Large magnetic cooling power involving frustrated antiferromagnetic spin-glass state inR2NiSi3(R=Gd,Er)

Abstract

The ternary intermetallic compounds ${\mathrm{Gd}}_{2}{\mathrm{NiSi}}_{3}$ and ${\mathrm{Er}}_{2}{\mathrm{NiSi}}_{3}$ are synthesized in chemically single phase, which are characterized using dc magnetization, ac magnetic susceptibility, heat capacity, and neutron diffraction studies. Neutron diffraction and heat capacity studies confirm that long-range magnetic ordering coexists with the frustrated glassy magnetic components for both compounds. The static and dynamical features of dc magnetization and frequency-dependent ac susceptibility data reveal that ${\mathrm{Gd}}_{2}{\mathrm{NiSi}}_{3}$ is a canonical spin-glass system, while ${\mathrm{Er}}_{2}{\mathrm{NiSi}}_{3}$ is a reentrant spin cluster-glass system. The spin freezing temperature merges with the long-range antiferromagnetic ordering temperature at 16.4 K for ${\mathrm{Gd}}_{2}{\mathrm{NiSi}}_{3}$. ${\mathrm{Er}}_{2}{\mathrm{NiSi}}_{3}$ undergoes antiferromagnetic ordering at 5.4 K, which is slightly above the spin freezing temperature at 3 K. The detailed studies of nonequilibrium dynamical behavior, viz., the memory effect and relaxation behavior using different protocols, suggest that both compounds favor the hierarchical model over the droplet model. A large magnetocaloric effect is observed for both compounds. Maximum values of isothermal entropy change $(\ensuremath{-}\mathrm{\ensuremath{\Delta}}{S}_{M})$ and relative cooling power (RCP) are found to be 18.4 J/kg K and 525 J/kg for ${\mathrm{Gd}}_{2}{\mathrm{NiSi}}_{3}$ and 22.6 J/kg K and 540 J/kg for ${\mathrm{Er}}_{2}{\mathrm{NiSi}}_{3}$, respectively, for a change in field from 0 to 70 kOe. The values of RCP are comparable to those of the promising refrigerant materials. A correlation between large RCP and magnetic frustration is discussed for developing new magnetic refrigerant materials.