arXiv subjects

S. Boseggia

Publications and source records attributed to S. Boseggia.

12 recordsLinked to original sources

arXiv2019

Critical fluctuations in the spin-orbit Mott insulator Sr$_3$Ir$_2$O$_7$

X-ray magnetic critical scattering measurements and specific heat measurements were performed on the perovskite iridate Sr$_3$Ir$_2$O$_7$. We find that the magnetic interactions close to the Néel temperature $T_N$ = 283.4(2) K are three-dimensional. This contrasts with previous studies which suggest two-dimensional behaviour like Sr$_2$IrO$_4$. Violation of the Harris criterion ($dν>2$) means that weak disorder becomes relevant. This leads a rounding of the antiferromagnetic phase transition at $T_N$, and modifies the critical exponents relative to the clean system. Specifically, we determine that the critical behaviour of Sr$_3$Ir$_2$O$_7$ is representative of the diluted 3D Ising universality class.

cond-mat.str-el↗

arXiv2018

Persistence of antiferromagnetic order upon La substitution in the $4d^4$ Mott insulator Ca$_2$RuO$_4$

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-Pbca space group of the parent compound is retained in all insulating samples [$x\leq0.07(1)$], but with significant changes to the atomic positions within the unit cell. These changes can be characterised 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 quasi-tetragonal 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 $x\approx0.11$. The only effects of La doping on the magnetic structure are to suppress the A-centred mode, favouring 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.

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arXiv2015

The importance of XY anisotropy in Sr2IrO4 revealed by magnetic critical scattering experiments

The magnetic critical scattering in Sr$_2$IrO$_4$ has been characterized using X-ray resonant magnetic scattering (XRMS) both below and above the 3D antiferromagnetic ordering temperature, T$_{\text{N}}$. The order parameter critical exponent below T$_{\text{N}}$ is found to be β=0.195(4), in the range of the 2D XYh$_4$ universality class. Over an extended temperature range above T$_{\text{N}}$, 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.

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arXiv2015

Evidence of quantum dimer excitations in Sr$_3$Ir$_2$O$_7$

The magnetic excitation spectrum in the bilayer iridate Sr$_3$Ir$_2$O$_7$ has been investigated using high-resolution resonant inelastic x-ray scattering (RIXS) performed at the iridium L$_3$ edge and theoretical techniques. A study of the systematic dependence of the RIXS spectrum on the orientation of the wavevector transfer, $\mathbf{Q}$, with respect to the iridium-oxide bilayer has revealed that the magnon dispersion is comprised of two branches well separated in energy and gapped across the entire Brillouin zone. Our results contrast with those of an earlier study which reported the existence of a single dominant branch. While these earlier results were interpreted as two overlapping modes within a spin-wave model of weakly coupled iridium-oxide planes, our results are more reminiscent of those expected for a system of weakly coupled dimers. In this latter approach the lower and higher energy modes find a natural explanation as those corresponding to transverse and longitudinal fluctuations, respectively. We have therefore developed a bond-operator theory which describes the magnetic dispersion in Sr$_3$Ir$_2$O$_7$ in terms of quantum dimer excitations. In our model dimerisation is produced by the leading Heisenberg exchange, $J_c$, which couples iridium ions in adjacent planes of the bilayer. The Hamiltonian also includes in plane exchange, $J$, as well as further neighbour couplings and relevant anisotropies. The bond-operator theory provides an excellent account of the dispersion of both modes, while the measured $\mathbf{Q}$ dependence of the RIXS intensities is in reasonable qualitative accord with the spin-spin correlation function calculated from the theory. We discuss our results in the context of the quantum criticality of bilayer dimer systems in the presence of anisotropic interactions derived from strong spin-orbit coupling.

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arXiv2014

Crystal field splitting in Sr$_{n+1}$Ir$_n$O$_{3n+1}$ ($n$ = 1, 2) iridates probed by x-ray Raman spectroscopy

Non-resonant Raman spectroscopy in the hard X-ray regime has been used to explore the electronic structure of the first two members of the Ruddlesden-Popper series Sr$_{n+1}$Ir$_n$O$_{3n+1}$ of iridates. By tuning the photon energy transfer around 530 eV we have been able to explore the oxygen K near edge structure with bulk sensitivity. The angular dependence of the spectra has been exploited to assign features in the 528-535 eV energy range to specific transitions involving the Ir 5d orbitals. This has allowed us to extract reliable values for both the t2g-eg splitting arising from the cubic component of the crystal field (10Dq), in addition to the splitting of the eg orbitals due to tetragonal distortions. The values we obtain are (3.8, 1.6) eV and (3.55, 1.9) eV for Sr$_2$IrO$_4$ and Sr$_3$Ir$_2$O$_7$, respectively.

cond-mat.str-el↗

arXiv2013

Orbital occupancies and the putative jeff = 1/2 groundstate in Ba2IrO4: a combined oxygen K edge XAS and RIXS study

The nature of the electronic groundstate of Ba2IrO4 has been addressed using soft X-ray absorption and inelastic scattering techniques in the vicinity of the oxygen K edge. From the polarization and angular dependence of XAS we deduce an approximately equal superposition of xy, yz and zx Ir4+ 5d orbitals. By combining the measured orbital occupancies, with the value of the spin-orbit coupling provided by RIXS, we estimate the crystal field splitting associated with the tetragonal distortion of the IrO6 octahedra to be small, Δ=50(50) meV. We thus conclude definitively that Ba2IrO4 is a close realization of a spin-orbit Mott insulator with a jeff = 1/2 groundstate, thereby overcoming ambiguities in this assignment associated with the interpretation of X-ray resonant scattering experiments.

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arXiv2013

Slaving of the magnetic moment canting to the correlated oxygen rotation in Sr2IrO4 revealed by X-ray resonant scattering

Sr2IrO4 is a prototype of the class of Mott insulators in the strong spin-orbit interaction (SOI) limit described by a $J_{\mathrm{eff}}=1/2$ ground state. In Sr2IrO4, the strong SOI is predicted to manifest itself in the slaving of the canting of the magnetic moments to the correlated rotation by 11.8(1)$^{\circ}$ of the oxygen octahedra that characterizes its distorted layered perovskite structure. Using X-ray resonant scattering at the Ir $L_3$ 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)$^{\circ}$. 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 $J_{\mathrm{eff}}=1/2$ state

cond-mat.str-el↗

arXiv2013

Resonant X-ray scattering and the $j_{\mathrm{eff}}=1/2$ electronic ground state in iridate perovskites

The resonant X-ray scattering (magnetic elastic, RXMS, and inelastic, RIXS) of Ir$^{4+}$ at the L$_{2,3}$ 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 non-trivial dependence on the direction of the magnetic moment, $\boldsymbolμ$. Crucially, we show that for $\boldsymbolμ$ in the \emph{ab}-plane, RXMS at the L$_2$ edge is zero \emph{irrespective} of the tetragonal crystal-field; spin-flip RIXS, relevant to measurements of magnons, behaves reciprocally being zero at L$_2$ when $\boldsymbolμ$ is perpendicular to the \emph{ab}-plane. Our results provide important insights into the interpretation of X-ray data from the iridates, including that a $j_{\mathrm{eff}}=1/2$ ground state cannot be assigned on the basis of L$_2$/L$_3$ intensity ratio alone.

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arXiv2012

Robustness of basal-plane antiferromagnetic order and the $J_{eff}=1/2$ state in single-layer iridate spin-orbit Mott insulators

The magnetic structure and electronic groundstate of the layered perovskite Ba2IrO4 have been investigated using x-ray resonant magnetic scattering (XRMS). Our results are compared with those for Sr2IrO4, 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 groundstate in Ba2IrO4, deduced from an investigation of the XRMS $L_3/L_2$ 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.

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arXiv2012

The J_{eff}=1/2 insulator Sr3Ir2O7 studied by means of angle-resolved photoemission spectroscopy

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 particuar, photoemission from the J_{eff}=1/2 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.

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arXiv2012

On the magnetic structure of Sr3Ir2O7: an x-ray resonant scattering study

This report presents azimuthal dependent and polarisation dependent x-ray resonant magnetic scattering at the Ir L3 edge for the bilayered iridate compound, Sr3Ir2O7. Two magnetic wave vectors, k1=(1/2,1/2,0) and k2=(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 Sr2IrO4 where the moments are confined to the ab plane.

cond-mat.str-el↗

arXiv2012

Antiferromagnetic order and domains in Sr3Ir2O7 probed by x-ray resonant scattering

This article reports a detailed x-ray resonant scattering study of the bilayer iridate compound, Sr3Ir2O7, at the Ir L2 and L3 edges. Resonant scattering at the Ir L3 edge has been used to determine that Sr3Ir2O7 is a long-range ordered antiferromagnet below TN 230K with an ordering wavevector, q=(1/2,1/2,0). The energy resonance at the L3 edge was found to be a factor of ~30 times larger than that at the L2. This remarkable effect has been seen in the single layer compound Sr2IrO4 and has been linked to the observation of a Jeff=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 programme SARAh, we have determined that the magnetic order consists of two domains with propagation vectors k1=(1/2,1/2,0) and k2=(1/2,-1/2,0), respectively. A raster measurement of a focussed x-ray beam across the surface of the sample yielded images of domains of the order of 100 microns size, with odd and even L components, respectively. Fully relativistic, monoelectronic calculations (FDMNES), using the Green's function technique for a muffin-tin potential have been employed to calculate the relative intensities of the L2,3 edge resonances, comparing the effects of including spin-orbit coupling and the Hubbard, U, term. A large L3 to L2 edge intensity ratio (~5) was found for calculations including spin-orbit coupling. Adding the Hubbard, U, term resulted in changes to the intensity ratio <5%.

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