Electronic Excitations and Correlation Effects in Metals

Theoretical descriptions of the spectrum of electronic excitations in real metals have not yet reached a fully predictive, "first-principles" stage. In this paper we begin by presenting brief highlights of recent progress made in the evaluation of dynamical electronic response in metals. A comparison between calculated and measured spectra - we use the loss spectra of Al and Cs as test cases - leads us to the conclusion that, even in "weakly-correlated" metals, correlation effects beyond mean-field theory play an important role. Furthermore, the effects of the underlying band structure turn out to be significant. Calculations which incorporate the effects of both dynamical correlations and band structure from first principles are not yet available. As a first step towards such goal, we outline a numerical algorithm for the self-consistent solution of the Dyson equation for the one-particle Green's function. The self-energy is evaluated within the shielded-interaction approximation of Baym and Kadanoff. Our method, which is fully conserving, is a finite-temperature scheme which determines the Green's function and the self-energy at the Matsubara frequencies on the imaginary axis. The analytical continuation to real frequencies is performed via Pade approximants. We present results for the homogeneous electron gas which exemplify the importance of many-body self-consistency.Comment: 32 pages, 6 figures; "Fifty Years of the Correlation Problem", invited paper, to be published in Mol.Phy

The Band-Gap Problem in Semiconductors Revisited: Effects of Core States and Many-Body Self-Consistency

A novel picture of the quasiparticle (QP) gap in prototype semiconductors Si and Ge emerges from an analysis based on all-electron, self-consistent, GW calculations. The deep-core electrons are shown to play a key role via the exchange diagram --if this effect is neglected, Si becomes a semimetal. Contrary to current lore, the Ge 3d semicore states (e.g., their polarization) have no impact on the GW gap. Self-consistency improves the calculated gaps --a first clear-cut success story for the Baym-Kadanoff method in the study of real-materials spectroscopy; it also has a significant impact on the QP lifetimes. Our results embody a new paradigm for ab initio QP theory

Mechanism of enhanced optical second-harmonic generation in the conducting pyrochlore-type Pb2_{2}Ir2_{2}O7−x_{7-x} oxide compound

The structural, electronic, and optical properties of pyrochlore-type Pb$_{2}$Ir$_{2}$O$_{6}$O'$_{0.55}$, which is a metal without spatial inversion symmetry at room temperature, were investigated. Structural analysis revealed that the structural distortion relevant to the breakdown of the inversion symmetry is dominated by the Pb-O' network but is very small in the Ir-O network. At the same time, gigantic second-harmonic generation signals were observed, which can only occur if the local environment of the Ir 5$d$ electrons features broken inversion symmetry. First-principles electronic structure calculations reveal that the underlying mechanism for this phenomenon is the induction of the noncentrosymmetricity in the Ir 5$d$ bands by the strong hybridization with O' 2$p$ orbitals. Our results stimulate theoretical study of inversion-broken iridates, where exotic quantum states such as a topological insulator and Dirac semimetal are anticipated

Plasmon Lifetime in K: A Case Study of Correlated Electrons in Solids Amenable to Ab Initio Theory

On the basis of a new ab initio, all-electron response scheme, formulated within time-dependent density-functional theory, we solve the puzzle posed by the anomalous dispersion of the plasmon linewidth in K. The key damping mechanism is shown to be decay into particle-hole pairs involving empty states of d-symmetry. While the effect of many-particle correlations is small, the correlations built into the "final-state" -d-bands play an important, and novel, role ---which is related to the phase-space complexity associated with these flat bands. Our case study of plasmon lifetime in K illustrates the importance of ab initio paradigms for the study of excitations in correlated-electron systems.Comment: 12 pages, 4 figures, for html browsing see http://web.utk.edu/~weik