Peculiar magnetic states in the double perovskite Nd2NiMnO6

We present magnetic measurements on Nd2NiMnO6 which exhibits a well-known insulating paramagnetic state to an insulating ferromagnetic state transition when cooled below 200 K. Beyond this basic fact, there is a great deal of diversity in the reported magnetic properties and interpretation of specific anomalies observed in the magnetic data of this compound below the Curie temperature. We address specifically two anomalies discussed in the past, namely, a spin-glass like behavior observed in some samples near 100 K and a downturn in the magnetization with a lowering of the temperature below approximately 50 K. We show for the first time that the application of an increasing magnetic field can systematically change the low-temperature behavior to make the down-turn in the magnetization into an upturn. With the help of first principle calculations and extensive simulations along with our experimental observations, we provide a microscopic understanding of all magnetic properties observed in this interesting system to point out that the glassiness around 100 K is absent in well-ordered samples and that the low-temperature magnetic anomaly below 50 K is a consequence of a ferromagnetic coupling of the Nd spin moments with the spin of the Ni-Mn ordered sublattice without giving rise to any ordering of the Nd sublattice that remains paramagnetic, contrary to earlier claims. We explain this counter-intuitive interpretation of a ferromagnetic coupling of Nd spins with Ni-Mn spin giving rise to a decrease in the total magnetic moment by noting the less than half-filled 4f occupation of Nd that ensures orbital and spin moments of Nd to be opposite to each other due to the spin-orbit coupling. Since the ground state total magnetic moment of Nd has a contribution from the orbital moment, that is larger than the spin moment, the total moment of Nd is indeed pointing in a direction opposite to the direction of spin moments of the Ni-Mn sublattice as a consequence of the ferromagn