Reentrant canonical spin-glass dynamics and tunable field-induced transitions in (GeMn)Co2O4 Kagomé lattice

Abstract

We report on the reentrant canonical semi spin-glass characteristics and controllable field-induced transitions in distorted Kagomé symmetry of (GeMn)Co2O4. This B-site spinel exhibits complicated, yet interesting magnetic behaviour in which the longitudinal ferrimagnetic (FiM) order sets in below the Néel temperature T FN ∼ 77 K due to uneven moments of divalent Co (↑ 5.33 μ B) and tetravalent Mn (↓ 3.87 μ B) which coexists with transverse spin-glass state below 72.85 K. Such complicated magnetic behaviour is suggested to result from the competing anisotropic superexchange interactions (J AB/k B ∼ 4.3 K, J AA/k B ∼ −6.2 K and J BB/k B ∼ −3.3 K) between the cations, which is extracted following the Néel’s expression for the two-sublattice model of FiM. Dynamical susceptibility (χ ac (f, T)) and relaxation of thermoremanent magnetization, M TRM (t) data have been analysed by means of the empirical scaling-laws such as Vogel–Fulcher law and Power law of critical slowing down. Both of which reveal the reentrant spin-glass like character which evolves through a number of intermediate metastable states. The magnitude of Mydosh parameter (Ω ∼ 0.002), critical exponent zυ = (6.7 ± 0.07), spin relaxation time τ 0 = (2.33 ± 0.1) × 10−18 s, activation energy E a/k B = (69.8 ± 0.95) K and interparticle interaction strength (T 0 = 71.6 K) provide the experimental evidences for canonical spin-glass state below the spin freezing temperature T F = 72.85 K. The field dependence of T F obtained from χ ac (T) follows the irreversibility in terms of de Almeida–Thouless mean-field instability in which the magnitude of crossover scaling exponent Φ turns out to be ∼2.9 for the (Ge0.8Mn0.2)Co2O4. Isothermal magnetization plots reveal two field-induced transitions across 9.52 kOe (H SF1) and 45.6 kOe (H SF2) associated with the FiM domains and spin-flip transition, respectively. Analysis of the inverse paramagnetic susceptibility after subtracting the temperature independent diamagnetic term (=−3 × 10−3 emu mol−1 Oe−1) results in the effective magnetic moment = 7.654 μ B/f.u. This agrees well with the theoretically obtained = 7.58 μ B/f.u. resulting the cation distribution in support of the Hund’s ground state spin configuration and of Mn4+ and Co2+, respectively. The H–T phase diagram has been established by analysing all the parameters (T F(H), T FN(H), H SF1(T) and H SF2(T)) extracted from various magnetization measurements. This diagram enables clear differentiation among the different phases of the (GeMn)Co2O4 and also illustrates the demarcation between short-range and long-range ordered regions.