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We investigated the iron-based ladder compounds (Ba,Cs)Fe$_2$Se$_3$. Their parent compounds, BaFe$_2$Se$_3$ and CsFe$_2$Se$_3$, have different space groups, formal valences of Fe and magnetic structures. Electrical resistivity, specific heat, magneti c susceptibility, X-ray diffraction and powder neutron diffraction measurements were conducted to obtain temperature and composition phase diagram of this system. Block magnetism observed in BaFe$_2$Se$_3$ is drastically suppressed with Cs doping. In contrast, stripe magnetism observed in CsFe$_2$Se$_3$ is not so fragile against Ba doping. New type of magnetic structure appears in intermediate compositions, which is similar to stripe magnetism of CsFe$_2$Se$_3$, but inter-ladder spin configuration is different. Intermediate compounds show insulating behavior, nevertheless finite $T$-linear contribution in specific heat was obtained at low temperatures.
Resonant x-ray diffraction experiments were performed for the metallic iridium oxide IrO$_{2}$. We observed anisotropic tensor of susceptibility (ATS) scattering, the spectrum of which shows a sharp contrast between the $L_{3}$ and $L_{2}$ edges. At the $L_{3}$ edge, resonance excitations were clearly observed from the core 2$p$ orbitals to both the 5$d$ $t_{2g}$ and $e_{g}$ orbitals. In contrast, the resonance mode associated with 5$d$ $t_{2g}$ orbitals was indiscernible at the $L_{2}$ edge. This contrasting behavior indicates that Ir 5$d$ $t_{2g}$ orbitals are fairly close to the $J_{rm eff}$ = 1/2 state due to the strong spin--orbit coupling in 5$d$ transition metal ions, as in the Mott insulator Sr$_{2}$IrO$_{4}$. Our results clearly demonstrate that ATS scattering is a useful probe for investigating complex orbital states in a metallic state. Such states induce novel phenomena such as the spin Hall effect.
Magnetism in the insulating BaFe$_2$Se$_3$ was examined through susceptibility, specific heat, resistivity and neutron diffraction measurements. After formation of a short-range magnetic correlation, a long-range ordering was observed below $T_{rm N} sim 255$ K. The transition is obscured by bulk properties. Magnetic moments ($parallel a$) are arranged to form a Fe$_4$ ferromagnetic unit, and each Fe$_4$ stacks antiferromagnetically. This block magnetism is of the third type among magnetic structures of ferrous materials. The magnetic ordering drives unusually large distortion via magnetoelastic coupling.
We performed resonant x-ray diffraction experiments at the $L$ absorption edges for the post-perovskite-type compound CaIrO$_{3}$ with $(t_{2g})^5$ electronic configuration. By observing the magnetic signals, we could clearly see that the magnetic st ructure was a striped order with an antiferromagnetic moment along the c-axis and that the wavefunction of a $t_{2g}$ hole is strongly spin-orbit entangled, the $J_{rm eff} =1/2$ state. The observed spin arrangement is consistent with theoretical work predicting a unique superexchange interaction in the $J_{rm eff} =1/2$ state and points to the universal importance of the spin-orbit coupling in Ir oxides, irrespective of the local coordination and lattice topology. We also propose that the non-magnetic resonant scattering is a powerful tool for unraveling an orbital state even in a metallic iridate.
We report results of 75As nuclear magnetic resonance (NMR) experiments on a self-flux grown high-quality single crystal of SrFe2As2. The NMR spectra clearly show sharp first-order antiferromagnetic (AF) and structural transitions occurring simultaneo usly. The behavior in the vicinity of the transition is compared with our previous study on BaFe2As2. No significant difference was observed in the temperature dependence of the static quantities such as the AF splitting and electric quadrupole splitting. However, the results of the NMR relaxation rate revealed difference in the dynamical spin fluctuations. The stripe-type AF fluctuations in the paramagnetic state appear to be more anisotropic in BaFe2As2 than in SrFe2As2.
We report results of 75As nuclear magnetic resonance (NMR) experiments on a self-flux grown single crystal of BaFe2As2. A first-order antiferromagnetic (AF) transition near 135 K was detected by the splitting of NMR lines, which is accompanied by sim ultaneous structural transition as evidenced by a sudden large change of the electric field gradient tensor at the As site. The NMR results lead almost uniquely to the stripe spin structure in the AF phase. The data of spin-lattice relaxation rate indicate development of anisotropic spin fluctuations of the stripe-type with decreasing temperature in the paramagnetic phase.
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