Determination of the tricritical point, H-T phase diagram and exchange interactions in the antiferromagnet MnTa2O6

Abstract

Using the analysis of the temperature and magnetic field dependence of the magnetization (M) measured in the temperature range of 1.5 K to 400 K in magnetic fields up to 250 kOe, the magnetic field-temperature (H–T) phase diagram, tricritical point and exchange constants of the antiferromagnetic MnTa2O6 are determined in this work. X-ray diffraction/Rietveld refinement and x-ray photoelectron spectroscopy of the polycrystalline MnTa2O6 sample verified its phase purity. Temperature dependence of the magnetic susceptibility χ (=M/H) yields the Néel temperature TN = 5.97 K determined from the peak in the computed ∂(χT)/∂T vs T plot, in agreement with the TN = 6.00 K determined from the peak in the CP vs T data. The experimental data of CP vs T near TN is fitted to CP = A|T − TN|−α yielding the critical exponent α = 0.10(0.13) for T > TN (T < TN). The χ vs T data for T > 25 K fits well with the modified Curie–Weiss law: χ = χ0 + C/(T − θ) with χ0 = −2.12 × 10−4 emu mol−1 Oe−1 yielding θ = −24 K, and C = 4.44 emu K mol−1 Oe−1, the later giving magnetic moment μ = 5.96 μB per Mn2+ ion. This yields the effective spin S = 5/2 and g = 2.015 for Mn2+, in agreement with g = 2.0155 measured using electron spin resonance spectroscopy. Using the magnitudes of θ and TN and molecular field theory, the antiferromagnetic exchange constants J0/kB = −1.5 ± 0.2 K and J⊥/kB = −0.85 ± 0.05 K for Mn2+ ions along the chain c-axis and perpendicular to the c-axis respectively are determined. The χ vs T data when compared to the prediction of a Heisenberg linear chain model provides semiquantitative agreement with the observed variation. The H–T phase diagram is mapped using the M–H isotherms and M–T data at different H yielding the tricritical point TTP (H, T) = (17.0 kOe, 5.69 K) separating the paramagnetic, antiferromagnetic, and spin-flop phases. At 1.5 K, the experimental magnitudes of the exchange field HE = 206.4 kOe and spin-flop field HSF = 23.5 kOe yield the anisotropy field HA = 1.34 kOe. These results for MnTa2O6 are compared with those reported recently in the isostructural MnNb2O6.