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Evolution of Magnetic Excitations Across the Metal-Insulator Transition in a Pyrochlore Iridate Eu$_{2}$Ir$_{2}$O$_{7}$

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 Added by Sae Hwan Chun
 Publication date 2018
  fields Physics
and research's language is English




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We report Resonant Inelastic X-ray Scattering (RIXS) study of the magnetic excitation spectrum in a highly insulating Eu$_{2}$Ir$_{2}$O$_{7}$ single crystal that exhibits a metal-insulator transition at $T_{MI}$ = 111(7) K. A propagating magnon mode with 20 meV bandwidth and 28 meV magnon gap is found in the excitation spectrum at 7 K, which is expected in the all-in-all-out (AIAO) magnetically ordered state. This magnetic excitation exhibits substantial softening as temperature is raised towards $T_{MI}$, and turns into highly damped excitation in the paramagnetic phase. Remarkably, the softening occurs throughout the whole Brillouin zone including the zone boundary. This observation is inconsistent with magnon renormalization expected in a local moment system, and indicates that the strength of electron correlation in Eu$_{2}$Ir$_{2}$O$_{7}$ is only moderate, so that electron itinerancy should be taken into account in describing its magnetism.



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In this study, we employ bulk electronic properties characterization and x-ray scattering/spectroscopy techniques to map the structural, magnetic and electronic properties of (Eu$_{1-x}$Ca$_{x}$)$_{2}$Ir$_{2}$O$_{7}$ as a function of Ca-doping. As expected, the metal-insulator transition temperature, $T_{MIT}$, decreases with Ca-doping until a metallic state is realized down to 2 K. In contrast, $T_{AFM}$ becomes decoupled from the MIT and (likely short-range) AFM order persists into the metallic regime. This decoupling is understood as a result of the onset of an electronically phase separated state, the occurrence of which seemingly depends on both synthesis method and rare earth site magnetism. PDF analysis suggests that electronic phase separation occurs without accompanying chemical phase segregation or changes in the short-range crystallographic symmetry while synchrotron x-ray diffraction confirms that there is no change in the long-range crystallographic symmetry. X-ray absorption measurements confirm the $J_{eff}$ = 1/2 character of (Eu$_{1-x}$Ca$_{x}$)$_{2}$Ir$_{2}$O$_{7}$. Surprisingly these measurements also indicate a net electron doping, rather than the expected hole doping, indicating a compensatory mechanism. Lastly, XMCD measurements show a weak Ir magnetic polarization that is largely unaffected by Ca-doping.
We report on the evolution of the thermal metal-insulator transition in polycrystalline samples of Nd$_2$Ir$_2$O$_7$ upon hole-doping via substitution of Ca$^{2+}$ for Nd$^{3+}$. Ca substitution mediates a filling-controlled Mott-like transition with minimal resolvable structural changes and without altering site symmetry. Local structure confirms that Ca substitution does not result in local chemical phase separation, and absorption spectroscopy establishes that Ir cations maintain a spin-orbit entangled electronic configuration. The metal-insulator transition coincides with antiferromagnetic ordering on the Ir sublattice for all measured samples, and both decrease in onset temperature with Ca content. Weak low-temperature upturns in susceptibility and resistivity for samples with high Ca content suggest that Nd sublattice antiferromagnetism continues to couple to carriers in the metallic regime.
We have studied the effect of pressure on the pyrochlore iridate Eu$_2$Ir$_2$O$_7$, which at ambient pressure has a thermally driven insulator to metal transition at $T_{MI}sim120$,K. As a function of pressure the insulating gap closes, apparently continuously, near $P sim 6$,GPa. However, rather than $T_{MI}$ going to zero as expected, the insulating ground state crosses over to a metallic state with a negative temperature coefficient of resistivity, calling into question the true nature of both ground states. The high temperature state also crosses over near 6 GPa, from an incoherent to a conventional metal, suggesting a connection between the high and the low temperature states.
Specific heat, elastic neutron scattering, and muon spin rotation ($mu$SR) experiments have been carried out on a well-characterized sample of stuffed (Pr-rich) Pr$_{2+x}$Ir$_{2-x}$O$_{7-delta}$. Elastic neutron scattering shows the onset of long-range spin-ice 2-in/2-out magnetic order at $T_M = 0.93$ K, with an ordered moment of 1.7(1)$mu_mathrm{B}$/Pr ion at low temperatures. Approximate lower bounds on the correlation length and correlation time in the ordered state are 170 AA and 0.7 ns, respectively. $mu$SR experiments yield an upper bound 2.6(7) mT on the local field $B_mathrm{loc}^{4f}$ at the muon site, which is nearly two orders of magnitude smaller than the expected dipolar field for long-range spin-ice ordering of 1.7$mu_B$ moments (120--270 mT, depending on muon site). This shortfall is due in part to splitting of the non-Kramers crystal-field ground-state doublets of near-neighbor Pr$^{3+}$ ions by the $mu^+$-induced lattice distortion. For this to be the only effect, however, $sim$160 Pr moments out to a distance of $sim$14 AA must be suppressed. An alternative scenario, which is consistent with the observed reduced nuclear hyperfine Schottky anomaly in the specific heat, invokes slow correlated Pr-moment fluctuations in the ordered state that average $B_mathrm{loc}^{4f}$ on the $mu$SR time scale (${sim}10^{-7}$ s), but are static on the time scale of the elastic neutron scattering experiments (${sim}10^{-9}$ s). In this picture the dynamic muon relaxation suggests a Pr$^{3+}$ $4f$ correlation time of a few nanoseconds, which should be observable in a neutron spin echo experiment.
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