Nature of the Insulating Ground State of the Two-Dimensional Sn Atom Lattice on SiC(0001).

Semiconductor surfaces with narrow surface bands provide unique playgrounds to search for Mott-insulating state. Recently, a combined experimental and theoretical study of the two-dimensional (2D) Sn atom lattice on a wide-gap SiC(0001) substrate proposed a Mott-type insulator driven by strong on-site Coulomb repulsion U within a single-band Hubbard model. However, our systematic density-functional theory (DFT) study with local, semilocal, and hybrid exchange-correlation functionals shows that the Sn dangling-bond state largely hybridizes with the substrate Si 3p and C 2p states to split into three surface bands due to the crystal field. Such a hybridization gives rise to the stabilization of the antiferromagnetic order via superexchange interactions. The band gap and the density of states predicted by the hybrid DFT calculation agree well with photoemission data. Our findings not only suggest that the Sn/SiC(0001) system can be represented as a Slater-type insulator driven by long-range magnetism, but also have an implication that taking into account long-range interactions beyond the on-site interaction would be of importance for properly describing the insulating nature of Sn/SiC(0001).

DFT and TB study of the geometry of hydrogen adsorbed on graphynes.

Using density-functional calculations (DFT) and a tight-binding model, we investigate the origin of distinct favorable geometries which depend on the type of graphyne used. The change in the H geometry is described in terms of the tuning of the hopping between sp(2)-bonded C atoms and sp-bonded C atoms hybridized with the H atoms. We find that the different preferred geometry for each type of graphyne is associated with the electronic effects due to different symmetries rather than a steric effect minimizing the repulsive interaction between the H atoms. The band gaps are significantly tuned as the hopping varies, except in α-graphyne, in agreement with the result of our previous DFT study (Koo J et al 2013 J. Phys. Chem. C 117 11960). Our model can be used to describe the geometry and electronic properties of hydrogenated graphynes.

Theoretical prediction of a strongly correlated Dirac metal.

Recently, the most intensely studied objects in the electronic theory of solids have been strongly correlated systems and graphene. However, the fact that the Dirac bands in graphene are made up of sp(2) electrons, which are subject to neither strong Hubbard repulsion U nor strong Hund's rule coupling J, creates certain limitations in terms of novel, interaction-induced physics that could be derived from Dirac points. Here we propose GaCu3(OH)6Cl2 (Ga-substituted herbertsmithite) as a correlated Dirac-Kagome metal combining Dirac electrons, strong interactions and frustrated magnetic interactions. Using density functional theory, we calculate its crystallographic and electronic properties, and observe that it has symmetry-protected Dirac points at the Fermi level. Its many-body physics is diverse, with possible charge, magnetic and superconducting instabilities. Through a combination of various many-body methods we study possible symmetry-lowering phase transitions such as Mott-Hubbard, charge or magnetic ordering, and unconventional superconductivity, which in this compound assumes an f-wave symmetry.

Absence of metallicity in K-doped picene: importance of electronic correlations.

Potassium-doped picene (K(x)picene) has recently been reported to be a superconductor at x=3 with critical temperatures up to 18 K. Here we study the electronic structure of K-doped picene films by photoelectron spectroscopy and ab initio density functional theory combined with dynamical mean-field theory (DFT+DMFT). Experimentally we observe that, except for spurious spectral weight due to the lack of a homogeneous chemical potential at low K concentrations (x≈1), the spectra always display a finite energy gap. This result is supported by our DFT+DMFT calculations which provide clear evidence that K(x)picene is a Mott insulator for integer doping concentrations x=1, 2, and 3. We discuss various scenarios to understand the discrepancies with previous reports of superconductivity and metallic behavior.

Dynamical cluster approximation study of the anisotropic two-orbital Hubbard model.

We investigate the properties of a two-orbital Hubbard model with unequal bandwidths on the square lattice in the framework of the dynamical cluster approximation (DCA) combined with a continuous-time quantum Monte Carlo algorithm. We explore the effect of short-range spatial fluctuations on the nature of the metal-insulator transition and the possible occurrence of an orbital-selective Mott transition (OSMT) as a function of cluster size N{c}. We observe that for N{c}=2 no OSMT is present, instead a band insulator state for both orbitals is stabilized at low temperatures due to the appearance of an artificial local ordered state. For N{c}=4 the DCA calculations suggest the presence of five different phases which originate out of the cooperation and competition between spatial fluctuations and orbitals of different bandwidths and an OSMT phase is stabilized. Based on our results, we discuss the nature of the gap opening.