Evidence for Weakly Correlated Oxygen Holes in the Highest-T_{c} Cuprate Superconductor HgBa_{2}Ca_{2}Cu_{3}O_{8+δ}.

We study the electronic structure of HgBa_{2}Ca_{2}Cu_{3}O_{8+δ} (Hg1223; T_{c}=134 K) using photoemission spectroscopy (PES) and x-ray absorption spectroscopy (XAS). Resonant valence band PES across the O K edge and Cu L edge identifies correlation satellites originating in O 2p and Cu 3d two-hole final states, respectively. Analyses using the experimental O 2p and Cu 3d partial density of states show quantitatively different on-site Coulomb energy for the Cu site (U_{dd}=6.5±0.5 eV) and O site (U_{pp}=1.0±0.5 eV). Cu_{2}O_{7}-cluster calculations with nonlocal screening explain the Cu 2p core level PES and Cu L-edge XAS spectra, confirm the U_{dd} and U_{pp} values, and provide evidence for the Zhang-Rice singlet state in Hg1223. In contrast to other hole-doped cuprates and 3d-transition metal oxides, the present results indicate weakly correlated oxygen holes in Hg1223.

Ultrafast Atomic Diffusion Inducing a Reversible (2sqrt[3]×2sqrt[3])R30°â†”(sqrt[3]×sqrt[3])R30° Transition on Sn/Si(111)∶B.

Dynamical phase transitions are a challenge to identify experimentally and describe theoretically. Here, we study a new reconstruction of Sn on silicon and observe a reversible transition where the surface unit cell divides its area by a factor of 4 at 250 °C. This phase transition is explained by the 24-fold degeneracy of the ground state and a novel diffusive mechanism, where four Sn atoms arranged in a snakelike cluster wiggle at the surface exploring collectively the different quantum mechanical ground states.

Understanding the insulating nature of alkali-metal/Si(111):B interfaces.

We have recently revisited the phase diagram of alkali-metal/Si(111):B semiconducting interfaces previously suggested as the possible realization of a Mott-Hubbard insulator on a triangular lattice. The insulating character of the 2√[3] × 2√[3]R30 surface reconstruction observed at the saturation coverage, i.e. 0.5 ML, has been shown to find its origin in a giant alkali-metal-induced vertical distortion. Low energy electron diffraction, photoemission spectroscopy and scanning tunneling microscopy and spectroscopy experiments coupled with linear augmented plane-wave density functional theory calculations allow a full understanding of the k-resolved band structure, explaining both the inhomogeneous charge transfers into an Si-B hybridized surface state and the opening of a band gap larger than 1 eV. Moreover, √[3] × âˆš[3]R30, 3 × 3 and 2√[3] × 2√[3]R30 surface reconstructions observed as a function of coverage may reveal a filling-controlled transition from a half-filled correlated magnetic material to a strongly distorted band insulator at saturation.

Giant alkali-metal-induced lattice relaxation as the driving force of the insulating phase of alkali-metal/Si(111):B.

Ab initio density-functional theory calculations, photoemission spectroscopy (PES), scanning tunneling microscopy, and spectroscopy (STM, STS) have been used to solve the 2sqrt[3]×2sqrt[3]R30 surface reconstruction observed previously by LEED on 0.5 ML K/Si:B. A large K-induced vertical lattice relaxation occurring only for 3/4 of Si adatoms is shown to quantitatively explain both the chemical shift of 1.14 eV and the ratio 1/3 measured on the two distinct B 1s core levels. A gap is observed between valence and conduction surface bands by ARPES and STS which is shown to have mainly a Si-B character. Finally, the calculated STM images agree with our experimental results. This work solves the controversy about the origin of the insulating ground state of alkali-metal/Si(111):B semiconducting interfaces which were believed previously to be related to many-body effects.

Phonon contribution to the lifetime of surface state quasiparticles confined in nanopyramids.

We present a scanning tunneling microscopy investigation of the dynamics of hot electrons and holes in Ag pyramidal nanostructures. The geometry of the nanostructure leads to a strong reduction of the decay mechanism into the bulk states and then to a large reflection coefficient of the surface electronic waves. Therefore, in contrast to quantum corrals and adatom islands which show a dominant lossy scattering contribution to the linewidth, the narrow observed structures in the differential conductivity spectra reveal the expected linewidth minimum at the Fermi energy. The electron-phonon contribution to the lifetime is shown to be dominant, in agreement with previous photoemission measurements.

Surface-state bipolaron formation on a triangular lattice in the sp-type alkali-metal/Si(111) Mott insulator.

We report on new low-energy electron diffraction, scanning tunneling microscopy, and angle-resolved photoemission spectroscopy studies of alkali-metal/Si(111) previously established as having a Mott-insulating ground state at surface. The observation of a strong temperature dependent Franck-Condon broadening of the surface band together with the novel sqrt[3] x sqrt[3] --> 2(sqrt[3] x sqrt[3]) charge and lattice ordering below 270 K evidence a surface charge density wave in the strong electron-phonon coupling limit (g approximately 8). Both the adiabatic ratio variant Planck's over 2piomega_{0}/t approximately 0.8 and the effective pairing energy V_{eff} = U - 2gvariant Planck's over 2piomega_{0} approximately -800 meV are consistent with the possible formation of a bipolaronic insulating phase consisting of alternating doubly occupied and unoccupied dangling bonds as expected in the Holstein-Hubbard model.

Structural origin of the Sn 4d core level line shape in Sn/Ge(111)-(3x3).

High-resolution photoemission of the Sn 4d core level of Sn/Ge(111)-(3x3) resolves three main components in the line shape, which are assigned to each of the three Sn atoms that form the unit cell. The line shape found is in agreement with an initial state picture and supports that the two down atoms are inequivalent. In full agreement with these results, scanning tunnel microscopy images directly show that the two down atoms are at slightly different heights in most of the surface, giving rise to an inequivalent-down-atoms (3x3) structure. These results solve a long-standing controversy on the interpretation of the Sn 4d core-level line shape and the structure of Sn/Ge(111)-(3x3).

Observation of a Mott insulating ground state for Sn/Ge(111) at low temperature.

We report an investigation on the properties of 0.33 ML of Sn on Ge(111) at temperatures down to 5 K. Low-energy electron diffraction and scanning tunneling microscopy show that the (3x3) phase formed at approximately 200 K, reverts to a new ((square root 3)x(square root 3))R30 degrees phase below 30 K. The vertical distortion characteristic of the (3x3) phase is lost across the phase transition, which is fully reversible. Angle-resolved photoemission experiments show that, concomitantly with the structural phase transition, a metal-insulator phase transition takes place. The ((square root 3)x(square root 3))R30 degrees ground state is interpreted as the formation of a Mott insulator for a narrow half-filled band in a two-dimensional triangular lattice.