Magnetic frustration driven by conduction carrier blocking in Nd${}_2$Co${}_{0.85}$Si${}_{2.88}$

Abstract

The intermetallic compound Nd${}_2$Co${}_{0.85}$Si${}_{2.88}$ having a triangular lattice could be synthesized in single-phase only with defect crystal structure. Investigation through different experimental techniques indicate the presence of two magnetic transitions in the system. As verified experimentally and theoretically, the high-temperature transition T${}_H$ ~ 140 K is associated with the development of ferromagnetic interaction between itinerant Co moments, whereas the low-temperature transition at T${}_L$ ~ 6.5 K is due to the coupling among Nd-4f and Co-3d moments, which is antiferromagnetic in nature. Detailed studies of temperature-dependent dc magnetic susceptibility, field dependence of isothermal magnetization, non-equilibrium dynamical behavior, viz. magnetic relaxation, aging effect, magnetic-memory effect, and temperature dependence of heat capacity, along with density functional theory (DFT) calculations, suggest that the ground state is magnetically frustrated spin-glass in nature, having competing magnetic interactions of equivalent energies. DFT results further reveal that the 3d/5d-conduction carriers are blocked in the system and act as a barrier for the 4f-4f RKKY interactions, resulting in spin-frustration. Presence of vacancy defects in the crystal are also conducive to the spin-frustration. This is an unique mechanism of magnetic frustration, not emphasized so far in any of the ternary R${}_2$TX${}_3$ (R=rare-earth, T=transition elements and X=Si, Ge, In) type compounds. Due to the competing character of the itinerant 3d and localized 4f moments, the compound exhibits anomalous field dependence of magnetic coercivity.

16 pages, 15 figures

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