Quasiparticle Band Structure and Density Functional Theory: Single-Particle Excitations and Band Gaps in Lattice Models

We compare the quasiparticle band structure for a model insulator obtained from the fluctuation exchange approximation (FEA) with the eigenvalues of the corresponding density functional theory (DFT) and local density approximation (LDA). The discontinuity in the exchange-correlation potential for this model is small and the FEA and DFT band structures are in good agreement. In contrast to conventional wisdom, the LDA for this model overestimates the size of the band gap. We argue that this is a consequence of an FEA self-energy that is strongly frequency dependent, but essentially local.Comment: 8 pages, and 5 figure

Coherent spin control by electromagnetic vacuum fluctuations

In coherent control, electromagnetic vacuum fluctuations usually cause coherence loss through irreversible spontaneous emission. However, since the dissipation via emission is essentially due to correlation of the fluctuations, when emission ends in a superposition of multiple final states, correlation between different pathways may build up if the "which-way" information is not fully resolved (i.e., the emission spectrum is broader than the transition energy range). Such correlation can be exploited for spin-flip control in a $\Lambda$-type three-level system, which manifests itself as an all-optical spin echo in nonlinear optics with two orders of optical fields saved as compared with stimulated Raman processes. This finding represents a new class of optical nonlinearity induced by electromagnetic vacuum fluctuations.Comment: 7 pages including 5 figure

CaB_6: a new semiconducting material for spin electronics

Ferromagnetism was recently observed at unexpectedly high temperatures in La-doped CaB_6. The starting point of all theoretical proposals to explain this observation is a semimetallic electronic structure calculated for CaB_6 within the local density approximation. Here we report the results of parameter-free quasiparticle calculations of the single-particle excitation spectrum which show that CaB_6 is not a semimetal but a semiconductor with a band gap of 0.8 eV. Magnetism in La_xCa_{1-x}B_6 occurs just on the metallic side of a Mott transition in the La-induced impurity band.Comment: 4 pages, 1 postscript figur

Optimized Effective Potential for Extended Hubbard Model

Antiferromagnetic and charge ordered Hartree-Fock solutions of the one-band Hubbard model with on-site and nearest-neighbor Coulomb repulsions are exactly mapped onto an auxiliary local Kohn-Sham (KS) problem within a density-functional theory. The mapping provides a new insight into the interpretation of the KS equations. (i) With an appropriate choice of the basic variable, there is a universal form of the KS potential, which is applicable both for the antiferromagnetic and the charge ordered solutions. (ii) The Kohn-Sham and Hartree-Fock eigenvalues are interconnected by a scaling transformation. (iii) The band-gap problem is attributed to the derivative discontinuity of the basic variable as the function of the electron number, rather than a finite discontinuity of the KS potential. (iv) It is argued that the conductivity gap and the energies of spin-wave excitations can be entirely defined by the parameters of the ground state and the KS eigenvalues.Comment: 21 page, 3 figure

Theoretical Study of Cubic Structures Based on Fullerene Carbon Clusters: C28_{28}C and (C28)2_{28})_{2}

We study a new hypothetical form of solid carbon \csc, with a unit cell which is composed of the \cs \ fullerene cluster and an additional single carbon atom arranged in the zincblende structure. Using {\it ab initio} calculations, we show that this new form of solid carbon has lower energy than hyperdiamond, the recently proposed form composed of \cs \ units in the diamond structure. To understand the bonding character of of these cluster-based solids, we analyze the electronic structure of \csc \ and of hyperdiamond and compare them to the electronic states of crystalline cubic diamond.Comment: 15 pages, latex, no figure

Density-Polarization Functional Theory of the response of a periodic insulating solid to an electric field.

The response of an infinite, periodic, insulating, solid to an infinitesimally small electric field is investigated in the framework of Density Functional Theory. We find that the applied perturbing potential is not a unique functional of the periodic density change~: it depends also on the change in the macroscopic {\em polarization}. Moreover, the dependence of the exchange-correlation energy on polarization induces an exchange-correlation electric field. These effects are exhibited for a model semiconductor. We also show that the scissor-operator technique is an approximate way of bypassing this polarization dependence.Comment: 11 pages, 1 Fig

Signatures of the excitonic memory effects in four-wave mixing processes in cavity polaritons

We report the signatures of the exciton correlation effects with finite memory time in frequency domain degenerate four-wave mixing (DFWM) in semiconductor microcavity. By utilizing the polarization selection rules, we discriminate instantaneous, mean field interactions between excitons with the same spins, long-living correlation due to the formation of biexciton state by excitons with opposite spins, and short-memory correlation effects in the continuum of unbound two-exciton states. The DFWM spectra give us the relative contributions of these effects and the upper limit for the time of the exciton-exciton correlation in the unbound two-exciton continuum. The obtained results reveal the basis of the cavity polariton scattering model for the DFWM processes in high-Q GaAs microcavity.Comment: 11 pages, 1 figur

Molecular spintronics: Coherent spin transfer in coupled quantum dots

Time-resolved Faraday rotation has recently demonstrated coherent transfer of electron spin between quantum dots coupled by conjugated molecules. Using a transfer Hamiltonian ansatz for the coupled quantum dots, we calculate the Faraday rotation signal as a function of the probe frequency in a pump-probe setup using neutral quantum dots. Additionally, we study the signal of one spin-polarized excess electron in the coupled dots. We show that, in both cases, the Faraday rotation angle is determined by the spin transfer probabilities and the Heisenberg spin exchange energy. By comparison of our results with experimental data, we find that the transfer matrix element for electrons in the conduction band is of order 0.08 eV and the spin transfer probabilities are of order 10%.Comment: 13 pages, 6 figures; minor change

Electron Spin Decoherence in Bulk and Quantum Well Zincblende Semiconductors

A theory for longitudinal (T1) and transverse (T2) electron spin coherence times in zincblende semiconductor quantum wells is developed based on a non-perturbative nanostructure model solved in a fourteen-band restricted basis set. Distinctly different dependences of coherence times on mobility, quantization energy, and temperature are found from previous calculations. Quantitative agreement between our calculations and measurements is found for GaAs/AlGaAs, InGaAs/InP, and GaSb/AlSb quantum wells.Comment: 11 pages, 3 figure

Density-functional Study of Small Molecules within the Krieger-Li-Iafrate Approximation

We report density-functional studies of several small molecules ($H_{2}, N_{2}, CO, H_{2}O$, and $CH_{4}$) within the Krieger-Li-Iafrate (KLI) approximation to the exact Kohn-Sham local exchange potential, using a three-dimensional real-space finite-difference pseudopotential method. It is found that exchange-only KLI leads to markedly improved eigenvalue spectra compared to those obtained within the standard local-density approximation (LDA), the generalized gradient approximation (GGA), and the Hartree-Fock (HF) method. For structural properties, exchange-only KLI results are close to the corresponding HF values. We find that the addition of LDA or GGA correlation energy functionals to the KLI exact exchange energy functional does not lead to systematic improvements.Comment: 16 pages including 1 fugure, to be published in Phys. Rev. A Nov. 1 '9