Magnetic and transport properties in pyrochlore iridates (Y$_{1-x}$Pr$_x$)$_2$Ir$_2$O$_7$: The role of $f$-$d$ exchange interaction and $d$-$p$ orbital hybridization

Abstract

The $f$-$d$ magnetic exchange interaction is considered to be a key ingredient for many exotic topological phases in pyrochlore iridates. Here, we have investigated the evolution of structural, magnetic and electronic properties in doped pyrochlore iridate, (Y$_{1-x}$Pr$_x$)$_2$Ir$_2$O$_7$. Apart from geometrical frustration, pyrochlore iridates are well known for its active spin-orbit coupling effect. The substitution of Pr$^{3+}$ (4$f^2$) for the nonmagnetic Y$^{3+}$ (4$d^0$) acts as a magnetic doping, which provides an ideal platform to study $f$-$d$ exchange interaction without altering the Ir-sublattice. With Pr substitution, system retains its original cubic structural symmetry but the local structural parameters show an evolution with the doping concentration $x$. The robust magnetic-insulating state in Y$_2$Ir$_2$O$_7$ is drastically weakened, while Pr$_2$Ir$_2$O$_7$ ($x$ = 1.0) shows a paramagnetic-metallic behavior. A metal-insulator transition is observed for $x$ = 0.8 sample. This evolution of magnetic and electronic properties are believed to be induced by an exchange interaction between localized Pr-4$f$ and itinerant Ir-5$d$ electrons as well as by an increased hybridization between Ir-$t_{2g}$ and (basal) O-$p$ orbitals as observed in XAS study. The resistivity in insulating materials follows a power-law behavior with a decreasing exponent with $x$. A negative magnetoresistance is observed for present series of samples at low temperature and where the magnetoresistance shows a quadratic field dependence at higher fields.