Magnetic frustration driven by conduction carrier blocking in Nd2Co0.85Si2.88

Abstract

The intermetallic compound ${\mathrm{Nd}}_{2}{\mathrm{Co}}_{0.85}{\mathrm{Si}}_{2.88}$ 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 ${T}_{\mathrm{H}}\ensuremath{\sim}$ 140 K is associated with the development of ferromagnetic interaction between itinerant Co moments, whereas the low-temperature transition at ${T}_{\mathrm{L}}\ensuremath{\sim}$ 6.5 K is due to the coupling among $\text{Nd}\text{\ensuremath{-}}4f$ and $\mathrm{Co}\text{\ensuremath{-}}3d$ moments, which is antiferromagnetic in nature. Detailed studies of temperature-dependent dc magnetic susceptibility, field dependence of isothermal magnetization, nonequilibrium 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 $4f\text{\ensuremath{-}}4f$ 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 ${R}_{2}T{X}_{3}$ ($R$ = 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. The system also exhibits a considerable magnetic entropy change of $\ensuremath{-}\mathrm{\ensuremath{\Delta}}{S}_{\mathrm{M}}\ensuremath{\sim}$ 13.3 J/kg K with a relative cooling power (RCP) of 220 J/kg and adiabatic temperature change $\mathrm{\ensuremath{\Delta}}{T}_{\mathrm{ad}}$ of 6 K for magnetic field change of 70 kOe.