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An electride is a compound that contains a localized electron in an empty crystallographic site. This class of materials has a wide range of applications, including superconductivity, batteries, photonics, and catalysis. Both polymorphs of Yb5Sb3 (the orthorhombic Ca5Sb3F structure type (β phase) and hexagonal Mn5Si3 structure type (α phase)) are known to be electrides with electrons localized in 0D tetrahedral cavities and 1D octahedral chains, respectively. In the case of the orthorhombic β phase, an interstitial H can occupy the 0D tetrahedral cavity, accepting the anionic electron that would otherwise occupy the site, providing the formula of Yb5Sb3Hx. DFT computations show that the hexagonal structure is energetically favored without hydrogen and that the orthorhombic structure is more stable with hydrogen. Polycrystalline samples of orthorhombic β phase Yb5Sb3Hx (x = 0.25, 0.50, 0.75, 1.0) were synthesized, and both PXRD lattice parameters and 1H MAS NMR were used to characterize H composition. Magnetic and electronic transport properties were measured to characterize the transition from the electride (semimetal) to the semiconductor. Magnetic susceptibility measurements indicate a magnetic moment that can be interpreted as resulting from either the localized antiferromagnetically coupled electride or the presence of a small amount of Yb3+. At lower H content (x = 0.25, 0.50), a low charge carrier mobility consistent with localized electride states is observed. In contrast, at higher H content (x = 0.75, 1.0), a high charge carrier mobility is consistent with free electrons in a semiconductor. All compositions show low thermal conductivity, suggesting a potentially promising thermoelectric material if charge carrier concentration can be fine-tuned. This work provides an understanding of the structure and electronic properties of the electride and semiconductor, Yb5Sb3Hx, and opens the door to the interstitial design of electrides to tune thermoelectric properties.

1D organic metal halide hybrids (OMHHs) exhibit strongly anisotropic optical properties, highly efficient light emission, and large Stokes shift, holding promise for novel photodetection and lighting applications. However, the fundamental mechanisms governing their unique optical properties and in particular the impacts of surface effects are not understood. Herein, 1D C4N2H14PbBr4 by polarization-dependent time-averaged and time-resolved photoluminescence (TRPL) spectroscopy, as a function of photoexcitation energy, is investigated. Surprisingly, it is found that the emission under photoexcitation polarized parallel to the 1D metal halide chains can be either stronger or weaker than that under perpendicular polarization, depending on the excitation energy. The excitation-energy-dependent anisotropic emission is attributed to fast surface recombination, supported by first-principles calculations of optical absorption in this material. The fast surface recombination is directly confirmed by TRPL measurements, when the excitation is polarized parallel to the chains. The comprehensive studies provide a more complete picture for a deeper understanding of the optical anisotropy in 1D OMHHs.

Chemical modifications such as intercalation can be used to modify surface properties or to further functionalize the surface states of topological insulators (TIs). Using ambient pressure x-ray photoelectron spectroscopy, we report copper migration in C u x B i 2 S e 3 , which occurs on a timescale of hours to days after initial surface cleaving. The increase in near-surface copper proceeds along with the oxidation of the sample surface and large changes in the selenium content. These complex changes are further modeled with core-level spectroscopy simulations, which suggest a composition gradient near the surface which develops with oxygen exposure. Our results shed light on a new phenomenon that must be considered for intercalated TIs—and intercalated materials in general—that surface chemical composition can change when specimens are exposed to ambient conditions.

Co3Sn2S2 is a magnetic Weyl semimetal, in which ferromagnetic ordering at 177K is predicted to stabilize Weyl points. We perform temperature and spatial dependent angle--resolved photoemission spectroscopy measurements through the Curie temperature (Tc), which show large band shifts and renormalization concomitant with the onset of magnetism. We argue that Co3Sn2S2 evolves from a Mott ferromagnet below Tc to a correlated metallic state above Tc. To understand the magnetism, we derive a tight-binding model of Co-3dx2−y2 orbitals on the kagome lattice. At the filling obtained by first-principles calculations, this model reproduces the ferromagnetic ground state, and results in the reduction of Coulomb interactions due to cluster effects. Using a disordered local moment simulation, we show how this reduced Hubbard-U leads to a collapse of the bands across the magnetic transition, resulting in a correlated state which carries associated characteristic photoemission signatures that are distinct from those of a simple lifting of exchange splitting. The behavior of topology across Tc is discussed in the context of this description of the magnetism.

Solid-state ionic approaches for modifying ion distributions in getter/oxide heterostructures offer exciting potentials to control material properties. Here, we report a simple, scalable approach allowing for manipulation of the superconducting transition in optimally doped YBa2Cu3O7-δ (YBCO) films via a chemically driven ionic migration mechanism. Using a thin Gd capping layer of up to 20 nm deposited onto 100 nm thick epitaxial YBCO films, oxygen is found to leach from deep within the YBCO. Progressive reduction of the superconducting transition is observed, with complete suppression possible for a sufficiently thick Gd layer. These effects arise from the combined impact of redox-driven electron doping and modification of the YBCO microstructure due to oxygen migration and depletion. This work demonstrates an effective step toward total ionic tuning of superconductivity in oxides, an interface-induced effect that goes well into the quasi-bulk regime, opening-up possibilities for electric field manipulation.

The pressure dependence of the structural, magnetic, and superconducting transitions and of the superconducting upper critical field were studied in sulfur-substituted Fe(Se1-xSx). Resistance measurements were performed on single crystals with three substitution levels (x=0.043, 0.096, 0.12) under hydrostatic pressures up to 1.8 GPa and in magnetic fields up to 9 T and were compared to data on pure FeSe. Our results illustrate the effects of chemical and physical pressure on Fe(Se1-xSx). On increasing sulfur content, magnetic order in the low-pressure range is strongly suppressed to a small domelike region in the phase diagrams. However, Ts is much less suppressed by sulfur substitution, and Tc of Fe(Se1-xSx) exhibits similar nonmonotonic pressure dependence with a local maximum and a local minimum present in the low-pressure range for all x. The local maximum in Tc coincides with the emergence of the magnetic order above Tc. At this pressure the slope of the upper critical field decreases abruptly, which may indicate a Fermi-surface reconstruction. The minimum of Tc correlates with a broad maximum of the upper critical field slope normalized by Tc.

Systematic measurements of temperature-dependent magnetization, resistivity, and angle-resolved photoemission spectroscopy (ARPES) at ambient pressure as well as resistivity under pressures up to 5.25 GPa were conducted on single crystals of CrAuTe4. Magnetization data suggest that magnetic moments are aligned antiferromagnetically along the crystallographic c axis below TN=255 K. ARPES measurements show band reconstruction due to the magnetic ordering. Magnetoresistance data show clear anisotropy, and, at high fields, quantum oscillations. The Néel temperature decreases monotonically under pressure, decreasing to TN=236 K at 5.22 GPa. The pressure dependencies of (i) TN, (ii) the residual resistivity ratio, and (iii) the size and power-law behavior of the low-temperature magnetoresistance all show anomalies near 2 GPa suggesting that there may be a phase transition (structural, magnetic, and/or electronic) induced by pressure. For pressures higher than 2 GPa a significantly different quantum oscillation frequency emerges, consistent with a pressure induced change in the electronic states.

We consider the phase diagram of a ferromagnetic system driven to a quantum phase transition with a tuning parameter p. Before being suppressed, the transition becomes of the first order at a tricritical point, from which wings emerge under application of the magnetic field H in the T-p-H phase diagram. We show that the edge of the wings merge with tangent slopes at the tricritical point.

Thorough resistivity measurements on single crystals of CeZn11 under pressure p and magnetic field H are presented. At ambient pressure, CeZn11 orders antiferromagnetically at TN=2 K. The pressure dependence of the resistivity reveals an increase of the Kondo effect. We determine the pressure evolution of the magnetic exchange interaction between conduction and localized 4f electrons. It qualitatively reproduces the pressure evolution of the magnetic ordering temperature TO1 (with T O1=TN at ambient pressure). In addition to TO1, a new anomaly TO2 appears under pressure. Both anomalies are found to increase with applied pressure up to 4.9 GPa, indicating that CeZn 11 is far from a pressure induced quantum critical point. Complex T-H phase diagrams are obtained under pressure which reveal the instability of the ground state in this compound. © 2013 American Physical Society.