Chemical disorder driven reentrant spin cluster glass state formation and associated magnetocaloric properties of Nd2Ni0.94Si2.94

Abstract

In this work, we report the synthesis of a new ternary intermetallic compound, Nd₂Ni_0.94Si_2.94, that forms in single phase only in a defect crystal structure. The compound exhibits an antiferromagnetic transition below 7.2 K (T_N) followed by a spin cluster freezing behaviour below 2.85 K (T_f), which makes the compound a reentrant spin cluster glass system. The detailed studies of dc and ac magnetization, heat capacity, non-equilibrium dynamical behaviour, viz., aging effect, temperature and field dependent magnetic relaxation and magnetic memory effect establish the compound to be a cluster-glass material below freezing temperature. The interplay between competing exchange coupling (c/a ≃ 1.04 ⇒ J_NN ≃ J_NNN) and chemical disorder driven variation in the electronic environment among the Nd ions has been argued to be responsible for such a metastable state formation. A considerable value of MCE parameters (−ΔS^max_M ∼ 11.4 J kg⁻¹ K⁻¹, RCP ∼ 160 J kg⁻¹ and ΔT_ad ∼ 5.2 K for a field change of 70 kOe) is obtained for this magnetically frustrated glassy compound.