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Register a new userX-ray scattering study of pyrochlore iridates: crystal structure, electronic and magnetic excitations
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James Patrick Clancy
Publication date
2015
fields
Physics
and research's language is
English
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We have investigated the structural, electronic, and magnetic properties of the pyrochlore iridates Eu2Ir2O7 and Pr2Ir2O7 using a combination of resonant elastic x-ray scattering, x-ray powder diffraction, and resonant inelastic x-ray scattering (RIXS). The structural parameters of Eu2Ir2O7 have been examined as a function of temperature and applied pressure, with a particular emphasis on regions of the phase diagram where electronic and magnetic phase transitions have been reported. We find no evidence of crystal symmetry change over the range of temperatures (~6 to 300 K) and pressures (~0.1 to 17 GPa) studied. We have also investigated the electronic and magnetic excitations in single crystal samples of Eu2Ir2O7 and Pr2Ir2O7 using high resolution Ir L3-edge RIXS. In spite of very different ground state properties, we find these materials exhibit qualitatively similar excitation spectra, with crystal field excitations at ~3-5 eV, spin-orbit excitations at ~0.5-1 eV, and broad low-lying excitations below ~0.15 eV. In Eu2Ir2O7 we observe highly damped magnetic excitations at ~45 meV, which display significant momentum dependence. We compare these results with recent dynamical structure factor calculations.
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Pyrochlore iridates A2Ir2O7 (A = rare earth elements, Y or Bi) hold great promise for realizing novel electronic and magnetic states owing to the interplay of spin-orbit coupling, electron correlation and geometrical frustration. A prominent example is the formation of all-in/all-out (AIAO)antiferromagnetic order in the Ir4+ sublattice that comprises of corner-sharing tetrahedra. Here we report on an unusual magnetic phenomenon, namely a cooling-field induced shift of magnetic hysteresis loop along magnetization axis, and its possible origin in pyrochlore iridates with non-magnetic Ir defects (e.g. Ir3+). In a simple model, we attribute the magnetic hysteresis loop to the formation of ferromagnetic droplets in the AIAO antiferromagnetic background. The weak ferromagnetism originates from canted antiferromagnetic order of the Ir4+ moments surrounding each non-magnetic Ir defect. The shift of hysteresis loop can be understood quantitatively based on an exchange-bias like effect in which the moments at the shell of the FM droplets are pinned by the AIAO AFM background via mainly the Heisenberg (J) and Dzyaloshinsky-Moriya (D) interactions. The magnetic pinning is stable and robust against the sweeping cycle and sweeping field up to 35 T, which is possibly related to the magnetic octupolar nature of the AIAO order.
Resonant inelastic x-ray scattering (RIXS) is an extremely valuable tool for the study of elementary, including magnetic, excitations in matter. Latest developments of this technique mostly aimed at improving the energy resolution and performing polarization analysis of the scattered radiation, with a great impact on the interpretation and applicability of RIXS. Instead, this article focuses on the sample environment and presents a setup for high-pressure low-temperature RIXS measurements of low-energy excitations. The feasibility of these experiments is proved by probing the magnetic excitations of the bilayer iridate Sr$_3$Ir$_2$O$_7$ at pressures up to 12 GPa.
The study of elementary bosonic excitations is essential toward a complete description of quantum electronic solids. In this context, resonant inelastic X-ray scattering (RIXS) has recently risen to becoming a versatile probe of electronic excitations in strongly correlated electron systems. The nature of the radiation-matter interaction endows RIXS with the ability to resolve the charge, spin and orbital nature of individual excitations. However, this capability has been only marginally explored to date. Here, we demonstrate a systematic method for the extraction of the character of excitations as imprinted in the azimuthal dependence of the RIXS signal. Using this novel approach, we resolve the charge, spin, and orbital nature of elastic scattering, (para-)magnon/bimagnon modes, and higher energy dd excitations in magnetically-ordered and superconducting copper-oxide perovskites (Nd2CuO4 and YBa2Cu3O6.75). Our method derives from a direct application of scattering theory, enabling us to deconstruct the complex scattering tensor as a function of energy loss. In particular, we use the characteristic tensorial nature of each excitation to precisely and reliably disentangle the charge and spin contributions to the low energy RIXS spectrum. This procedure enables to separately track the evolution of spin and charge spectral distributions in cuprates with doping. Our results demonstrate a new capability that can be integrated into the RIXS toolset, and that promises to be widely applicable to materials with intertwined spin, orbital, and charge excitations.
Fully relativistic first-principles electronic structure calculations based on a noncollinear local spin density approximation (LSDA) are performed for pyrochlore iridates Y$_2$Ir$_2$O$_7$ and Pr$_2$Ir$_2$O$_7$. The all-in, all-out antiferromagnetic (AF) order is stablized by the on-site Coulomb repulsion $U>U_c$ in the LSDA+$U$ scheme, with $U_csim1.1$~eV and 1.3~eV for Y$_2$Ir$_2$O$_7$ and Pr$_2$Ir$_2$O$_7$, respectively. AF semimetals with and without Weyl points and then a topologically trivial AF insulator successively appear with further increasing $U$. For $U=1.3$~eV, Y$_2$Ir$_2$O$_7$ is a topologically trivial narrow-gap AF insulator having an ordered local magnetic moment $sim0.5mu_B$/Ir, while Pr$_2$Ir$_2$O$_7$ is barely a paramagnetic semimetal with electron and hole concentrations of $0.016$/Ir, in overall agreements with experiments. With decreasing oxygen position parameter $x$ describing the trigonal compression of IrO$_6$ octahedra, Pr$_2$Ir$_2$O$_7$ is driven through a non-Fermi-liquid semimetal having only an isolated Fermi point of $Gamma_8^+$, showing a quadratic band touching, to a $Z_2$ topological insulator.
We report a resonant inelastic x-ray scattering study of the dispersion relations of charge transfer excitations in insulating La$_2$CuO$_4$. These data reveal two peaks, both of which show two-dimensional characteristics. The lowest energy excitation has a gap energy of $sim 2.2$ eV at the zone center, and a dispersion of $sim 1$ eV. The spectral weight of this mode becomes dramatically smaller around ($pi$, $pi$). The second peak shows a smaller dispersion ($sim 0.5$ eV) with a zone-center energy of $sim 3.9$ eV. We argue that these are both highly dispersive exciton modes damped by the presence of the electron-hole continuum.
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