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) i
s 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.
Interest in many strongly spin-orbit coupled 5d-transition metal oxide insulators stems from mapping their electronic structures to a J=1/2 Mott phase. One of the hopes is to establish their Mott parent states and explore these systems potential of r
ealizing novel electronic states upon carrier doping. However, once doped, little is understood regarding the role of their reduced Coulomb interaction U relative to their strongly correlated 3d-electron cousins. Here we show that, upon hole-doping a candidate J=1/2 Mott insulator, carriers remain localized within a nanoscale phase separated ground state. A percolative metal-insulator transition occurs with interplay between localized and itinerant regions, stabilizing an antiferromagnetic metallic phase beyond the critical region. Our results demonstrate a surprising parallel between doped 5d- and 3d-electron Mott systems and suggest either through the near degeneracy of nearby electronic phases or direct carrier localization that U is essential to the carrier response of this doped spin-orbit Mott insulator.
We present magnetization and Hall effect measurements on the pyrochlore iridate Nd2Ir2O7. Previous muon spin rotation measurements have shown that the system undergoes an unusual transition at T$_M$ = 110 K into a magnetic phase lacking long-range or
der, followed by a transition at T$_LRO$ = 6 K into a state with long-range magnetic order. We observe a small remnant magnetization when cycling through zero magnetic field at temperatures below T$_M$. Below T$_LRO$, this remnant magnetization increases sharply, and new hysteresis effects appear at a higher field B$_c$ = 2.5 T, while the Hall resistance develops a non-monotonic and hysteretic magnetic field dependence, with a maximum at B$_c$ and signatures of an anomalous Hall effect. The dependence on field sweep direction demonstrates a non-trivial transition into a magnetically ordered state with properties paralleling those of known spin-ice systems and suggests a spin reorientation transition across the metal insulator transition in the A-227 series.
Neutron diffraction measurements are presented exploring the magnetic and structural phase behaviors of the candidate J$_{eff}=1/2$ Mott insulating iridate Sr$_2$IrO$_4$. Comparisons are drawn between the correlated magnetism in this single layer sys
tem and its bilayer analog Sr$_3$Ir$_2$O$_7$ where both materials exhibit magnetic domains originating from crystallographic twinning and comparable moment sizes. Weakly temperature dependent superlattice peaks violating the reported tetragonal space group of Sr$_2$IrO$_4$ are observed supporting the notion of a lower structural symmetry arising from a high temperature lattice distortion, and we use this to argue that moments orient along a unique in-plane axis demonstrating an orthorhombic symmetry in the resulting spin structure. Our results demonstrate that the correlated spin order and structural phase behaviors in both single and bilayer Sr$_{n+1}$Ir$_{n}$O$_{3n+1}$ systems are remarkably similar and suggest comparable correlation strengths in each system.
Through a neutron scattering, charge transport, and magnetization study, the correlated ground state in the bilayer iridium oxide Sr$_3$Ir$_2$O$_7$ is explored. Our combined results resolve scattering consistent with a high temperature magnetic phase
that persists above 600 K, reorients at the previously defined $T_{AF}=280$ K, and coexists with an electronic ground state whose phase behavior suggests the formation of a fluctuating charge or orbital phase that freezes below $T^{*}approx70$ K. Our study provides a window into the emergence of multiple electronic order parameters near the boundary of the metal to insulator phase transition of the 5d $J_{eff}=1/2$ Mott phase.
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.
We report a combined muon spin relaxation/rotation, bulk magnetization, neutron scattering, and transport study of the electronic properties of the pyrochlore iridate Nd2Ir2O7. We observe the onset of strongly hysteretic behavior in the temperature d
ependent magnetization below 120 K, and an abrupt increase in the temperature dependent resistivity below 8 K. Zero field muon spin relaxation measurements show that the hysteretic magnetization is driven by a transition to a magnetically disordered state, and that below 8 K a complex magnetically ordered ground state sets in, as evidenced by the onset of heavily damped spontaneous muon precession. Our measurements point toward the absence of a true metal-to-insulator phase transition in this material and suggest that Nd2Ir2O7 lies either within or on the metallic side of the boundary of the Dirac semimetal regime within its topological phase diagram.
We demonstrate that magnetic phase separation and competing spin order in the colossal magnetoresistive (CMR) manganites can be directly explored via tuning strain in bulk samples of nanocrystalline La$_{1-x}$Ca$_x$MnO$_3$. Our results show that stra
in can be reversibly frozen into the lattice in order to stabilize coexisting antiferromagnetic domains within the nominally ferromagnetic metallic state of La$_{5/8}$Ca$_{3/8}$MnO$_3$. The measurement of tunable phase separation via magnetic neutron powder diffraction presents a direct route of exploring the correlated spin properties of phase separated charge/magnetic order in highly strained CMR materials and opens a potential avenue for realizing intergrain spin tunnel junction networks with enhanced CMR behavior in a chemically homogeneous material.
