Spectroscopic evidence for temperature-dependent convergence of light and heavy hole valence bands of PbQ (Q=Te, Se, S)

We have conducted temperature dependent Angle Resolved Photoemission Spectroscopy (ARPES) study of the electronic structures of PbTe, PbSe and PbS. Our ARPES data provide direct evidence for the \emph{light} hole upper valence bands (UVBs) and hitherto undetected \emph{heavy} hole lower valence bands (LVBs) in these materials. An unusual temperature dependent relative movement between these bands leads to a monotonic decrease in the energy separation between their maxima with increasing temperature, which is referred as band convergence and has long been believed to be the driving factor behind extraordinary thermoelectric performances of these compounds at elevated temperatures.Comment: 6 pages, 4 figures. arXiv admin note: text overlap with arXiv:1404.180

Orbital selectivity causing anisotropy and particle-hole asymmetry in the charge density wave gap of 2H2H-TaS2_2

We report an in-depth Angle Resolved Photoemission Spectroscopy (ARPES) study on $2H$-TaS$_2$, a canonical incommensurate Charge Density Wave (CDW) system. This study demonstrates that just as in related incommensurate CDW systems, $2H$-TaSe$_2$ and $2H$-NbSe$_2$, the energy gap ($\Delta_{\text{cdw}}\,$) of $2H$-TaS$_2$ is localized along the K-centered Fermi surface barrels and is particle-hole asymmetric. The persistence of $\Delta_{\text{cdw}}\,$ even at temperatures higher than the CDW transition temperature $\it{T}_{\text{cdw}}\,$ in $2H$-TaS$_2$, reflects the similar pseudogap (PG) behavior observed previously in $2H$-TaSe$_2$ and $2H$-NbSe$_2$. However, in sharp contrast to $2H$-NbSe$_2$, where $\Delta_{\text{cdw}}\,$ is non-zero only in the vicinity of a few "hot spots" on the inner K-centered Fermi surface barrels, $\Delta_{\text{cdw}}\,$ in $2H$-TaS$_2$ is non-zero along the entirety of both K-centered Fermi surface barrels. Based on a tight-binding model, we attribute this dichotomy in the momentum dependence and the Fermi surface specificity of $\Delta_{\text{cdw}}\,$ between otherwise similar CDW compounds to the different orbital orientations of their electronic states that are involved in CDW pairing. Our results suggest that the orbital selectivity plays a critical role in the description of incommensurate CDW materials.Comment: 6 pages, 4 figure

Cova de Can Sadurní, la transformació d’un jaciment. L’episodi sepulcral del neolític postcardial

The present study deals with the structural characterization and classification of the novel compounds <b>1</b>–<b>8</b> into perovskite subclasses and proceeds in extracting the structure–band gap relationships between them. The compounds were obtained from the employment of small, 3–5-atom-wide organic ammonium ions seeking to discover new perovskite-like compounds. The compounds reported here adopt unique or rare structure types akin to the prototype structure perovskite. When trimethylammonium (TMA) was employed, we obtained TMASnI₃ (<b>1</b>), which is our reference compound for a “perovskitoid” structure of face-sharing octahedra. The compounds EASnI₃ (<b>2b</b>), GASnI₃ (<b>3a</b>), ACASnI₃ (<b>4</b>), and IMSnI₃ (<b>5</b>) obtained from the use of ethylammonium (EA), guanidinium (GA), acetamidinium (ACA), and imidazolium (IM) cations, respectively, represent the first entries of the so-called “hexagonal perovskite polytypes” in the hybrid halide perovskite library. The hexagonal perovskites define a new family of hybrid halide perovskites with a crystal structure that emerges from a blend of corner- and face-sharing octahedral connections in various proportions. The small organic cations can also stabilize a second structural type characterized by a crystal lattice with reduced dimensionality. These compounds include the two-dimensional (2D) perovskites GA₂SnI₄ (<b>3b</b>) and IPA₃Sn₂I₇ (<b>6b</b>) and the one-dimensional (1D) perovskite IPA₃SnI₅ (<b>6a</b>). The known 2D perovskite BA₂MASn₂I₇ (<b>7</b>) and the related all-inorganic 1D perovskite “RbSnF₂I” (<b>8</b>) have also been synthesized. All compounds have been identified as medium-to-wide-band-gap semiconductors in the range of <i>E</i>_g = 1.90–2.40 eV, with the band gap progressively decreasing with increased corner-sharing functionality and increased torsion angle in the octahedral connectivity

Structure inhomogeneities, shallow defects, and charge transport in the series of thermoelectric materials K2Bi8−xSbxSe13

The charge transport properties of the low-dimensional thermoelectric materials K2Bi8-xSbxSe13 (02Bi8-xSbxSe13 was analyzed on the basis of the classical semiconductor theory and discussed in the context of recent band calculations. The results suggest that the K2Bi8-xSbxSe13 materials possess coexisting domains with semimetallic and semiconducting characters whose ratio is influenced by the value of x and by local defects. The extent and relative distribution of these domains control the charge transport properties. Electron diffraction experiments performed on samples of K2Bi8-xSbxSe13 with x=1.6 show evidence for such domains by indicating regions with long range ordering of K+/Bi3+ atoms and regions with increased disorder. The semiconducting behavior is enhanced with increasing x (i.e., Sb/Bi ratio) in the composition through a decrease of the semimetallic fraction

Local atomic structure and discommensurations in the charge density wave of CeTe3

The local structure of CeTe3 in the incommensurate charge density wave (IC-CDW) state has been obtained using atomic pair distribution function (PDF) analysis of x-ray diffraction data. Local atomic distortions in the Te-nets due to the CDW are larger than observed crystallographically, resulting in distinct short and long Te-Te bonds. Observation of different distortion amplitudes in the local and average structures are explained by the discommensurated nature of the CDW since the PDF is sensitive to the local displacements within the commensurate regions whereas the crystallographic result averages over many discommensurated domains. The result is supported by STM data. This is the first quantitative local structural study within the commensurate domains in an IC-CDW system.Comment: 4 pages, 4 figure

Effect of magnetic impurities on the vortex lattice properties in NbSe2 single crystals

We report a pronounced peak effect in the magnetization of CoxNbSe2 single crystals with critical temperatures T-c ranging between 7.1 and 5.0 K, and MnxNbSe2 single crystals with critical temperatures down to 3.4 K. We correlate the peak effect in magnetization with the structure of the vortex lattice across the peak-effect region using scanning-tunneling microscopy. Magnetization measurements show that the amplitude of the peak effect in the case of CoxNbSe2 exhibits a nonmonotonic behavior as a function of the Co content, reaching a maximum for concentration of Co of about 0.4 at. % (corresponding to a T-c of 5.7 K) and after that gradually decreasing in amplitude with the increase in the Co content. The normalized value of the peak position H-p/H-c2 has weak dependence on Co concentration. In the case of MnxNbSe2 the features of the peak effect as a function of the Mn content are different and they can be understood in terms of strong pinning

Emergence of coherence in the charge-density wave state of 2H-NbSe2_2

A charge-density wave (CDW) state has a broken symmetry described by a complex order parameter with an amplitude and a phase. The conventional view, based on clean, weak-coupling systems, is that a finite amplitude and long-range phase coherence set in simultaneously at the CDW transition temperature T$_{cdw}$. Here we investigate, using photoemission, X-ray scattering and scanning tunneling microscopy, the canonical CDW compound 2H-NbSe$_2$ intercalated with Mn and Co, and show that the conventional view is untenable. We find that, either at high temperature or at large intercalation, CDW order becomes short-ranged with a well-defined amplitude that impacts the electronic dispersion, giving rise to an energy gap. The phase transition at T$_{cdw}$ marks the onset of long-range order with global phase coherence, leading to sharp electronic excitations. Our observations emphasize the importance of phase fluctuations in strongly coupled CDW systems and provide insights into the significance of phase incoherence in `pseudogap' states.Comment: main manuscript plus supplementary informatio

Direct Evidence for Dominant Bond-directional Interactions in a Honeycomb Lattice Iridate Na2IrO3

Heisenberg interactions are ubiquitous in magnetic materials and have been prevailing in modeling and designing quantum magnets. Bond-directional interactions offer a novel alternative to Heisenberg exchange and provide the building blocks of the Kitaev model, which has a quantum spin liquid (QSL) as its exact ground state. Honeycomb iridates, A2IrO3 (A=Na,Li), offer potential realizations of the Kitaev model, and their reported magnetic behaviors may be interpreted within the Kitaev framework. However, the extent of their relevance to the Kitaev model remains unclear, as evidence for bond-directional interactions remains indirect or conjectural. Here, we present direct evidence for dominant bond-directional interactions in antiferromagnetic Na2IrO3 and show that they lead to strong magnetic frustration. Diffuse magnetic x-ray scattering reveals broken spin-rotational symmetry even above Neel temperature, with the three spin components exhibiting nano-scale correlations along distinct crystallographic directions. This spin-space and real-space entanglement directly manifests the bond-directional interactions, provides the missing link to Kitaev physics in honeycomb iridates, and establishes a new design strategy toward frustrated magnetism.Comment: Nature Physics, accepted (2015