Initio Dynamical Mean-field Theory Research Articles

Efficient Formulation of Ab Initio Quantum Embedding in Periodic Systems: Dynamical Mean-Field Theory.

We present an efficient ab initio dynamical mean-field theory (DMFT) implementation for quantitative simulations in solids. Our DMFT scheme employs ab initio Hamiltonians defined for impurities comprising the full unit cell or a supercell of atoms and for realistic quantum chemical basis sets. We avoid double counting errors by using Hartree-Fock as the low-level theory. Intrinsic and projected atomic orbitals (IAO + PAO) are chosen as the local embedding basis, facilitating numerical bath truncation. Using an efficient integral transformation and coupled-cluster Green's function impurity solvers, we are able to handle embedded impurity problems with several hundred orbitals. We apply our ab initio DMFT approach to study a hexagonal boron nitride monolayer, crystalline silicon, and nickel oxide in the antiferromagnetic phase, with up to 104 and 78 impurity orbitals in the spin-restricted and unrestricted cluster DMFT calculations and over 100 bath orbitals. We show that our scheme produces accurate spectral functions compared to both benchmark periodic coupled-cluster computations and experimental spectra.

Linear behavior of the optical conductivity and incoherent charge transport in BaCoS2

Optical conductivity measurements on a BaCoS2 single crystal show an unusual linear behavior over a broad spectral range. In the paramagnetic phase above 300 K, the spectrum shows no gap, which contradicts the previously proposed scenario of a charge-transfer Mott insulator. Ab initio dynamical mean field theory calculations including a retarded Hubbard interaction explain the data in terms of an incipient opening of a Co(3d)-S(3p) charge-transfer gap concomitant to incoherent charge transport driven by electronic correlations. These results point to a non-Fermi liquid scenario with Hund's metal properties in the paramagnetic state, which arises from an incipient Mott phase destabilized by low-energy charge fluctuations across the vanishing 3d-3p charge-transfer gap.

Large effects of subtle electronic correlations on the energetics of vacancies inα-Fe

We study the effect of electronic Coulomb correlations on the vacancy formation energy in paramagnetic alpha-Fe within ab initio dynamical mean-field theory. The calculated value for the formation energy is substantially lower than in standard density-functional calculations and in excellent agreement with experiment. The reduction is caused by an enhancement of electronic correlations at the nearest neighbors of the vacancy. This effect is explained by subtle changes in the corresponding spectral function of the d-electrons. The local lattice relaxations around the vacancy are substantially increased by many-body effects.

Impact of electronic correlations on the equation of state and transport inε-Fe

We have obtained the equilibrium volumes, bulk moduli, equations of state of the ferromagnetic cubic $\alpha$ and paramagnetic hexagonal $\epsilon$ phases of iron in close agreement with experiment using an ab initio dynamical mean-field theory approach. The local dynamical correlations are shown to be crucial for a successful description of the ground-state properties of paramagnetic $\epsilon$-Fe. Moreover, they enhance the effective mass of the quasiparticles and reduce their lifetimes across the $\alpha \to \epsilon$ transition leading to a step-wise increase of the resistivity, as observed in experiment. The calculated magnitude of the jump is significantly underestimated, which points to non-local correlations. The implications of our results for the superconductivity and non-Fermi-liquid behavior of $\epsilon$-Fe are discussed.

Exploring strongly correlated quantum many‐body systems with ultracold atoms in optical lattices

AbstractUltracold quantum gases in optical lattices can be used as novel model system for the exploration of strongly correlated many‐body phases of bosonic or fermionic particles. Here we report on the realization of metallic, Mott‐insulating and band insulating phases in ultracold spin mixtures of fermionic 40K atoms. The experimental results are compared to ab initio dynamical mean field theory (DMFT) calculations.

Metallic and Insulating Phases of Repulsively Interacting Fermions in a 3D Optical Lattice

The fermionic Hubbard model plays a fundamental role in the description of strongly correlated materials. We have realized this Hamiltonian in a repulsively interacting spin mixture of ultracold (40)K atoms in a three-dimensional (3D) optical lattice. Using in situ imaging and independent control of external confinement and lattice depth, we were able to directly measure the compressibility of the quantum gas in the trap. Together with a comparison to ab initio dynamical mean field theory calculations, we show how the system evolves for increasing confinement from a compressible dilute metal over a strongly interacting Fermi liquid into a band-insulating state. For strong interactions, we find evidence for an emergent incompressible Mott insulating phase. This demonstrates the potential to model interacting condensed-matter systems using ultracold fermionic atoms.