Thermodynamic measurements of Fe-Rh alloys

FeRh undergoes an unusual antiferromagnetic-to-ferromagnetic (AFM-FM) transition just above room temperature (T(AFM>FM)) that can be tuned or even completely suppressed with small changes in composition. The underlying temperature-dependent entropy difference between the competing AFM and FM states that drives this transition is measured by specific heat as a function of temperature from 2 to 380 K on two nearly equiatomic epitaxial Fe-Rh films, one with a ferromagnetic ground state (Fe-rich) and the other with an antiferromagnetic ground state (Rh-rich). The FM state shows an excess heat capacity near 100 K associated with magnetic excitations that are not present in the AFM state. The integrated entropy and enthalpy differences between the two alloys up to T(AFM>FM) agree with the previously measured entropy of the transition (ΔS = 17 ± 3 J/kg/K) and yield a T=0 energy difference of 3.4 J/g, consistent with literature calculations and experimental data; this agreement supports the use of the Fe-rich FM sample as a proxy for the (unstable) FM state of the AFM Rh-rich sample. From the low-temperature specific heat, along with sound velocity and photoemission measurements, the lattice contribution to the difference (ΔS(latt) = -33 ± 9 J/kg/K) and electronic contribution (ΔS(el) = 8 ± 1 J/kg/K) to the difference in entropy are calculated, from which the excess heat capacity in the FM phase and the resulting entropy difference are shown to be dominated by magnetic fluctuations (ΔS(mag) = 43 ± 9 J/kg/K). The excess magnetic heat capacity is dominated by the magnetic heat capacity of the FM phase, which can be fit to a Schottky-like anomaly with an energy splitting of 16 ± 1 meV and a multiplicity of 1 per unit cell.