The magnetic structure and electronic ground state of the layered perovskite Ba(2)IrO(4) have been investigated using x-ray resonant magnetic scattering. Our results are compared with those for Sr(2)IrO(4), for which we provide supplementary data on its magnetic structure. We find that the dominant, long-range antiferromagnetic order is remarkably similar in the two compounds and that the electronic ground state in Ba(2)IrO(4), deduced from an investigation of the x-ray resonant magnetic scattering L(3)/L(2) intensity ratio, is consistent with a J(eff)=1/2 description. The robustness of these two key electronic properties to the considerable structural differences between the Ba and Sr analogues is discussed in terms of the enhanced role of the spin-orbit interaction in 5d transition metal oxides.
We report on a detailed x-ray resonant scattering study of the bilayer iridate compound Sr 3 Ir 2 O 7 at the Ir L 2 and L 3 edges. Resonant scattering at the Ir L 3 edge has been used to determine that Sr 3 Ir 2 O 7 is a long-range ordered antiferromagnet below T N ≈ 230 K with an ordering wave vector q = ( 1 2 , 1 2 ,0). The energy resonance at the L 3 edge was found to be a factor of ∼30 times larger than that at the L 2 edge. This remarkable effect has been seen in the single-layer compound Sr 2 IrO 4 and has been linked to the observation of a J eff = 1 2 spin-orbit insulator. Our result shows that despite the modified electronic structure of the bilayer compound, caused by the larger bandwidth, the effect of strong spin-orbit coupling on the resonant magnetic scattering persists. Using the program SARAh, we have determined that the magnetic order consists of two domains with propagation vectors k 1 = ( 1 2 , 1 2 ,0) and k 2 = ( 1 2 , − 1 2 ,0), respectively. A raster measurement of a focused x-ray beam across the surface of the sample yielded images of domains of the order of 100 μm, with odd and even L components, respectively. Fully relativistic, monoelectronic calculations using the Green's function technique for a muffin-tin potential have been employed to calculate the relative intensities of the L 2,3 edge resonances, comparing the effects of including spin-orbit coupling and the Hubbard U term. A large L 3 to L 2 edge intensity ratio (∼5) was found for calculations including spin-orbit coupling. Adding the Hubbard U term had no significant effect on the calculated spectra.
Sr2IrO4 is a prototype of the class of Mott insulators in the strong spin-orbit interaction (SOI) limit described by a Jeff = 1/2 ground state. In Sr2IrO4, the strong SOI is predicted to manifest itself in the locking of the canting of the magnetic moments to the correlated rotation by 11.8(1)° of the oxygen octahedra that characterizes its distorted layered perovskite structure. Using x-ray resonant scattering at the Ir L3 edge we have measured accurately the intensities of Bragg peaks arising from different components of the magnetic structure. From a careful comparison of integrated intensities of peaks due to basal-plane antiferromagnetism, with those due to b-axis ferromagnetism, we deduce a canting of the magnetic moments of 12.2(8)°. We thus confirm that in Sr2IrO4 the magnetic moments rigidly follow the rotation of the oxygen octahedra, indicating that, even in the presence of significant non-cubic structural distortions, it is a close realization of the Jeff = 1/2 state.
The magnetic critical scattering in Sr 2 IrO 4 has been characterized using x-ray resonant magnetic scattering (XRMS) both below and above the three-dimensional antiferromagnetic ordering temperature T N . The order parameter critical exponent below T N is found to be β = 0.195(4), in the range of the two-dimensional (2D) XY h 4 universality class. Over an extended temperature range above T N , the amplitude and correlation length of the intrinsic critical fluctuations are well described by the 2D Heisenberg model with XY anisotropy. This contrasts with an earlier study of the critical scattering over a more limited range of temperature, which found agreement with the theory of the isotropic 2D Heisenberg quantum antiferromagnet, developed to describe the critical fluctuations of the conventional Mott insulator La 2 CuO 4 and related systems. Our study therefore establishes the importance of XY anisotropy in the low-energy effective Hamiltonian of Sr 2 IrO 4 , the prototypical spin-orbit Mott insulator. The Ruddlesden-Popper series Sr n+1 Ir n O 3n+1 of perovskite iridates has emerged as a fruitful arena in which to explore the effects of electron correlations in the strong spin-orbit coupling limit. The first two members of this series, single-layer Sr 2 IrO 4 (n = 1) and bilayer Sr 3 Ir 2 O 7 (n = 2), are believed to exemplify a new class of spin-orbit Mott insulators. Of central importance to our understanding of these materials is the emergence of a j eff = 1/2 ground state by the combined action of a strong cubic crystal field and spin-orbit interactions on the 5d 5 electrons of the Ir 4+ ions [1]. The weakened electron correlations typical of the 5d elements then split the j eff = 1/2 band, opening a gap, leading to a Mott-like state.Sr 2 IrO 4 in particular has attracted considerable attention because of its striking similarities to La 2 CuO 4 in terms of both its structural and magnetic properties. The magnetic structures and excitations of Sr 2 IrO 4 have been investigated in a number of x-ray resonant magnetic scattering (XRMS) studies [1][2][3][4][5][6][7] which have allowed an effective low-energy Hamiltonian to be proposed and refined. Sr 2 IrO 4 forms an antiferromagnetic structure below T N ∼ 225 K in which the moments are confined to the a − b planes and canted to follow rigidly the correlated rotation of the oxygen octahedra of the I 4 1 /acd crystal structure [8]. A resonant inelastic x-ray scattering (RIXS) experiment [2] has revealed a dispersion relation somewhat reminiscent of that displayed by La 2 CuO 4 , albeit with a lower-energy scale and much stronger further neighbor couplings, which can be derived from a smaller ratio of on-site repulsion over hopping amplitude [9]. This result * j.vale@ucl.ac.uk suggests that the low-energy isospin dynamics of the j eff = 1/2 states in Sr 2 IrO 4 may, to leading order, be mapped onto an effective isotropic two-dimensional Heisenberg Hamiltonian, in agreement with predictions by Jackeli and Khaliullin [10].Critical scattering studies provide informa...
Abstract. This report presents azimuthal dependent and polarisation dependent xray resonant magnetic scattering at the Ir L 3 edge for the bilayered iridate compound, Sr 3 Ir 2 O 7 . Two magnetic wave vectors, k 1 =( 1 2 , 1 2 ,0) and k 2 =( 1 2 ,-1 2 ,0), result in domains of two symmetry-related G-type antiferromagnetic structures, noted A and B, respectively. These domains are approximately 0.02 mm 2 and are independent of the thermal history. An understanding of this key aspect of the magnetism is necessary for an overall picture of the magnetic behaviour in this compound. Azimuthal and polarisation dependence of magnetic reflections, relating to both magnetic wave vectors, show that the Ir magnetic moments in the bilayer compound are oriented along the c axis. This contrasts with single layer Sr 2 IrO 4 where the moments are confined to the ab plane.
The low-energy electronic structure of the J(eff) = 1/2 spin-orbit insulator Sr3Ir2O7 has been studied by means of angle-resolved photoemission spectroscopy. A comparison of the results for bilayer Sr3Ir2O7 with available literature data for the related single-layer compound Sr2IrO4 reveals qualitative similarities and similar J(eff) = 1/2 bandwidths for the two materials, but also pronounced differences in the distribution of the spectral weight. In particular, photoemission from J(eff) = 1/2 the states appears to be suppressed. Yet, it is found that the Sr3Ir2O7 data are in overall better agreement with band-structure calculations than the data for Sr2IrO4.
The chemical and magnetic structures of the series of compounds Ca 2−x La x RuO 4 [x = 0, 0.05(1), 0.07(1), 0.12(1)] have been investigated using neutron diffraction and resonant elastic x-ray scattering. Upon La doping, the low-temperature S-P bca space group of the parent compound is retained in all insulating samples [x 0.07(1)], but with significant changes to the atomic positions within the unit cell. These changes can be characterized in terms of the local RuO 6 octahedral coordination: with increasing doping, the structure, crudely speaking, evolves from an orthorhombic unit cell with compressed octahedra to a quasitetragonal unit cell with elongated ones. The magnetic structure on the other hand, is found to be robust, with the basic k = (0,0,0), b-axis antiferromagnetic order of the parent compound preserved below the critical La doping concentration of x ≈ 0.11. The only effects of La doping on the magnetic structure are to suppress the A-centred mode, favoring the B mode instead, and to reduce the Néel temperature somewhat. Our results are discussed with reference to previous experimental reports on the effects of cation substitution on the d 4 Mott insulator Ca 2 RuO 4 , as well as with regard to theoretical studies on the evolution of its electronic and magnetic structure. In particular, our results rule out the presence of a proposed ferromagnetic phase, and suggest that the structural effects associated with La substitution play an important role in the physics of the system.
The resonant x-ray scattering (magnetic elastic, RXMS, and inelastic, RIXS) of Ir4+ at the L2,3 edges relevant to spin-orbit Mott insulators A(n+1)Ir(n)O(3n+1) (A = Sr, Ba, etc.) are calculated using a single-ion model which treats the spin-orbit and tetragonal crystal-field terms on an equal footing. Both RXMS and RIXS in the spin-flip channel are found to display a nontrivial dependence on the direction of the magnetic moment, μ. Crucially, we show that for μ in the ab plane, RXMS in the cross-polarized channel at the L2 edge is zero irrespective of the tetragonal crystal field; spin-flip RIXS, relevant to measurements of magnons, behaves reciprocally, being zero at L2 when μ is perpendicular to the ab plane. Our results have important implications for the assignment of a j(eff) = 1/2 ground state on the basis of resonant x-ray experiments.
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