Chirality-driven intrinsic spin-glass ordering and field-induced ferromagnetism in Ni3Al nanoparticle aggregates

Weak itinerant-electron ferromagnet Ni3Al is driven to magnetic instability (quantum critical point, QCP, where the long-range ferromagnetic order of the bulk ceases to exist) by reducing the average crystallite size to d=50 nm. 'Zero-field' (H=0) linear and nonlinear ac-susceptibilities, measured on Ni3Al nanoparticle aggregates, with d=50 nm (S1) and d=5 nm (S2), provide strong evidence for two spin glass (SG)-like thermodynamic phase transitions: one at Ti(H=0)≃30K (Ti†(H=0)≃230K) and the other at a lower temperature Tp(H=0)≃8K (Th(H=0)≃52K) in S1 (S2). 'In-field' (H≠0) linear ac-susceptibility and dc magnetization demonstrate that the thermodynamic nature of these transitions is preserved in finite fields. The presently determined H-T phase diagrams for the samples S1 and S2 are compared with those predicted by the Kotliar-Sompolinsky and Gabay-Toulouse mean-field models and Monte Carlo simulations, based on the chirality-driven spin glass (SG) ordering scenario, for a three-dimensional nearest-neighbor Heisenberg SG system with or without weak random anisotropy. Such a detailed comparison permits us to unambiguously identify various 'zero-field' and 'in-field' SG phase transitions as: (i) the simultaneous paramagnetic (PM)-chiral glass (CG) and PM-SG phase transitions at Ti(H), (ii) the PM-CG transition at Ti†(H), (iii) the replica symmetry-breaking SG transition at Tp(H), and (iv) the continuous spin-rotation symmetry-breaking SG transition at Th(H). In the presence of random anisotropy, magnetization fails to saturate even at 90 kOe in S1 whereas negligibly small anisotropy allows even fields as weak as 1 kOe to saturate magnetization and induce ferromagnetism in S2. Due to the proximity to CG/SG-QCP, magnetization and susceptibility both exhibit non-Fermi liquid behavior over a wide range at low temperatures.