The evolution of ferromagnetic (FM) domains across the temperature-driven antiferromagnetic (AF) to FM phase transition in uncapped and capped epitaxial FeRh thin films was studied by x-ray magnetic circular dichroism and photoemission electron microscopy. The coexistence of the AF and FM phases was evidenced across the broad transition and the different stages of nucleation, growth, and coalescence were directly imaged. The FM phase nucleates into single domain islands and the width of the transition of an individual nucleus is sharper than that of the transition in a macroscopic average.

A spin reorientation accompanying the temperature-induced antiferromagnetic (AFM) to ferromagnetic (FM) phase transition is reported in strained epitaxial FeRh thin films. (57)Fe conversion electron Mössbauer spectrometry showed that the Fe moments have different orientations in FeRh grown on thick single-crystalline MgO and in FeRh grown on ion-beam-assist-deposited (IBAD) MgO. It was also observed, in both samples, that the Fe moments switch orientations at the AFM to FM phase transition. Perpendicular anisotropy was evidenced in the AFM phase of the film grown on IBAD MgO and in the FM phase of that grown on regular MgO. Density-functional theory calculations enabled this spin-reorientation transition to be accurately reproduced for both FeRh films across the AFM-FM phase transition and show that these results are due to differences in strain.

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.