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Effect of carrier concentration on magnetism and magnetic order in the pyrochlore iridates

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 Added by Michael J. Graf
 Publication date 2014
  fields Physics
and research's language is English




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We present resistivity, magnetization, and zero field muon spin relaxation ($mu$SR) data for the pyrochlore iridate materials Nd$_{2-x}$Ca$_{x}$Ir$_{2}$O$_{7}$ ($x = 0, 0.06$, and $0.10$) and Sm$_2$Ir$_2$O$_7$. While Nd$_{2}$Ir$_{2}$O$_{7}$ (Nd227) is weakly conducting, Sm$_{2}$Ir$_{2}$O$_{7}$ (Sm227) has slowly diverging resistivity at low temperature. Nd227 and Sm227 exhibit magnetic anomalies at $T_{M} = 105 K$ and $137 K$, respectively. However, zero-field $mu$SR measurements show that long-range magnetic order of the Ir$^{4+}$ sublattice sets in at much lower temperatures ($T_{LRO} sim 8 K$ for Nd227 and $70 K$ for Sm227); both materials show heavily damped muon precession with a characteristic frequency near 9 MHz. The magnetic anomaly at $T_{M}$ in Nd227 is not significantly affected by the introduction of hole carriers by Ca-substitution in the conducting Nd$_{2-x}$Ca$_{x}$Ir$_{2}$O$_{7}$ samples, but the muon precession is fully suppressed for both.



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We present results from muon spin relaxation/rotation, magnetization, neutron scattering and transport measurements on polycrystalline samples of the pyrochlore iridates Y2Ir2O7 (Y-227) and Yb2Ir2O7 (Yb-227). Well-defined spontaneous oscillations of the muon asymmetry are observed together with hysteretic behavior in magnetization below 130 K in Yb-227, indicative of commensurate long-range magnetic order. Similar oscillations are observed in Y-227 below 150 K; however the onset of hysteretic magnetization at T = 190 K indicates a transition to an intermediate state lacking long-range order as observed in Nd-227. Our results also show that insulating members of the iridate family have nearly identical magnetic ground states, and that the presence of magnetic A-site species does not play any significant role in altering the ground state properties.
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.
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 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.
Nonequilibrium many-body dynamics is becoming one of the central topics of modern condensed matter physics. Floquet topological states were suggested to emerge in photodressed band structures in the presence of periodic laser driving. Here we propose a viable nonequilibrium route without requiring coherent Floquet states to reach the elusive magnetic Weyl semimetallic phase in pyrochlore iridates by ultrafast modification of the effective electron-electron interaction with short laser pulses. Combining textit{ab initio} calculations for a time-dependent self-consistent reduced Hubbard $U$ controlled by laser intensity and nonequilibrium magnetism simulations for quantum quenches, we find dynamically modified magnetic order giving rise to transiently emerging Weyl cones that are probed by time- and angle-resolved photoemission spectroscopy. Our work offers a unique and realistic pathway for nonequilibrium materials engineering beyond Floquet physics to create and sustain Weyl semimetals. This may lead to ultrafast, tens-of-femtoseconds switching protocols for light-engineered Berry curvature in combination with ultrafast magnetism.
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