No Arabic abstract
We report the results of ac and dc magnetization (M) and heat-capacity (C) measurements on the solid solution, Sr$_3$Cu$_{1-x}$Zn$_x$IrO$_6$. While the Zn end member is known to form in a rhombohedral pseudo one-dimensional K$_4$CdCl$_6$ structure with an antiferromagnetic ordering temperature of (T$_N$ =) 19 K, the Cu end member has been reported to form in a monoclinically distorted form with a Curie temperature of (T$_C$ =) 19 K. The magnetism of the Zn compound is found to be robust to synthetic conditions and is broadly consistent with the behavior known in the literature. However, we find a lower magnetic ordering temperature (T$_o$) for our Cu compound (~ 13 K), thereby suggesting that T$_o$ is sensitive to synthetic conditions. The Cu sample appears to be in a spin-glass-like state at low temperatures, judged by a frequency dependence of ac magnetic susceptibility and a broadening of the C anomaly at the onset of magnetic ordering, in sharp contrast to earlier proposals. Small applications of magnetic field, however, drive this system to ferromagnetism as inferred from the M data. Small substitutions for Cu/Zn (x = 0.75 or 0.25) significantly depress magnetic ordering; in other words, T$_o$ varies non-monotonically with x (T$_o$ ~ 6, 3 and 4 K for x = 0.25, 0.5, and 0.67 respectively). The plot of inverse susceptibility versus temperature is non-linear in the paramagnetic state as if correlations within (or among) the magnetic chains continuously vary with temperature. The results establish
We report the signatures of dynamic spin fluctuations in the layered honeycomb Li$_3$Cu$_2$SbO$_6$ compound, with a 3$d$ S = 1/2 $d^9$ Cu$^{2+}$ configuration, through muon spin rotation and relaxation ($mu$SR) and neutron scattering studies. Our zero-field (ZF) and longitudinal-field (LF)-$mu$SR results demonstrate the slowing down of the Cu$^{2+}$ spin fluctuations below 4.0 K. The saturation of the ZF relaxation rate at low temperature, together with its weak dependence on the longitudinal field between 0 and 3.2 kG, indicates the presence of dynamic spin fluctuations persisting even at 80 mK without static order. Neutron scattering study reveals the gaped magnetic excitations with three modes at 7.7, 13.5 and 33 meV. Our DFT calculations reveal that the next nearest neighbors (NNN) AFM exchange ($J_{AFM}$ = 31 meV) is stronger than the NN FM exchange ($J_{FM}$ = -21 meV) indicating the importance of the orbital degrees of freedom. Our results suggest that the physics of Li$_3$Cu$_2$SbO$_6$ can be explained by an alternating AFM chain rather than the honeycomb lattice.
Double-perovskite oxides that contain both 3d and 5d transition metal elements have attracted growing interest as they provide a model system to study the interplay of strong electron interaction and large spin-orbit coupling (SOC). Here, we report on experimental and theoretical studies of the magnetic and electronic properties of double-perovskites (La$_{1-x}$Sr$_x$)$_2$CuIrO$_6$ ($x$ = 0.0, 0.1, 0.2, and 0.3). The undoped La$_2$CuIrO$_6$ undergoes a magnetic phase transition from paramagnetism to antiferromagnetism at T$_N$ $sim$ 74 K and exhibits a weak ferromagnetic behavior below $T_C$ $sim$ 52 K. Two-dimensional magnetism that was observed in many other Cu-based double-perovskites is absent in our samples, which may be due to the existence of weak Cu-Ir exchange interaction. First-principle density-functional theory (DFT) calculations show canted antiferromagnetic (AFM) order in both Cu$^{2+}$ and Ir$^{4+}$ sublattices, which gives rise to weak ferromagnetism. Electronic structure calculations suggest that La$_2$CuIrO$_6$ is an SOC-driven Mott insulator with an energy gap of $sim$ 0.3 eV. Sr-doping decreases the magnetic ordering temperatures ($T_N$ and $T_C$) and suppresses the electrical resistivity. The high temperatures resistivity can be fitted using a variable-range-hopping model, consistent with the existence of disorders in these double-pervoskite compounds.
Ac and dc magnetization and heat-capacity (C) measurements performed on the pseudo-one-dimensional compound Sr$_3$CuIrO$_6$ reveal a competition between antiferromagnetic (AF) and ferromagnetic (F) exchange couplings, as evidenced by frequency dependence of ac susceptibility and by the absence of a C anomaly at the magnetic transition. The value of the saturation moment (about 0.35 $mu_B$/formula unit) is much smaller than expected for ferromagnetism from the two S=1/2 ions (Cu and Ir). Thus, this compound is not a ferromagnet in zero magnetic field, in contrast to earlier beliefs. Of particular importance is the finding that the value of the magnetic ordering temperature is sample dependent, sensitive to synthetic conditions resulting from deviations in oxygen/Cu content. We propose that this compound serves as a unique model system to test theories on random AF-F interaction in a chain system, considering that this competition can be tuned without any chemical substitution.
Oxides containing iridium ions display a range of magnetic and conducting properties that depend on the delicate balance between interactions and are controlled, at least in part, by the details of the crystal architecture. We have used muon-spin rotation ($mu$SR) to study the local field in four iridium oxides, Ca$_4$IrO$_6$, Ca$_5$Ir$_3$O$_{12}$, Sr$_3$Ir$_2$O$_7$ and Sr$_2$IrO$_4$, which show contrasting behavior. Our $mu$SR data on Ca$_4$IrO$_6$ and Ca$_5$Ir$_3$O$_{12}$ are consistent with conventional antiferromagnetism where quasistatic magnetic order develops below $T_{rm N}=13.85(6)$ K and 7.84(7) K respectively. A lower internal field is observed for Ca$_5$Ir$_3$O$_{12}$, as compared to Ca$_4$IrO$_6$ reflecting the presence of both Ir$^{4+}$ and Ir$^{5+}$ ions, resulting in a more magnetically dilute structure. Muon precession is only observed over a restricted range of temperature in Sr$_3$Ir$_2$O$_7$, while the Mott insulator Sr$_2$IrO$_4$ displays more complex behavior, with the $mu$SR signal containing a single, well-resolved precession signal below $T_{rm N}=230$,K, which splits into two precession signals at low temperature following a reorientation of the spins in the ordered state.
We have systematically studied the magnetic properties of Cu$_{4-x}$Zn$_x$(OH)$_6$FBr by the neutron diffraction and muon spin rotation and relaxation ($mu$SR) techniques. Neutron-diffraction measurements suggest that the long-range magnetic order and the orthorhombic nuclear structure in the $x$ = 0 sample can persist up to $x$ = 0.23 and 0.43, respectively. The temperature dependence of the zero-field (ZF) $mu$SR spectra provide two characteristic temperatures, $T_{A0}$ and $T_{lambda}$. Comparison between $T_{A0}$ and $T_M$ from previously reported magnetic-susceptibility measurements suggest that the former comes from the short-range interlayer-spin clusters that persist up to $x$ = 0.82. On the other hand, the doping level where $T_{lambda}$ becomes zero is about 0.66, which is much higher than threshold of the long-range order, i.e., $sim$ 0.4. Our results suggest that the change in the nuclear structure may alter the spin dynamics of the kagome layers and a gapped quantum-spin-liquid state may exist above $x$ = 0.66 with the perfect kagome planes.