In materials where two or more ordering degrees of freedom are closely matched in their free energies, coupling between them, or multiferroic behavior can occur. These phenomena can produce a very rich phase behavior, as well as emergent phases that offer useful properties and opportunities to reveal novel phenomena in phase transitions. The ordered alloy FeRh undergoes an antiferromagnetic to ferromagnetic phase transition at ~375 K, which illustrates the interplay between structural and magnetic order mediated by a delicate energy balance between two configurations. We have examined this transition using a combination of high-resolution x-ray structural and magnetic imaging and comprehensive x-ray magnetic circular dichroism spectroscopy. We find that the transition proceeds via a defect-driven domain nucleation and growth mechanism, with significant return point memory in both the structural and magnetic domain configurations. The domains show evidence of inhibited growth after nucleation, resulting in a quasi-2 nd order temperature behavior.Magneto-structural phase transitions offer new ways of accessing multiferroic properties, as well as a probe of the relationships between structure, magnetic and electronic ordering 1 . The phenomenology of these coupled transitions is immensely varied, as they may arise in any condensed matter system where structural, magnetic and electronic energies are closely matched. This can result in large changes of electronic/magnetic order with very subtle structural transitions. Often, materials that display such multiferroic behaviors have complex crystalline structures, with multiple avenues for distortions and symmetry changes that may result in electronic property modifications. While these materials offer much promise for discovery of new phases and applications, systems that exhibit coupled transitions with a relatively simple structural change may enable better control of the transition as well as the opportunity to study the physics of the coupling.The CsCl-structured alloy FeRh experiences a first-order structural phase transition above room temperature characterized by a ~1% isotropic volume expansion coupled with a magnetic transition from a low-temperature antiferromagnetic (AFM) phase to a high-temperature ferromagnetic (FM) phase [2][3][4][5][6][7][8][9][10] . During the magnetic transition, the Fe sublattice switches from antiparallel to parallel exchange, while the Rh develops a magnetic moment of approximately 0.9 µ B 11-14 . The transition temperature can be tuned easily by an applied magnetic field, with a reported effect of −9 K/T 15,16 . In addition, other external stimuli, such as piezoelectric strain has been found to influence the magnetization of the FM phase 9 as well as the magnetocaloric properties 17 near the transition. In epitaxial films, the isotropic expansion is modified by substrate clamping to become an out-of-plane tetragonal distortion 18 . The transition temperature may vary in films with thickness and substrate mismatch playing a role, ho...