X-ray studies of magnetic and structural transitions in iridates

In this thesis, I describe x-ray experiments that rst detect the symmetry breaking at magnetic and structural transitions in iridium based transition metal oxides, and then characterise the ensuing state. The magnetic transition in pyrochlore iridates R2Ir2O7, where R = Sm, Nd and Tb, was studied with resonant x-ray scattering at the Ir L3 edge. In all samples, k = 0 magnetic order was discovered below 120 K (Sm), 5 K (Nd) and 78 K (Tb), respectively. It is demonstrated how resonant x-ray scattering can determine the size of the magnetic moment, yielding approximately 0:3 B (Sm) and 0:06 B (Tb). The magnetic dynamics of Sm and Nd pyrochlores could be well described by excitations from an all-in all-out magnetic structure within a minimal nearest-neighbour Hamiltonian of Heisenberg exchange (27 meV) and Dzyaloshinskii-Moriya interactions (5 meV). This provides a consistent description of the magnetic order and excitations, and suggests that a topological Weyl semimetal could be realised in pyrochlore iridates. A structural transition from tetragonal to monoclinic symmetry was discovered in the perovskite iridate Sr3Ir2O7 at 54 GPa using x-ray di raction. The high-pressure phase adopts an altered stacking sequence of perovskite layers, and may coupled to the emergence of a metallic state. X-ray absorption spectroscopy was used to characterise the resulting electronic state at high pressure. Compared to the spin-orbit induced insulating state at ambient conditions, the in uence of spin-orbit coupling in the high-pressure, metallic phase appears diminished

Anisotropic exchange and spin-wave damping in pure and electron-doped Sr2_2IrO4_4

The collective magnetic excitations in the spin-orbit Mott insulator (Sr$_{1-x}$La$_x$)$_2$IrO$_4$ ($x=0,\,0.01,\,0.04,\, 0.1$) were investigated by means of resonant inelastic x-ray scattering. We report significant magnon energy gaps at both the crystallographic and antiferromagnetic zone centers at all doping levels, along with a remarkably pronounced momentum-dependent lifetime broadening. The spin-wave gap is accounted for by a significant anisotropy in the interactions between $J_\text{eff}=1/2$ isospins, thus marking the departure of Sr$_2$IrO$_4$ from the essentially isotropic Heisenberg model appropriate for the superconducting cuprates.Comment: 6 pages, 4 figure

Evolution of the magnetic excitations in NaOsO3_3 through its metal-insulator transition

The temperature dependence of the excitation spectrum in NaOsO$_{\text{3}}$ through its metal-to-insulator transition (MIT) at 410 K has been investigated using resonant inelastic X-ray scattering (RIXS) at the Os L$_{\text{3}}$ edge. High resolution ($\Delta E \sim$ 56 meV) measurements show that the well-defined, low energy magnons in the insulating state weaken and dampen upon approaching the metallic state. Concomitantly, a broad continuum of excitations develops which is well described by the magnetic fluctuations of a nearly antiferromagnetic Fermi liquid. By revealing the continuous evolution of the magnetic quasiparticle spectrum as it changes its character from itinerant to localized, our results provide unprecedented insight into the nature of the MIT in NaOsO$_{\text{3}}$.Comment: Accepted in Physical Review Letters, part of a joint submission to Physical Review B. Supersedes arXiv:1707.0555

Crossover from itinerant to localized magnetic excitations through the metal-insulator transition in NaOsO3_{\text{3}}

NaOsO$_{\text{3}}$ undergoes a metal-insulator transition (MIT) at 410 K, concomitant with the onset of antiferromagnetic order. The excitation spectra have been investigated through the MIT by resonant inelastic x-ray scattering (RIXS) at the Os L$_{\text{3}}$ edge. Low resolution ($\Delta E \sim$ 300 meV) measurements over a wide range of energies reveal that local electronic excitations do not change appreciably through the MIT. This is consistent with a picture in which structural distortions do not drive the MIT. In contrast, high resolution ($\Delta E \sim$ 56 meV) measurements show that the well-defined, low energy magnons in the insulating state weaken and dampen upon approaching the metallic state. Concomitantly, a broad continuum of excitations develops which is well described by the magnetic fluctuations of a nearly antiferromagnetic Fermi liquid. By revealing the continuous evolution of the magnetic quasiparticle spectrum as it changes its character from itinerant to localized, our results provide unprecedented insight into the nature of the MIT in \naoso. In particular, the presence of weak correlations in the paramagnetic phase implies a degree of departure from the ideal Slater limit.Comment: Joint submission with Physical Review Letters [Phys. Rev. Lett. 120, 227203 (2018), accepted version at arXiv:1805.03176]. This article includes further discussion about the calculations performed, models used, and so o

Spin and orbital dynamics through the metal-to-insulator transition in Cd2_2Os2_2O7_7 probed with high-resolution RIXS

High-resolution resonant inelastic x-ray scattering (RIXS) measurements ($\Delta$E = 46 meV) have been performed on Cd$_2$Os$_2$O$_7$ through the metal-to-insulator transition (MIT). A magnetic excitation at 125 meV evolves continuously through the MIT, in agreement with recent Raman scattering results, and provides further confirmation for an all-in, all-out magnetic ground state. Asymmetry of this feature is likely a result of coupling between the electronic and magnetic degrees of freedom. We also observe a broad continuum of interband excitations centered at 0.3 eV energy loss. This is indicative of significant hybridization between Os 5$d$ and O 2$p$ states, and concurrent itinerant nature of the system. In turn, this suggests a possible break down of the free-ion model for Cd$_2$Os$_2$O$_7$.Comment: Accepted in Physical Review B (10 pages

Neuroantibodies: Ectopic expression of a recombinant anti-substance P antibody in the central nervous system of transgenic mice

AbstractRecombinant antibodies are efficiently secreted by cells of the nervous system. Thus, their local expression in the CNS of transgenic mice could be used to perturb the function of the corresponding antigen. As a first application of this approach, we have generated transgenic mice that express antibodies against the neuropeptide substance P, under the transcriptional control of the promoter of the neuronal gene vgf. The transgenic antibodies are expressed in a tissue-specific and developmentally regulated manner and are effective in competing with the endogenous substance P, as demonstrated by a marked Inhibition of neurogenic inflammation and by motor deficits. This phenotypic knockout approach may provide a complementary alternative to gene knockout by homologous recombination

Strongly Gapped Spin-Wave Excitation in the Insulating Phase of NaOsO3

NaOsO3 hosts a rare manifestation of a metal-insulator transition driven by magnetic correlations, placing the magnetic exchange interactions in a central role. We use resonant inelastic x-ray scattering to directly probe these magnetic exchange interactions. A dispersive and strongly gapped (58 meV) excitation is observed indicating appreciable spin-orbit coupling in this 5d3 system. The excitation is well described within a minimal model Hamiltonian with strong anisotropy and Heisenberg exchange (J1=J2=13.9 meV). The observed behavior places NaOsO3 on the boundary between localized and itinerant magnetism

All-in all-out magnetic order and propagating spin-waves in Sm2Ir2O7

Using resonant magnetic x-ray scattering we address the unresolved nature of the magnetic groundstate and the low-energy effective Hamiltonian of Sm2Ir2O7, a prototypical pyrochlore iridate with a finite temperature metal-insulator transition. Through a combination of elastic and inelastic measurements, we show that the magnetic ground state is an all-in all-out (AIAO) antiferromagnet. The magnon dispersion indicates significant electronic correlations and can be well-described by a minimal Hamiltonian that includes Heisenberg exchange (J = 27:3(6) meV) and Dzyaloshinskii- Moriya interaction (D = 4:9(3) meV), which provides a consistent description of the magnetic order and excitations. In establishing that Sm2Ir2O7 has the requisite inversion symmetry preserv- ing AIAO magnetic groundstate, our results support the notion that pyrochlore iridates may host correlated Weyl semimetals