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SignificanceThere is an intense ongoing search for two-level quantum systems with long lifetimes for applications in quantum communication and computation. Much research has been focused on studying isolated spins in semiconductors or band insulators. Mott insulators provide an interesting alternative platform but have been far less explored. In this work we use a technique capable of resolving individual spins at atomic length scales, to measure the two-level switching of spin states in 1T-TaS2. We find quasi-1D chains of spin-1/2 electrons embedded in 1T-TaS2 which have exceptionally long lifetimes. The discovery of long-lived spin states in a tractable van der Waal material opens doors to using Mott systems in future quantum information applications.
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Reacting RE2O3 and H3BO3 in an ultra-alkaline NaOH hydroflux at about 250 °C yielded pure, crystalline samples of Na2[RE(BO3)(OH)2] (RE = Y, Gd-Er). The compounds dehydrate to Na3RE(BO3)2 upon heating in air to about 500 °C. Na2[RE(BO3)(OH)2] (RE = Tb-Er) are photoluminescent under UV radiation. Their UV-Vis spectra show the typical absorptions associated with 4f-4f transitions and absorption edges in the UV (band gaps ≥ 5.7 eV). The RE3+ cation is coordinated by seven oxygen atoms, which define a distorted pentagonal bipyramid. The bipyramids share trans-edges of their base forming infinite chains. Triangular (BO3)3- groups connect the chains into layers. The crystal structure of Na2[Ho(BO3)(OH)2] was investigated at various temperatures in the range 100 K ≤ T ≤ 320 K. Above 310(2) K, the compound crystallizes in the orthorhombic space group Cmcm (ß-phase), below, it undergoes a displacive phase transition of second order resulting in a monoclinic structure in space group C2/c (α-phase). The critical exponents derived from different structural parameters indicate a cooperative distortion of the borate layers, but a rather uncorrelated adaptation of the sodium cations to their local environment. The other compounds of the series also adopt the structure of the α-phase at 296 K.
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The manipulation of topological states in quantum matter is an essential pursuit of fundamental physics and next-generation quantum technology. Here we report the magnetic manipulation of Weyl fermions in the kagome spin-orbit semimetal Co_{3}Sn_{2}S_{2}, observed by high-resolution photoemission spectroscopy. We demonstrate the exchange collapse of spin-orbit-gapped ferromagnetic Weyl loops into paramagnetic Dirac loops under suppression of the magnetic order. We further observe that topological Fermi arcs disappear in the paramagnetic phase, suggesting the annihilation of exchange-split Weyl points. Our findings indicate that magnetic exchange collapse naturally drives Weyl fermion annihilation, opening new opportunities for engineering topology under correlated order parameters.
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The Jahn-Teller (JT) theorem constitutes one of the most fundamental concepts in chemistry. In transition-element chemistry, the 3d4 and 3d9 configurations in octahedral complexes are particularly illustrative, where a distortion in local geometry is associated with a reduction of the electronic energy. However, there has been a lasting debate about the fact that the octahedra are found to exclusively elongate. In contrast, for Na9 Bi5 Os3 O24 , the octahedron around Os6+ (5d2 ) is heavily compressed, lifting the degeneracy of the t2g set of 5d orbitals such that in the sense of a JT compression a diamagnetic ground state results. This effect is not forced by structural constraints, the structure offers sufficient space for osmium to shift the apical oxygen atoms to a standard distance. The relevance of these findings is far reaching, since they provide new insights in the hierarchy of perturbations defining ground states of open shell electronic systems.
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The seminal qualitative concepts of chemical bonding, as presented by Walter Kossel and Gilbert Newton Lewis back in 1916, have lasting general validity. These basic rules of chemical valence still serve as a touchstone for validating the plausibility of composition and constitution of a given chemical compound. We report on Ag7Pt2O7, with a composition that violates the basic rules of chemical valence and an exotic crystal structure. The first coordination sphere of platinum is characteristic of tetravalent platinum. Thus, the electron count corresponds to Ag7Pt2O7*e-, where excess electrons are associated with the silver substructure. Such conditions given, it is commonly assumed that the excess electrons are either itinerant or localized in Ag-Ag bonds. However, the material does not show metallic conductivity, nor does the structure feature Ag-Ag pairs. Instead, the excess electrons organize themselves in 2e-4c bonds within the silver substructure. This subvalent silver oxide reveals a new general facet pertinent to silver chemistry.
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Three-dimensional (3D) Dirac semimetals exist close to topological phase boundaries which, in principle, should make it possible to drive them into exotic new phases, such as topological superconductivity, by breaking certain symmetries. A practical realization of this idea has, however, hitherto been lacking. Here we show that the mesoscopic point contacts between pure silver (Ag) and the 3D Dirac semimetal Cd3As2 (ref. ) exhibit unconventional superconductivity with a critical temperature (onset) greater than 6 K whereas neither Cd3As2 nor Ag are superconductors. A gap amplitude of 6.5 meV is measured spectroscopically in this phase that varies weakly with temperature and survives up to a remarkably high temperature of 13 K, indicating the presence of a robust normal-state pseudogap. The observations indicate the emergence of a new unconventional superconducting phase that exists in a quantum mechanically confined region under a point contact between a Dirac semimetal and a normal metal.
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The fascination of mankind towards a sudden change of a property, like colour, shape, elasticity, viscosity, electrical conductivity and magnetism, is well known. If the change in property is such that it leads to disapperance of an existing property or development of a new property then the effect is magical. It is for this reason that superconductivity remains an enigma for scientists for over a century after Kammerlingh Onnes discovered that the electrical resistance of mercury falls to zero below a temperature of 4.2 K. Since then scientists have been enchanted by superconductivity. Over these hundred years attempts have been made to discover materials which show this effect at higher temperatures. After a very exciting period of Cu oxide superconductors (1986-1993) there has been a lull in the search for high T(c) materials. The discovery of superconductivity in 2008 at 26 K in LaOFeAs (F-doped) has renewed the excitement in the field of superconductivity. This breakthrough in an Fe-containing compound led to the discovery of several new families of Fe-based superconductors having either pnictogens (P, As) or chalcogen (Se, Te) of the type AFFeAs (A = alkaline-earth metal), AFe(2)As(2), AFeAs (A = alkali metals), A(3)M(2)O(5)Fe(2)As(2) (M = transition metals) and A(4)M(2)O(6)Fe(2)As(2). This review article discusses in detail the structural aspects of these new Fe-based superconductors which primarily consist of edge-shared distorted FeX(4) (X = pnictogen and chalcogen) tetrahedra and these tetrahedral layers are reponsible for enabling superconductivity. Extremely large upper critical field (>200 Tesla) of these superconductors make them promising for high field application. Structural commonalities and differences among different families of these superconductors have been outlined. We also discuss the common features and differences with the copper-oxide based superconductors. Here we have discussed all the Fe-based oxypnictide families (like LnOFePn, AFe(2)Pn(2), AFFePn and A(4)M(2)M'Fe(2)As(2)O(6)etc.) known today and have also included the phosphides and antimonides other than the arsenides. We have in addition discussed in detail the various factors like pressure, hole and electron doping, transition metal doping, which have not been reviewed earlier.
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The design of new complex mixed metal tellurides (containing low toxicity cations) with intrinsic ultralow thermal conductivity is of paramount importance in the field of thermoelectrics. Herein, we report the synthesis and characterization of polycrystalline and single crystals of a new mixed-metal quaternary telluride Mn1.8(1)In0.8(1)Si2Te6. The structural aspects and chemical formula of this phase at room temperature have been established using single crystal X-ray diffraction and EDX studies. The trigonal centrosymmetric (space group: P3Ì1m) structure of the title phase has cell constants of a = b = 7.0483(7) Å and c = 7.1277(8) Å. The structure has three independent cationic sites, one mixed (In1/Mn1), one partially filled Mn2, and one Si1, which are bonded with Te1 atoms. Each metal atom (In and Mn) in the structure is octahedrally coordinated with six neighboring Te1 atoms. The structure also features dimers of Si atoms, and each Si atom is bonded to three Te1 atoms to form ethane-like Si2Te6 units. The optical absorption study of a polycrystalline Mn1.8In0.8Si2Te6 sample shows a narrow optical bandgap of 0.6(2) eV. Temperature-dependent resistivity and Seebeck coefficient studies confirmed the p-type semiconducting nature of the sample with high values of S (301 µV K-1 to 444 µV K-1). The total thermal conductivity (ktot) study of the polycrystalline sample shows a decreasing trend on heating with an extremely low value of 0.28 W m-1 K-1 at 773 K. Magnetic measurements indicate a glassy magnetic behavior for the sample below 8 K.
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Topological Weyl semimetals have recently attracted considerable attention among materials scientists as their properties are predicted to be protected against perturbations such as lattice distortion and chemical substitution. However, any experimental proof of such robustness is still lacking. In this study, we experimentally demonstrate that the topological properties of the ferromagnetic kagomé compound Co3Sn2S2 are preserved upon Ni substitution. We systematically vary the Ni content in Co3Sn2S2 single crystals and study their magnetic and anomalous transport properties. For the intermediate Ni substitution, we observe a remarkable increase in the coercive field while still maintaining significant anomalous Hall conductivity. The large anomalous Hall conductivity of these compounds is intrinsic, consistent with first-principles calculations, which proves its topological origin. Our results can guide further studies on the chemical tuning of topological materials for better understanding.
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The crystal structure redetermination of Sr2PdO3 (distrontium palladium trioxide) was carried out using high-quality single-crystal X-ray data. The Sr2PdO3 structure has been described previously in at least three reports [Wasel-Nielen & Hoppe (1970 â¸). Z. Anorg. Allg. Chem. 375, 209-213; Muller & Roy (1971 â¸). Adv. Chem. Ser. 98, 28-38; Nagata et al. (2002 â¸). J. Alloys Compd. 346, 50-56], all based on powder X-ray diffraction data. The current structure refinement of Sr2PdO3, as compared to previous powder data refinements, leads to more precise cell parameters and fractional coordinates, together with anisotropic displacement parameters for all sites. The compound is confirmed to have the ortho-rhom-bic Sr2CuO3 structure type (space group Immm) as reported previously. The structure consists of infinite chains of corner-sharing PdO4 plaquettes inter-spersed by SrII atoms. A brief comparison of Sr2PdO3 with the related K2NiF4 structure type is given.
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We have carried out detailed magnetic and transport studies of the new Sr0.5Ce0.5FBiS2-xSex (0.0 ≤ x ≤ 1.0) superconductors derived by doping Se in Sr0.5Ce0.5FBiS2. Se-doping produces several effects: it suppresses semiconducting-like behavior observed in the undoped Sr0.5Ce0.5FBiS2, the ferromagnetic ordering temperature, TFM, decreases considerably from 7.5 K (in Sr0.5Ce0.5FBiS2) to 3.5 K and the superconducting transition temperature, Tc, gets enhanced slightly to 2.9-3.3 K. Thus in these Se-doped materials, TFM is marginally higher than Tc. Magnetization studies provide evidence of bulk superconductivity in Sr0.5Ce0.5FBiS2-xSex at x ≥ 0.5 in contrast to the undoped Sr0.5Ce0.5FBiS2 (x = 0) where magnetization measurements indicate a small superconducting volume fraction. Quite remarkably, as compared with the effective paramagnetic Ce-moment (~2.2 µB), the ferromagnetically ordered Ce-moment in the superconducting state is rather small (~0.1 µB) suggesting itinerant ferromagnetism. To the best of our knowledge, Sr0.5Ce0.5FBiS2-x Sex (x = 0.5 and 1.0) are distinctive Ce-based bulk superconducting itinerant ferromagnetic materials with Tc < TFM. Furthermore, a novel feature of these materials is that they exhibit a dual and quite unusual hysteresis loop corresponding to both the ferromagnetism and the coexisting bulk superconductivity.
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From temperature and magnetic field dependent point-contact spectroscopy on the ferromagnetic superconductor Sr0.5Ce0.5FBiS2 (bulk superconducting [Formula: see text] K) we observe (a) a pseudogap in the normal state that sustains to a remarkably high temperature of 40 K and (b) two-fold enhancement of T c upto 5 K in the point-contact geometry. In addition, Andreev reflection spectroscopy reveals a superconducting gap of 6 meV for certain point-contacts suggesting that the mean field T c of this system could be approximately 40 K, the onset temperature of pseudo-gap. Our results suggest that quantum fluctuations originating from other competing orders in Sr0.5Ce0.5FBiS2 forbid a global phase coherence at high temperatures thereby suppressing T c. Apart from the known ordering to a ferromagnetic state, our first-principles calculations reveal nesting of a multi-band Fermi surface and a significant electron-phonon coupling that could result in charge density wave-like instabilities.
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A graphitic carbon nitride (g-C3 N4 ) polymer matrix was embedded with AgNi alloy nanoparticles using a simple and direct inâ situ solid-state heat treatment method to develop a novel AgNi/g-C3 N4 photocatalyst. The characterization confirms that the AgNi alloy particles are homogeneously distributed throughout the g-C3 N4 matrix. The catalyst shows excellent photoelectrochemical activity for water splitting with a maximum photocurrent density of 1.2â mA cm-2 , which is the highest reported for doped g-C3 N4 . Furthermore, a detailed experimental study of the photocatalytic degradation of Rhodamine B (RhB) dye using doped g-C3 N4 showed the highest reported degradation efficiency of approximately 95 % after 90â min. The electronic conductivity increased upon incorporation of AgNi alloy nanoparticles on g-C3 N4 and the material showed efficient charge carrier separation and transfer characteristics, which are responsible for the enhanced photoelectrochemical and photocatalytic performance under visible light.