Unraveling the Nature of Magnetism of the 5d

ABSTRACT

We report electron spin resonance (ESR) spectroscopy results on the double perovskite Ba_{2}YIrO_{6}. On general grounds, this material is expected to be nonmagnetic due to the strong coupling of the spin and orbital momenta of Ir^{5+} (5d^{4}) ions. However, controversial experimental reports on either strong antiferromagnetism with static order at low temperatures or just a weakly paramagnetic behavior have triggered a discussion on the breakdown of the generally accepted scenario of the strongly spin-orbit coupled ground states in the 5d^{4} iridates and the emergence of a novel exotic magnetic state. Our data evidence that the magnetism of the studied material is solely due to a few percent of Ir^{4+} and Ir^{6+} magnetic defects while the regular Ir^{5+} sites remain nonmagnetic. Remarkably, the defect Ir^{6+} species manifest magnetic correlations in the ESR spectra at T≲20 K, suggesting a long-range character of superexchange in the double perovskites as proposed by recent theories.