Lifetime of d-holes at Cu surfaces: Theory and experiment

We have investigated the hole dynamics at copper surfaces by high-resolution angle-resolved photoemission experiments and many-body quasiparticle GW calculations. Large deviations from a free-electron-like picture are observed both in the magnitude and the energy dependence of the lifetimes, with a clear indication that holes exhibit longer lifetimes than electrons with the same excitation energy. Our calculations show that the small overlap of d- and sp-states below the Fermi level is responsible for the observed enhancement. Although there is qualitative good agreement of our theoretical predictions and the measured lifetimes, there still exist some discrepancies pointing to the need of a better description of the actual band structure of the solid.Comment: 15 pages, 7 figures, 1 table, to appear in Phys. Rev.

Hole dynamics in noble metals

We present a detailed analysis of hole dynamics in noble metals (Cu and Au), by means of first-principles many-body calculations. While holes in a free-electron gas are known to live shorter than electrons with the same excitation energy, our results indicate that d-holes in noble metals exhibit longer inelastic lifetimes than excited sp-electrons, in agreement with experiment. The density of states available for d-hole decay is larger than that for the decay of excited electrons; however, the small overlap between d- and sp-states below the Fermi level increases the d-hole lifetime. The impact of d-hole dynamics on electron-hole correlation effects, which are of relevance in the analysis of time-resolved two-photon photoemission experiments, is also addressed.Comment: 4 pages, 2 figures, to appear in Phys. Rev. Let

Symmetry-Breaking Phase Transition without Peierls Mechanism in Conducting Monoatomic Chains

The one-dimensional (1D) model system Au/Ge(001), consisting of linear chains of single atoms on a surface, is scrutinized for lattice instabilities predicted in the Peierls paradigm. By scanning tunneling microscopy and electron diffraction we reveal a second-order phase transition at 585 K. It leads to charge ordering with transversal and vertical displacements and complex interchain correlations. However, the structural phase transition is not accompanied by the electronic signatures of a charge density wave, thus precluding a Peierls instability as origin. Instead, this symmetry-breaking transition exhibits three-dimensional critical behavior. This reflects a dichotomy between the decoupled 1D electron system and the structural elements that interact via the substrate. Such substrate-mediated coupling between the wires thus appears to have been underestimated also in related chain systems.Comment: 5 pages, 4 figures, accepted at Physical Review Letters 09/201

Dynamics of Excited Electrons in Copper: Role of Auger Electrons

Within a theoretical model based on the Boltzmann equation, we analyze in detail the structure of the unusual peak recently observed in the relaxation time in Cu. In particular, we discuss the role of Auger electrons in the electron dynamics and its dependence on the d-hole lifetime, the optical transition matrix elements and the laser pulse duration. We find that the Auger contribution to the distribution is very sensitive to both the d-hole lifetime tau_h and the laser pulse duration tau_l and can be expressed as a monotonic function of tau_l/tau_h. We have found that for a given tau_h, the Auger contribution is significantly smaller for a short pulse duration than for a longer one. We show that the relaxation time at the peak depends linearly on the d-hole lifetime, but interestingly not on the amount of Auger electrons generated. We provide a simple expression for the relaxation time of excited electrons which shows that its shape can be understood by a phase space argument and its amplitude is governed by the d-hole lifetime. We also find that the height of the peak depends on both the ratio of the optical transition matrix elements R=|M_{d \to sp}|^2/|M_{sp \to sp}|^2 and the laser pulse duration. Assuming a reasonable value for the ratio, namely R = 2, and a d-hole lifetime of tau_h=35 fs, we obtain for the calculated height of the peak Delta tau_{th}=14 fs, in fair agreement with Delta tau_{exp} \approx 17 fs measured for polycrystalline Cu.Comment: 6 pages, 6 figure

Atomic-scale images of charge ordering in a mixed-valence manganite

Transition-metal perovskite oxides exhibit a wide range of extraordinary but imperfectly understood phenomena. Charge, spin, orbital, and lattice degrees of freedom all undergo order-disorder transitions in regimes not far from where the best-known of these phenomena, namely high-temperature superconductivity of the copper oxides, and the 'colossal' magnetoresistance of the manganese oxides, occur. Mostly diffraction techniques, sensitive either to the spin or the ionic core, have been used to measure the order. Unfortunately, because they are only weakly sensitive to valence electrons and yield superposition of signals from distinct mesoscopic phases, they cannot directly image mesoscopic phase coexistence and charge ordering, two key features of the manganites. Here we describe the first experiment to image charge ordering and phase separation in real space with atomic-scale resolution in a transition metal oxide. Our scanning tunneling microscopy (STM) data show that charge order is correlated with structural order, as well as with whether the material is locally metallic or insulating, thus giving an atomic-scale basis for descriptions of the manganites as mixtures of electronically and structurally distinct phases.Comment: 8 pages, 4 figures, 19 reference

Magnetic Phase Diagram of Ca2-xSrxRuO4 Governed by Structural Distortions

We constructed, by the first-principles calculations, a magnetic phase diagram of Sr$_{2}$RuO$_4$ in the space spanned by structural distortions. Our phase diagram can qualitatively explain the experimental one for Ca$_{2-x}$Sr$_x$RuO$_4$. We found that the rotation and the tilting of RuO$_6$ octahedron are responsible for the ferro- and antiferro-magnetism, respectively, while the flattening of RuO$_6$ is the key factor to stabilize those magnetic ground states. Our results imply that the magnetic and the structural instabilities in Sr$_2$RuO$_4$ are closely correlated cooperatively rather than competitively.Comment: 3 figures; accepted by PRB as rapid communicatio

Surfaces: a playground for physics with broken symmetry in reduced dimensionality

Abstract With our crystal ball in front of us, we attempt to articulate the opportunities and challenges for a surface physicist in the beginning of the new millennium. The challenge is quite clear: to use the unique environment of a surface or interface to do fascinating physics, while taking full advantage of the skills the community has developed over the last 30 years. The opportunities appear to be endless! In this age of Nanotechnology where the promise is to shape the world atom by atom, leading to the next industrial revolution [Nanotechnology: shaping the world atom by atom, National Science and Technology Council, Committee on Technology, 1999], surface science should be at the very forefront of both technological and scientific advances. The smaller objects become, the more important their surfaces become. In this article we focus on the role of a surface physicist in the emergence of nanoscale collective phenomena in complex materials.

Image resonance in the many-body density of states at a metal surface

The electronic properties of a semi-infinite metal surface without a bulk gap are studied by a formalism that is able to account for the continuous spectrum of the system. The density of states at the surface is calculated within the GW approximation of many-body perturbation theory. We demonstrate the presence of an unoccupied surface resonance peaked at the position of the first image state. The resonance encompasses the whole Rydberg series of image states and cannot be resolved into individual peaks. Its origin is the shift in spectral weight when many-body correlation effects are taken into account

Photoemission and x-ray absorption study of MgC_(1-x)Ni_3

We investigated electronic structure of MgC_(1-x)Ni_3 with photoemission and x-ray absorption spectroscopy. Both results show that overall band structure is in reasonable agreement with band structure calculations including the existence of von Hove singularity (vHs)near E_F. However, we find that the sharp vHs peak theoretically predicted near the E_F is substantially suppressed. As for the Ni core level and absorption spectrum, there exist the satellites of Ni 2p which have a little larger energy separation and reduced intensity compared to the case of Ni-metal. These facts indicate that correlation effects among Ni 3d electrons may be important to understand various physical properties.Comment: 12 pages, 4 figure