Kinetic frustration and the nature of the magnetic and paramagnetic states in iron pnictides and iron chalcogenides

The iron pnictide and chalcogenide compounds are a subject of intensive investigations due to their high temperature superconductivity.\cite{a-LaFeAsO} They all share the same structure, but there is significant variation in their physical properties, such as magnetic ordered moments, effective masses, superconducting gaps and T$_c$. Many theoretical techniques have been applied to individual compounds but no consistent description of the trends is available \cite{np-review}. We carry out a comparative theoretical study of a large number of iron-based compounds in both their magnetic and paramagnetic states. We show that the nature of both states is well described by our method and the trends in all the calculated physical properties such as the ordered moments, effective masses and Fermi surfaces are in good agreement with experiments across the compounds. The variation of these properties can be traced to variations in the key structural parameters, rather than changes in the screening of the Coulomb interactions. Our results provide a natural explanation of the strongly Fermi surface dependent superconducting gaps observed in experiments\cite{Ding}. We propose a specific optimization of the crystal structure to look for higher T$_c$ superconductors.Comment: 5 pages, 3 figures with a 5-page supplementary materia

Quantum fluctuations in high field magnetization of 2D square lattice J1-J2 antiferromagnets

The J1-J2 square lattice Heisenberg model with spin S=1/2 has three phases with long-range magnetic order and two unconventionally ordered phases depending on the ratio of exchange constants. It describes a number of recently found layered vanadium oxide compounds. A simple means of investigating the ground state is the study of the magnetization curve and high-field susceptibility. We discuss these quantities by using the spin-wave theory and the exact diagonalization in the whole J1-J2 plane. We compare both results and find good overall agreement in the sectors of the phase diagram with magnetic order. Close to the disordered regions the magnetization curve shows strong deviations from the classical linear behaviour caused by large quantum fluctuations and spin-wave approximation breaks down. On the FM side (J1<0) where one approaches the quantum gapless spin nematic ground state this region is surprisingly large. We find that inclusion of second order spin-wave corrections does not lead to fundamental improvement. Quantum corrections to the tilting angle of the ordered moments are also calculated. They may have both signs, contrary to the always negative first order quantum corrections to the magnetization. Finally we investigate the effect of the interlayer coupling and find that the quasi-2D picture remains valid up to |J_\perp/J1| ~ 0.3.Comment: 13 pages, 6figure

Structural phase transition in IrTe2_2: A combined study of optical spectroscopy and band structure calculations

Ir$_{1-x}$Pt$_x$Te$_2$ is an interesting system showing competing phenomenon between structural instability and superconductivity. Due to the large atomic numbers of Ir and Te, the spin-orbital coupling is expected to be strong in the system which may lead to nonconventional superconductivity. We grew single crystal samples of this system and investigated their electronic properties. In particular, we performed optical spectroscopic measurements, in combination with density function calculations, on the undoped compound IrTe$_2$ in an effort to elucidate the origin of the structural phase transition at 280 K. The measurement revealed a dramatic reconstruction of band structure and a significant reduction of conducting carriers below the phase transition. We elaborate that the transition is not driven by the density wave type instability but caused by the crystal field effect which further splits/separates the energy levels of Te (p$_x$, p$_y$) and Te p$_z$ bands.Comment: 16 pages, 5 figure

Magnetism and Charge Dynamics in Iron Pnictides

In a wide variety of materials, such as copper oxides, heavy fermions, organic salts, and the recently discovered iron pnictides, superconductivity is found in close proximity to a magnetically ordered state. The character of the proximate magnetic phase is thus believed to be crucial for understanding the differences between the various families of unconventional superconductors and the mechanism of superconductivity. Unlike the AFM order in cuprates, the nature of the magnetism and of the underlying electronic state in the iron pnictide superconductors is not well understood. Neither density functional theory nor models based on atomic physics and superexchange, account for the small size of the magnetic moment. Many low energy probes such as transport, STM and ARPES measured strong anisotropy of the electronic states akin to the nematic order in a liquid crystal, but there is no consensus on its physical origin, and a three dimensional picture of electronic states and its relations to the optical conductivity in the magnetic state is lacking. Using a first principles approach, we obtained the experimentally observed magnetic moment, optical conductivity, and the anisotropy of the electronic states. The theory connects ARPES, which measures one particle electronic states, optical spectroscopy, probing the particle hole excitations of the solid and neutron scattering which measures the magnetic moment. We predict a manifestation of the anisotropy in the optical conductivity, and we show that the magnetic phase arises from the paramagnetic phase by a large gain of the Hund's rule coupling energy and a smaller loss of kinetic energy, indicating that iron pnictides represent a new class of compounds where the nature of magnetism is intermediate between the spin density wave of almost independent particles, and the antiferromagnetic state of local moments.Comment: 4+ pages with additional one-page supplementary materia

Similarities between structural distortions under pressure and chemical doping in superconducting BaFe2As2

The discovery of a new family of high Tc materials, the iron arsenides (FeAs), has led to a resurgence of interest in superconductivity. Several important traits of these materials are now apparent, for example, layers of iron tetrahedrally coordinated by arsenic are crucial structural ingredients. It is also now well established that the parent non-superconducting phases are itinerant magnets, and that superconductivity can be induced by either chemical substitution or application of pressure, in sharp contrast to the cuprate family of materials. The structure and properties of chemically substituted samples are known to be intimately linked, however, remarkably little is known about this relationship when high pressure is used to induce superconductivity in undoped compounds. Here we show that the key structural features in BaFe2As2, namely suppression of the tetragonal to orthorhombic phase transition and reduction in the As-Fe-As bond angle and Fe-Fe distance, show the same behavior under pressure as found in chemically substituted samples. Using experimentally derived structural data, we show that the electronic structure evolves similarly in both cases. These results suggest that modification of the Fermi surface by structural distortions is more important than charge doping for inducing superconductivity in BaFe2As2

Electronic correlations in the iron pnictides

In correlated metals derived from Mott insulators, the motion of an electron is impeded by Coulomb repulsion due to other electrons. This phenomenon causes a substantial reduction in the electron's kinetic energy leading to remarkable experimental manifestations in optical spectroscopy. The high-Tc superconducting cuprates are perhaps the most studied examples of such correlated metals. The occurrence of high-Tc superconductivity in the iron pnictides puts a spotlight on the relevance of correlation effects in these materials. Here we present an infrared and optical study on single crystals of the iron pnictide superconductor LaFePO. We find clear evidence of electronic correlations in metallic LaFePO with the kinetic energy of the electrons reduced to half of that predicted by band theory of nearly free electrons. Hallmarks of strong electronic many-body effects reported here are important because the iron pnictides expose a new pathway towards a correlated electron state that does not explicitly involve the Mott transition.Comment: 10 page

Lignin biomarkers as tracers of mercury sources in lakes water column

This study presents the role of specific terrigenous organic compounds as important vectors of mercury (Hg) transported from watersheds to lakes of the Canadian boreal forest. In order to differentiate the autochthonous from the allochthonous organic matter (OM), lignin derived biomarker signatures [Lambda, S/V, C/V, P/(V ? S), 3,5-Bd/V and (Ad/Al)v] were used. Since lignin is exclusively produced by terrigenous plants, this approach can give a non equivocal picture of the watershed inputs to the lakes. Moreover, it allows a characterization of the source of OM and its state of degradation. The water column of six lakes from the Canadian Shield was sampled monthly between June and September 2005. Lake total dissolved Hg concentrations and Lambda were positively correlated, meaning that Hg and ligneous inputs are linked (dissolved OM r2 = 0.62, p\0.0001; particulate OM r2 = 0.76, p\0.0001). Ratios of P/(V ? S) and 3,5-Bd/V from both dissolved OM and particulate OM of the water column suggest an inverse relationship between the progressive state of pedogenesis and maturation of the OM in soil before entering the lake, and the Hg concentrations in the water column. No relation was found between Hg levels in the lakes and the watershed flora composition—angiosperm versus gymnosperm or woody versus non-woody compounds. This study has significant implications for watershed management of ecosystems since limiting fresh terrestrial OM inputs should reduce Hg inputs to the aquatic systems. This is particularly the case for largescale land-use impacts, such as deforestation, agriculture and urbanization, associated to large quantities of soil OM being transferred to aquatic systems