic phases, but it was often thought that the superconductivity at sufficiently high doping is governed by conventional mean-field Bardeen-Cooper-Schrieffer (BCS) theory[1]. However, recent measurements show that the number of paired electrons (the superfluid density) vanishes when the transition temperature Tc goes to zero[2], in contradiction to expectation from BCS theory. The origin of this anomalous vanishing is unknown. Our scanning tunneling spectroscopy measurements in the overdoped regime of the (Pb,Bi)2Sr2CuO6+{\delta} high-temperature superconductor show that it is due to the emergence of puddled superconductivity, featuring nanoscale superconducting islands in a metallic matrix[3,4]. Our measurements further reveal that this puddling is driven by gap filling, while the gap itself persists beyond the breakdown of superconductivity. The important implication is that it is not a diminishing pairing interaction that causes the breakdown of superconductivity. Unexpectedly, the measured gap-to-filling correlation also reveals that pair-breaking by disorder does not play a dominant role and that the mechanism of superconductivity in overdoped cuprate superconductors is qualitatively different from conventional mean-field theory.

We report charge-transfer up to a single electron per interfacial unit cell across non-polar heterointerfaces from the Mott insulator LaTiO3 to the charge transfer insulator LaCoO3. In high-quality bi- and tri-layer systems grown using pulsed laser deposition, soft X-ray absorption, dichroism and STEM-EELS are used to probe the cobalt 3d-electron count and provide an element-specific investigation of the magnetic properties. The experiments prove a deterministically-tunable charge transfer process acting in the LaCoO3 within three unit cells of the heterointerface, able to generate full conversion to 3d7 divalent Co, which displays a paramagnetic ground state. The number of LaTiO3 / LaCoO3 interfaces, the thickness of an additional "break" layer between the LaTiO3 and LaCoO3, and the LaCoO3 film thickness itself in tri-layers provide a trio of sensitive control knobs for the charge transfer process, illustrating the efficacy of O2p-band alignment as a guiding principle for property design in complex oxide heterointerfaces.

The field of topological materials science has recently been focussing on three-dimensional Dirac semimetals, which exhibit robust Dirac phases in the bulk. However, the absence of characteristic surface states in accidental Dirac semimetals (DSM) makes it difficult to experimentally verify claims about the topological nature using commonly used surface-sensitive techniques. The chiral magnetic effect (CME), which originates from the Weyl nodes, causes an $\textbf{E}\cdot\textbf{B}$-dependent chiral charge polarization, which manifests itself as negative magnetoresistance. We exploit the extended lifetime of the chirally polarized charge and study the CME through both local and non-local measurements in Hall bar structures fabricated from single crystalline flakes of the DSM Bi$_{0.97}$Sb$_{0.03}$. From the non-local measurement results we find a chiral charge relaxation time which is over one order of magnitude larger than the Drude transport lifetime, underlining the topological nature of Bi$_{0.97}$Sb$_{0.03}$., Comment: 6 pages, 6 figures + 7 pages of supplemental material

VO2 is a much-discussed material for oxide electronics and neuromorphic computing applications. Here, heteroepitaxy of vanadium dioxide (VO2) was realized on top of oxide nanosheets that cover either the amorphous silicon dioxide surfaces of Si substrates or X-ray transparent silicon nitride membranes. The out-of-plane orientation of the VO2 thin films was controlled at will between (011)M1/(110)R and (-402)M1/(002)R by coating the bulk substrates with Ti0.87O2 and NbWO6 nanosheets, respectively, prior to VO2 growth. Temperature dependent X-ray diffraction and automated crystal orientation mapping in microprobe TEM mode (ACOM-TEM) characterized the high phase purity, the crystallographic and orientational properties of the VO2 films. Transport measurements and soft X-ray absorption in transmission are used to probe the VO2 metal-insulator transition, showing results of a quality equal to those from epitaxial films on bulk single-crystal substrates. Successful local manipulation of two different VO2 orientations on a single substrate is demonstrated using VO2 grown on lithographically-patterned lines of Ti0.87O2 and NbWO6 nanosheets investigated by electron backscatter diffraction. Finally, the excellent suitability of these nanosheet-templated VO2 films for advanced lensless imaging of the metal-insulator transition using coherent soft X-rays is discussed.

The quantum Hall effect is studied in the topological insulator BiSbTeSe$_2$. By employing top- and back-gate electric fields at high magnetic field, the Landau levels of the Dirac cones in the top and bottom topological surface states can be tuned independently. When one surface is tuned to the electron-doped side of the Dirac cone and the other surface to the hole-doped side, the quantum Hall edge channels are counter-propagating. The opposite edge mode direction, combined with the opposite helicities of top and bottom surfaces, allows for scattering between these counter-propagating edge modes. The total Hall conductance is integer valued only when the scattering is strong. For weaker interaction, a non-integer quantum Hall effect is expected and measured.

The combination of superconductivity and the helical spin-momentum locking at the surface state of a topological insulator (TI) has been predicted to give rise to p-wave superconductivity and Majorana bound states. The superconductivity can be induced by the proximity effect of a an s-wave superconductor (S) into the TI. To probe the superconducting correlations inside the TI, dI/dV spectroscopy has been performed across such S-TI interfaces. Both the alloyed Bi$_{1.5}$Sb$_{0.5}$Te$_{1.7}$Se$_{1.3}$ and the stoichiometric BiSbTeSe$_2$ have been used as three dimensional TI. In the case of Bi$_{1.5}$Sb$_{0.5}$Te$_{1.7}$Se$_{1.3}$, the presence of disorder induced electron-electron interactions can give rise to an additional zero-bias resistance peak. For the stoichiometric BiSbTeSe$_2$ with less disorder, tunnel barriers were employed in order to enhance the signal from the interface. The general observations in the spectra of a large variety of samples are conductance dips at the induced gap voltage, combined with an increased sub-gap conductance, consistent with p-wave predictions. The induced gap voltage is typically smaller than the gap of the Nb superconducting electrode, especially in the presence of an intentional tunnel barrier. Additional uncovered spectroscopic features are oscillations that are linearly spaced in energy, as well as a possible second order parameter component., Comment: Semiconductor Science and Technology; Special Issue on Hybrid Quantum Materials and Devices

Electrons in a Dirac semimetals possess linear dispersion in all three spatial dimensions, and form part of a developing platform of novel quantum materials. Bi$_{1-x}$Sb$_x$ supports a three-dimensional Dirac cone at the Sb-induced band inversion point. Nanoscale phase-sensitive junction technology is used to induce superconductivity in this Dirac semimetal. Radio frequency irradiation experiments reveal a significant contribution of 4$\pi$-periodic Andreev bound states to the supercurrent in Nb-Bi$_{0.97}$Sb$_{0.03}$-Nb Josephson junctions. The conditions for a substantial $4\pi$ contribution to the supercurrent are favourable because of the Dirac cone's topological protection against backscattering, providing very broad transmission resonances. The large g-factor of the Zeeman effect from a magnetic field applied in the plane of the junction, allows tuning of the Josephson junctions from 0 to $\pi$ regimes., Comment: Supplementary information is included

Atomic nanowires on semiconductor surfaces induced by the adsorption of metallic atoms have attracted a lot of attention as possible hosts of the elusive, Tomonaga-Luttinger liquid. The Au/Ge(100) system in particular is the subject of controversy as to whether the Au-induced nanowires do indeed host exotic, 1D metallic states. We report on a thorough study of the electronic properties of high quality nanowires formed at the Au/Ge(100) surface. High resolution ARPES data show the low-lying Au-induced electronic states to possess a dispersion relation that depends on two orthogonal directions in k-space. Comparison of the E(k$_x$,k$_y$) surface measured using ARPES to tight-binding calculations yields hopping parameters in the two different directions that differ by a factor of two. We find that the larger of the two hopping parameters corresponds, in fact, to the direction perpendicular to the nanowires (t$_{\perp}$). This, the topology of the $E$=$E_F$ contour in k$_{\||}$, and the fact that $t_{\||}$/$t_{\perp}\sim 0.5$ proves that the Au-induced electron pockets possess a 2D, closed Fermi surface, this firmly places the Au/Ge(100) nanowire system outside being a potential hosts of a Tomonaga-Luttinger liquid. We combine these ARPES data with STS measurements of the spatially-resolved electronic structure and find that the spatially straight conduction channels observed up to energies of order one electron volt below the Fermi level do not originate from the Au-induced states seen in the ARPES data. The former are more likely to be associated with bulk Ge states that are localized to the subsurface region. Despite our proof of the 2D nature of the Au-induced nanowire and sub-surface Ge-related states, an anomalous suppression of the density of states at the Fermi level is observed in both the STS and ARPES data, this phenomenon is discussed in the light of the effects of disorder., Comment: 17 pages, 8 figures

Strong electron correlations in rare earth hexaborides can give rise to a variety of interesting phenomena like ferromagnetism, Kondo hybridization, mixed valence, superconductivity and possibly topological characteristics. The theoretical prediction of topological properties in SmB$_{6}$ and YbB$_{6}$, has rekindled the scientific interest in the rare earth hexaborides, and high-resolution ARPES has been playing a major role in the debate. The electronic band structure of the hexaborides contains the key to understand the origin of the different phenomena observed, and much can be learned by comparing the experimental data from different rare earth hexaborides. We have performed high-resolution ARPES on the (001) surfaces of YbB$_{6}$, CeB$_{6}$ and SmB$_{6}$. On the most basic level, the data show that the differences in the valence of the rare earth element are reflected in the experimental electronic band structure primarily as a rigid shift of the energy position of the metal 5$\textit{d}$ states with respect to the Fermi level. Although the overall shape of the $\textit{d}$-derived Fermi surface contours remains the same, we report differences in the dimensionality of these states between the compounds studied. Moreover, the spectroscopic fingerprint of the 4$\textit{f}$ states also reveals considerable differences that are related to their coherence and the strength of the $\textit{d}$-$\textit{f}$ hybridization. For the SmB$_6$ case, we use ARPES in combination with STM imaging and electron diffraction to reveal time dependent changes in the structural symmetry of the highly debated SmB$_{6}$(001) surface. All in all, our study highlights the suitability of electron spectroscopies like high-resolution ARPES to provide links between electronic structure and function in complex and correlated materials such as the rare earth hexaborides., Comment: 10 pages, 5 figures

Topological insulators are a novel materials platform with high applications potential in fields ranging from spintronics to quantum computation. In the ongoing scientific effort to demonstrate controlled manipulation of their electronic structure by external means, stoichiometric variation and surface decoration are two effective approaches that have been followed. In ARPES experiments, both approaches are seen to lead to electronic band structure changes. Such approaches result in variations of the energy position of bulk and surface-related features and the creation of two-dimensional electron gases.The data presented here demonstrate that a third manipulation handle is accessible by utilizing the amount of illumination a topological insulator surface has been exposed to under typical experimental ARPES conditions. Our results show that this new, third, knob acts on an equal footing with stoichiometry and surface decoration as a modifier of the electronic band structure, and that it is in continuous competition with the latter. The data clearly point towards surface photovoltage and photo-induced desorption as the physical phenomena behind modifications of the electronic band structure under exposure to high-flux photons. We show that the interplay of these phenomena can minimize and even eliminate the adsorbate-related surface band bending on typical binary, ternary and quaternary Bi-based topological insulators. Including the influence of the sample temperature, these data set up a framework for the external control of the electronic band structure in topological insulator compounds in an ARPES setting. Four external knobs are available: bulk stoichiometry, surface decoration, temperature and photon exposure. These knobs can be used in conjunction to tune the band energies near the surface and consequently influence the topological properties of the relevant electronic states., Comment: 16 pages, 8 figures

In an ideal 3D topological insulator (TI), the bulk is insulating and the surface conducting due to the existence of metallic states that are localized on the surface; these are the topological surface states. Quaternary Bi-based compounds of Bi$_{2-x}$Sb$_{x}$Te$_{3-y}$Se$_{y}$ with finely-tuned bulk stoichiometries are good candidates for realizing ideal 3D TI behavior due to their bulk insulating character. However, despite its insulating bulk in transport experiments, the surface region of Bi$_{2-x}$Sb$_{x}$Te$_{3-y}$Se$_{y}$ crystals cleaved in ultrahigh vacuum also exhibits occupied states originating from the bulk conduction band. This is due to adsorbate-induced downward band-bending, a phenomenon known from other Bi-based 3D TIs. Here we show, using angle-resolved photoemission, how an EUV light beam of moderate flux can be used to exclude these topologically trivial states from the Fermi level of Bi$_{1.46}$Sb$_{0.54}$Te$_{1.7}$Se$_{1.3}$ single crystals, thereby re-establishing the purely topological character of the low lying electronic states of the system. We furthermore prove that this process is highly local in nature in this bulk-insulating TI, and are thus able to imprint structures in the spatial energy landscape at the surface. We illustrate this by `writing' micron-sized letters in the Dirac point energy of the system., Comment: 7 pages, 3 figures, includes Supplementary Information

We report high resolution Angle Resolved PhotoElectron Spectroscopy (ARPES) results on the (001) cleavage surface of YbB$_{6}$, a rare-earth compound which has been recently predicted to host surface electronic states with topological character. We observe two types of well-resolved metallic states, whose Fermi contours encircle the time-reversal invariant momenta of the YbB$_{6}$(001) surface Brillouin zone, and whose full (E,$k$)-dispersion relation can be measured wholly unmasked by states from the rest of the electronic structure. Although the two-dimensional character of these metallic states is confirmed by their lack of out-of-plane dispersion, two new aspects are revealed in these experiments. Firstly, these states do not resemble two branches of opposite, linear velocity that cross at a Dirac point, but rather straightforward parabolas which terminate to high binding energy with a clear band bottom. Secondly, these states are sensitive to time-dependent changes of the YbB$_{6}$ surface under ultrahigh vacuum conditions. Adding the fact that these data from cleaved YbB$_{6}$ surfaces also display spatial variations in the electronic structure, it appears there is little in common between the theoretical expectations for an idealized YbB$_{6}$(001) crystal truncation on the one hand, and these ARPES data from real cleavage surfaces on the other., Comment: 8 pages, 4 figures (accepted in Physical Review B)

Low energy electron diffraction (LEED) experiments, LEED simulations and finite slab density functional calculations are combined to study the cleavage surface of Co doped BaFe_{2-x}Co_{x}As_{2} (x = 0.1, 0.17). We demonstrate that the energy dependence of the LEED data can only be understood from a terminating 1/2 Ba layer accompanied by distortions of the underlying As-Fe_2-As block. As a result, surface related Fe 3d states are present in the electronic structure, which we identify in angle resolved photoemission experiments. The close proximity of the surface-related states to the bulk bands inevitably leads to broadening of the ARPES signals, which excludes the use of the BaFe_{2-x}Co_{x}As_{2} system for accurate determination of self-energies using ARPES., Comment: 4 pages, 5 figures includes supplementary material

The electronic structure of YBa2Cu3O6+x and La2-xSrxCuO4 for various values of x has been investigated using hard x-ray photoemission spectroscopy. The experimental results establish that the cleaving of YBa2Cu3O6+x compounds occurs predominantly in the BaCuO3 complex leading to charged surfaces at higher x and to uncharged surfaces at lower x values. The bulk component of the core level spectra exhibits a shift in binding energy as a function of x, from which a shift of the chemical potential as a function of hole concentration in the CuO2 layers could be derived. The doping dependence of the chemical potential across the transition from a Mott-Hubbard insulator to a Fermi-liquid-like metal is very different in these two series of compounds. In agreement with previous studies in the literature the chemical potential shift in La2-xSrxCuO4 is close to zero for small hole concentrations. In YBa2Cu3O6+x, similar to all other doped cuprates studied so far, a strong shift of the chemical potential at low hole doping is detected. However, the results for the inverse charge susceptibility at small x shows a large variation between different doped cuprates. The results are discussed in view of various theoretical models. None of these models turns out to be satisfactory., Comment: 18 pages, 15 figures

We report studies of the electronic structure and elementary excitations of doped and undoped cuprate chains, ladders and planes. Using high energy spectroscopies such as x-ray absorption, core level photoemission and angle resolved photoemission spectroscopy, important information regarding the charge distribution and hole dynamics can be obtained. The comparison of the experimental data with suitable theoretical models sets constraints on the parameters entering into the model calculations, and offers insight into the important physical quantities governing the electronic structure of these materials. Recurring themes include the importance of the dimensionality of the Cu-O network (1D->2D) and the crucial role played by the spin-background in determining the dynamics of low-lying excitations in these strongly correlated systems., Comment: J. Electron Spec. Relat. Phenom.: special issue on electron correlation, in press