Violation of particle number conservation in the it GW approximation

We present a nontrivial model system of interacting electrons that can be solved analytically in the GW approximation. We obtain the particle number from the GW Green's function strictly analytically, and prove that there is a genuine violation of particle number conservation if the self-energy is calculated non-self-consistently from a zeroth order Green's function, as done in virtually all practical implementations. We also show that a simple shift of the self-energy that partially restores self-consistency reduces the numerical deviation significantly

Image states in metal clusters

The existence of image states in small clusters is shown, using a quantum-mechanical many-body approach. We present image state energies and wave functions for spherical jellium clusters up to 186 atoms, calculated in the GW approximation, where G is the Green's function and W is the dynamically screened Coulomb interaction, which by construction contains the dynamic long-range correlation effects that give rise to image effects. In addition, we find that image states are also subject to quantum confinement. To extrapolate our investigations to clusters in the mesoscopic size range, we propose a semiclassical model potential, which we test against our full GW results

Systematic vertex corrections through iterative solution of Hedin's equations beyond the it GW approximation

We present a general procedure for obtaining progressively more accurate functional expressions for the electron self-energy by iterative solution of Hedin's coupled equations. The iterative process starting from Hartree theory, which gives rise to the GW approximation, is continued further, and an explicit formula for the vertex function from the second full cycle is given. Calculated excitation energies for a Hubbard Hamiltonian demonstrate the convergence of the iterative process and provide further strong justification for the GW approximation

Quasiparticle properties of a coupled quantum wire electron-phonon system

We study leading-order many-body effects of longitudinal optical (LO) phonons on electronic properties of one-dimensional quantum wire systems. We calculate the quasiparticle properties of a weakly polar one dimensional electron gas in the presence of both electron-phonon and electron-electron interactions. The leading-order dynamical screening approximation (GW approximation) is used to obtain the electron self-energy, the quasiparticle spectral function, and the quasiparticle damping rate in our calculation by treating electrons and phonons on an equal footing. Our theory includes effects (within the random phase approximation) of Fermi statistics, Landau damping, plasmon-phonon mode coupling, phonon renormalization, dynamical screening, and impurity scattering. In general, electron-electron and electron-phonon many-body renormalization effects are found to be nonmultiplicative and nonadditive in our theoretical results for quasiparticle properties.Comment: 21 pages, Revtex, 12 figures enclose

Multiple Core-Hole Coherence in X-Ray Four-Wave-Mixing Spectroscopies

Correlation-function expressions are derived for the coherent nonlinear response of molecules to three resonant ultrafast pulses in the x-ray regime. The ability to create two-core-hole states with controlled attosecond timing in four-wave-mixing and pump probe techniques should open up new windows into the response of valence electrons, which are not available from incoherent x-ray Raman and fluorescence techniques. Closed expressions for the necessary four-point correlation functions are derived for the electron-boson model by using the second order cumulant expansion to describe the fluctuating potentials. The information obtained from multidimensional nonlinear techniques could be used to test and refine this model, and establish an anharmonic oscillator picture for electronic excitations

Optical excitations in organic molecules, clusters and defects studied by first-principles Green's function methods

Spectroscopic and optical properties of nanosystems and point defects are discussed within the framework of Green's function methods. We use an approach based on evaluating the self-energy in the so-called GW approximation and solving the Bethe-Salpeter equation in the space of single-particle transitions. Plasmon-pole models or numerical energy integration, which have been used in most of the previous GW calculations, are not used. Fourier transforms of the dielectric function are also avoided. This approach is applied to benzene, naphthalene, passivated silicon clusters (containing more than one hundred atoms), and the F center in LiCl. In the latter, excitonic effects and the $1s \to 2p$ defect line are identified in the energy-resolved dielectric function. We also compare optical spectra obtained by solving the Bethe-Salpeter equation and by using time-dependent density functional theory in the local, adiabatic approximation. From this comparison, we conclude that both methods give similar predictions for optical excitations in benzene and naphthalene, but they differ in the spectra of small silicon clusters. As cluster size increases, both methods predict very low cross section for photoabsorption in the optical and near ultra-violet ranges. For the larger clusters, the computed cross section shows a slow increase as function of photon frequency. Ionization potentials and electron affinities of molecules and clusters are also calculated.Comment: 9 figures, 5 tables, to appear in Phys. Rev. B, 200

Concentration Dependence of the Effective Mass of He-3 Atoms in He-3/He-4 Mixtures

Recent measurements by Yorozu et al. (S. Yorozu, H. Fukuyama, and H. Ishimoto, Phys. Rev. B 48, 9660 (1993)) as well as by Simons and Mueller (R. Simons and R. M. Mueller, Czhechoslowak Journal of Physics Suppl. 46, 201 (1976)) have determined the effective mass of He-3 atoms in a He-3/He-4 mixture with great accuracy. We here report theoretical calculations for the dependence of that effective mass on the He-3 concentration. Using correlated basis functions perturbation theory to infinite order to compute effective interactions in the appropriate channels, we obtain good agreement between theory and experiment.Comment: 4 pages, 1 figur

Band gap renormalization in photoexcited semiconductor quantum wire structures in the GW approximation

We investigate the dynamical self-energy corrections of the electron-hole plasma due to electron-electron and electron-phonon interactions at the band edges of a quasi-one dimensional (1D) photoexcited electron-hole plasma. The leading-order $GW$ dynamical screening approximation is used in the calculation by treating electron-electron Coulomb interaction and electron-optical phonon Fr\"{o}hlich interaction on an equal footing. We calculate the exchange-correlation induced band gap renormalization (BGR) as a function of the electron-hole plasma density and the quantum wire width. The calculated BGR shows good agreement with existing experimental results, and the BGR normalized by the effective quasi-1D excitonic Rydberg exhibits an approximate one-parameter universality.Comment: 11 pages, 3 figure