Charge self-consistent many-body corrections using optimized projected localized orbitals.

In order for methods combining ab initio density-functional theory and many-body techniques to become routinely used, a flexible, fast, and easy-to-use implementation is crucial. We present an implementation of a general charge self-consistent scheme based on projected localized orbitals in the projector augmented wave framework in the Vienna Ab Initio Simulation Package. We give a detailed description on how the projectors are optimally chosen and how the total energy is calculated. We benchmark our implementation in combination with dynamical mean-field theory: first we study the charge-transfer insulator NiO using a Hartree-Fock approach to solve the many-body Hamiltonian. We address the advantages of the optimized against non-optimized projectors and furthermore find that charge self-consistency decreases the dependence of the spectral function-especially the gap-on the double counting. Second, using continuous-time quantum Monte Carlo we study a monolayer of SrVO3, where strong orbital polarization occurs due to the reduced dimensionality. Using total-energy calculation for structure determination, we find that electronic correlations have a non-negligible influence on the position of the apical oxygens, and therefore on the thickness of the single SrVO3 layer.

Coulomb correlations in 4d and 5d oxides from first principles-or how spin-orbit materials choose their effective orbital degeneracies.

The interplay of spin-orbit coupling and Coulomb correlations has become a hot topic in condensed matter theory and is especially important in 4d and 5d transition metal oxides, like iridates or rhodates. Here, we review recent advances in dynamical mean-field theory (DMFT)-based electronic structure calculations for treating such compounds, introducing all necessary implementation details. We also discuss the evaluation of Hubbard interactions in spin-orbit materials. As an example, we perform DMFT calculations on insulating strontium iridate (Sr2IrO4) and its 4d metallic counterpart, strontium rhodate (Sr2RhO4). While a Mott-insulating state is obtained for Sr2IrO4 in its paramagnetic phase, the spectral properties and Fermi surfaces obtained for Sr2RhO4 show excellent agreement with available experimental data. Finally, we discuss the electronic structure of these two compounds by introducing the notion of effective spin-orbital degeneracy as the key quantity that determines the correlation strength. We stress that effective spin-orbital degeneracy introduces an additional axis into the conventional picture of a phase diagram based on filling and on the ratio of interactions to bandwidth, analogous to the degeneracy-controlled Mott transition in d1 perovskites.

Importance of correlation effects in hcp iron revealed by a pressure-induced electronic topological transition.

We discover that hcp phases of Fe and Fe(0.9)Ni(0.1) undergo an electronic topological transition at pressures of about 40 GPa. This topological change of the Fermi surface manifests itself through anomalous behavior of the Debye sound velocity, c/a lattice parameter ratio, and Mössbauer center shift observed in our experiments. First-principles simulations within the dynamic mean field approach demonstrate that the transition is induced by many-electron effects. It is absent in one-electron calculations and represents a clear signature of correlation effects in hcp Fe.

Significant reduction of electronic correlations upon isovalent Ru substitution of BaFe2As2.

We investigate Ba(Fe0.65Ru0.35)2As2, a compound in which superconductivity appears at the expense of magnetism, by transport measurements and angle resolved photoemission spectroscopy. By resolving the different Fermi surface pockets and deducing from their volumes the number of hole and electron carriers, we show that Ru induces neither hole nor electron doping. However, the Fermi surface pockets are about twice larger than in BaFe2As2. A change of sign of the Hall coefficient with decreasing temperature evidences the contribution of both carriers to the transport. Fermi velocities increase significantly with respect to BaFe2As2, suggesting a reduction of correlation effects.

Superconducting gap in the hubbard model and the two-gap energy scales of high-T{c} cuprate superconductors.

Recent experiments (angle-resolved photoemission spectroscopy and Raman) suggest the presence of two distinct energy gaps in high-temperature superconductors (HTSC), exhibiting different doping dependences. The results of a variational cluster approach to the superconducting state of the two-dimensional Hubbard model are presented which show that this model qualitatively describes this gap dichotomy. The antinodal gap increases with less doping, a behavior long considered as reflecting the general gap behavior of the HTSC. On the other hand, the near-nodal gap does even slightly decrease with underdoping. An explanation of this unexpected behavior is given which emphasizes the crucial role of spin fluctuations in the pairing mechanism.

Variational cluster approach to correlated electron systems in low dimensions.

A self-energy-functional approach is applied to construct cluster approximations for correlated lattice models. It turns out that the cluster-perturbation theory [Phys. Rev. Lett. 84, 522 (2000)]] and the cellular dynamical mean-field theory [Phys. Rev. Lett. 87, 186401 (2001)]] are limiting cases of a more general cluster method. The results for the one-dimensional Hubbard model are discussed with regard to boundary conditions, bath degrees of freedom, and cluster size.