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Register a new userSite-selective $d^{10}$/$d^0$ substitution in a $S = 1/2$ spin ladder Ba$_2$CuTe$_{1-x}$W$_x$O$_6$ ($0 leq x leq 0.3$)
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Remarkably, doping isovalent $d^{10}$ and $d^0$ cations onto the $B$ site in $A_2B$$B$O$_6$ double perovskites has the power to direct the magnetic interactions between magnetic $B$ cations. This is due to changes in orbital hybridization, which favors different superexchange pathways, and leads to the formation of alternative magnetic structures depending on whether $B$ is $d^{10}$ or $d^0$. Furthermore, the competition generated by introducing mixtures of $d^{10}$ and $d^0$ cations can drive the material into the realms of exotic quantum magnetism. Here, a W$^{6+}$ $d^0$ dopant was introduced to a $d^{10}$ hexagonal perovskite Ba$_2$CuTeO$_6$, which possesses a spin ladder geometry of Cu$^{2+}$ cations, creating a Ba$_2$CuTe$_{1-x}$W$_x$O$_6$ solid solution ($x$ = 0 - 0.3). Neutron and synchrotron X-ray diffraction show that W$^{6+}$ is almost exclusively substituted for Te$^{6+}$ on the corner-sharing site within the spin ladder, in preference to the face-sharing site between ladders. This means the intra-ladder interactions are selectively tuned by the $d^0$ cations. Bulk magnetic measurements suggest this suppresses magnetic ordering in a similar manner to that observed for the spin-liquid like material Sr$_2$CuTe$_{1-x}$W$_x$O$_6$. This further demonstrates the utility of $d^{10}$ and $d^0$ dopants as a tool for tuning magnetic ground states in a wide range of perovskites and perovskite-derived structures.
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The 3$d$-5$d$ based double perovskites offer an ideal playground to study the interplay between electron correlation ($U$) and spin-orbit coupling (SOC) effect, showing exotic physics. The Sr$_2$FeIrO$_6$ is an interesting member in this family with ionic distribution of Fe$^{3+}$ (3$d^5$) and Ir$^{5+}$ (5$d^4$) where the later is believed to be nonmagnetic under the picture of strong SOC. Here, we report detailed investigation of structural, magnetic and electronic transport properties along with electronic structure calculations in (Sr$_{1-x}$Ca$_x$)$_2$FeIrO$_6$ series with $x$ from 0 to 1. While the basic interactions such as, $U$ and SOC are unlikely to be modified but a structural modification is expected due to ionic size difference between Sr$^{2+}$ and Ca$^{2+}$ which would influence other properties such as crystal field effect and band widths. While a nonmonotonic changes in lattice parameters are observed across the series, the spectroscopic investigations reveal that 3+/5+ charge state of Fe/Ir continue till end of the series. An analysis of magnetic data suggests similar nonmonotonic evolution of magnetic parameters with doping. Temperature dependent crystal structure as well as low temperature (5 K) magnetic structure have been determined from neutron powder diffraction measurements. The whole series shows insulating behavior. The electronic structure calculations show, SOC enhanced, a noncollinear antiferromagnetic and Mott-type insulating state is the stable ground state for present series with a substantial amount of orbital moment, but less than the spin magnetic moment, at the Ir site and the magnetocrystalline anisotropy. The obtained results imply that the Ca$^{2+}$ has large influence on the magnetic and transport properties, further showing a large agreement between experimental results as well as theoretical calculations.
We report the successful synthesis of FeSe$_{1-x}$S$_{x}$ single crystals with $x$ ranging from 0 to 1 via a hydrothermal method. A complete phase diagram of FeSe$_{1-x}$S$_{x}$ has been obtained based on resistivity and magnetization measurements. The nematicity is suppressed with increasing $x$, and a small superconducting dome appears within the nematic phase. Outside the nematic phase, the superconductivity is continuously suppressed and reaches a minimum $T_c$ at $x$ = 0.45; beyond this point, $T_c$ slowly increases until $x$ = 1. Intriguingly, an anomalous resistivity upturn with a characteristic temperature $T^*$ in the intermediate region of $0.31 leq x leq 0.71$ is observed. $T^{*}$ shows a dome-like behavior with a maximum value at $x$ = 0.45, which is opposite the evolution of $T_c$, indicating competition between $T^*$ and superconductivity. The origin of $T^*$ is discussed in detail. Furthermore, the normal state resistivity evolves from non-Fermi-liquid to Fermi-liquid behavior with S doping at low temperatures, accompanied by a reduction in electronic correlations. Our study addresses the lack of single crystals in the high-S doping region and provides a complete phase diagram, which will promote the study of relations among nematicity, superconductivity, and magnetism.
We report on the emergence of robust superconducting order in single crystal alloys of 2H-TaSe$_{2-x}$S$_{x}$ (0$leq$x$leq$2) . The critical temperature of the alloy is surprisingly higher than that of the two end compounds TaSe$_{2}$ and TaS$_{2}$. The evolution of superconducting critical temperature T$_{c} (x)$ correlates with the full width at half maximum of the Bragg peaks and with the linear term of the high temperature resistivity. The conductivity of the crystals near the middle of the alloy series is higher or similar than that of either one of the end members 2H-TaSe$_{2}$ and/or 2H-TaS$_{2}$. It is known that in these materials superconductivity (SC) is in close competition with charge density wave (CDW) order. We interpret our experimental findings in a picture where disorder tilts this balance in favor of superconductivity by destroying the CDW order.
Electron-electron (e-e) and electron-hole (e-h) interactions are often associated with many exotic phenomena in correlated electron systems. Here, we report an observation of anomalous excitons at 3.75 , 4.67 and 6.11 eV at 4.2 K in bulk-SrTiO$_3$. Fully supported by ab initio GW Bethe-Salpeter equation calculations, these excitons are due to surprisingly strong e-h and e-e interactions with different characters: 4.67 and 6.11 eV are resonant excitons and 3.75 eV is a bound Wannier-like exciton with an unexpectedly higher level of delocalization. Measurements and calculations on SrTi$_{1-x}$Nb$_x$O$_3$ for 0.0001$leq$x$leq$0.005 further show that energy and spectral-weight of the excitonic peaks vary as a function of electron doping (x) and temperature, which are attributed to screening effects. Our results show the importance of e-h and e-e interactions yielding to anomalous excitons and thus bring out a new fundamental perspective in SrTiO$_3$.
A quantum spin liquid state has long been predicted to arise in spin-1/2 Heisenberg square-lattice antiferromagnets at the boundary region between Neel (nearest-neighbor interaction dominates) and columnar (next-nearest-neighbor dominates) antiferromagnetic order. However, there are no known compounds in this region. Here we use $d^{10}$-$d^0$ cation mixing to tune the magnetic interactions on the square lattice while simultaneously introducing disorder. We find spin-liquid-like behavior in the double perovskite Sr$_2$Cu(Te$_{0.5}$W$_{0.5}$)O$_6$, where the isostructural end phases Sr$_2$CuTeO$_6$ and Sr$_2$CuWO$_6$ are Neel and columnar type antiferromagnets, respectively. We show that magnetism in Sr$_2$Cu(Te$_{0.5}$W$_{0.5}$)O$_6$ is entirely dynamic down to 19 mK. Additionally, we observe at low temperatures for Sr$_2$Cu(Te$_{0.5}$W$_{0.5}$)O$_6$, similar to several spin liquid candidates, a plateau in muon spin relaxation rate and a strong $T$-linear dependence in specific heat. Our observations for Sr$_2$Cu(Te$_{0.5}$W$_{0.5}$)O$_6$ highlight the role of disorder in addition to magnetic frustration in spin liquid physics.
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