La$_2$O$_3$Fe$_2$Se$_2$ can be explained in terms of Mott localization in sharp contrast with the metallic behavior of FeSe and other parent parent compounds of iron superconductors. We demonstrate that the key ingredient that makes La$_2$O$_3$Fe$_2$Se$_2$ a Mott insulator, rather than a correlated metal dominated by the Hunds coupling is the enhanced crystal-field splitting, accompanied by a smaller orbital-resolved kinetic energy. The strong deviation from orbital degeneracy introduced by the crystal-field splitting also pushes this materials close to an orbital-selective Mott transition. We predict that either doping or uniaxial external pressure can drive the material into an orbital-selective Mott state, where only one or few orbitals are metallized while the others remain insulating.
We report the physical properties and electronic structure calculations of a layered chromium oxypnictide, Sr$_2$Cr$_3$As$_2$O$_2$, which crystallizes in a Sr$_2$Mn$_3$As$_2$O$_2$-type structure containing both CrO$_2$ planes and Cr$_2$As$_2$ layers. The newly synthesized material exhibits a metallic conduction with a dominant electron-magnon scattering. Magnetic and specific-heat measurements indicate at least two intrinsic magnetic transitions below room temperature. One is an antiferromagnetic transition at 291 K, probably associated with a spin ordering in the Cr$_2$As$_2$ layers. Another transition is broad, occurring at around 38 K, and possibly due to a short-range spin order in the CrO$_2$ planes. Our first-principles calculations indicate predominant two-dimensional antiferromagnetic exchange couplings, and suggest a KG-type (i.e. K$_2$NiF$_4$ type for CrO$_2$ planes and G type for Cr$_2$As$_2$ layers) magnetic structure, with reduced moments for both Cr sublattices. The corresponding electronic states near the Fermi energy are mostly contributed from Cr-3$d$ orbitals which weakly (modestly) hybridize with the O-2$p$ (As-4$p$) orbitals in the CrO$_2$ (Cr$_2$As$_2$) layers. The bare bandstructure density of states at the Fermi level is only $sim$1/4 of the experimental value derived from the low-temperature specific-heat data, consistent with the remarkable electron-magnon coupling. The title compound is argued to be a possible candidate to host superconductivity.
1T-TaS$_2$ undergoes successive phase transitions upon cooling and eventually enters an insulating state of mysterious origin. Some consider this state to be a band insulator with interlayer stacking order, yet others attribute it to Mott physics that support a quantum spin liquid state.Here, we determine the electronic and structural properties of 1T-TaS$_2$ using angle-resolved photoemission spectroscopy and X-Ray diffraction. At low temperatures, the 2$pi$/2c-periodic band dispersion, along with half-integer-indexed diffraction peaks along the c axis, unambiguously indicates that the ground state of 1T-TaS$_2$ is a band insulator with interlayer dimerization. Upon heating, however, the system undergoes a transition into a Mott insulating state, which only exists in a narrow temperature window. Our results refute the idea of searching for quantum magnetism in 1T-TaS$_2$ only at low temperatures, and highlight the competition between on-site Coulomb repulsion and interlayer hopping as a crucial aspect for understanding the materials electronic properties.
The electronic structure and magnetic properties of the strongly correlated material La$_2$O$_3$Fe$_2$Se$_2$ are studied by using both the density function theory plus $U$ (DFT+$U$) method and the DFT plus Gutzwiller (DFT+G) variational method. The ground-state magnetic structure of this material obtained with DFT+$U$ is consistent with recent experiments, but its band gap is significantly overestimated by DFT+$U$, even with a small Hubbard $U$ value. In contrast, the DFT+G method yields a band gap of 0.1 - 0.2 eV, in excellent agreement with experiment. Detailed analysis shows that the electronic and magnetic properties of of La$_2$O$_3$Fe$_2$Se$_2$ are strongly affected by charge and spin fluctuations which are missing in the DFT+$U$ method.
The topochemical transformation of single crystals of Sr$_3$Ir$_2$O$_7$ into Sr$_3$Ir$_2$O$_7$F$_2$ is reported via fluorine insertion. Characterization of the newly formed Sr$_3$Ir$_2$O$_7$F$_2$ phase shows a nearly complete oxidation of Ir$^{4+}$ cations into Ir$^{5+}$ that in turn drives the system from an antiferromagnetic Mott insulator with a half-filled J$_{eff}=1/2$ band into a nonmagnetic $J=0$ band insulator. First principles calculations reveal a remarkably flat insertion energy that locally drives the fluorination process to completion. Band structure calculations support the formation of a band insulator whose charge gap relies on the strong spin-orbit coupling inherent to the Ir metal ions of this compound.
We present evidence of strain-induced modulation of electron correlation effects and increased orbital anisotropy in the rutile phase of epitaxial VO$_2$/TiO$_2$ films from hard x-ray photoelectron spectroscopy and soft V L-edge x-ray absorption spectroscopy, respectively. By using the U(1) slave spin formalism, we further argue that the observed anisotropic correlation effects can be understood by a model of orbital selective Mott transition at a filling that is non-integer, but close to the half-filling. Because the overlaps of wave functions between $d$ orbitals are modified by the strain, orbitally-dependent renormalizations of the bandwidths and the crystal fields occur with the application of strain. These renormalizations generally result in different occupation numbers in different orbitals. We find that if the system has a non-integer filling number near the half-filling such as for VO$_2$, certain orbitals could reach an occupation number closer to half-filling under the strain, resulting in a strong reduction in the quasiparticle weight $Z_{alpha}$ of that orbital. Moreover, an orbital selective Mott transition, defined as the case with $Z_{alpha} = 0$ in some, but not all orbitals, could be accessed by epitaxial strain-engineering of correlated electron systems.
Gianluca Giovannetti
,Luca de Medici
,Markus Aichhorn
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(2014)
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"La$_2$O$_3$Fe$_2$Se$_2$, a Mott insulator on the brink of orbital-selective metalization"
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Gianluca Giovannetti GG
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