Collapse of the standard ferromagnetic domain structure in hybrid Co/Molecule bilayers

The interplay between Hund’s coupling, exchange interaction and magnetic anisotropy is responsible for a multitude of magnetic phases, ranging from conventional ferromagnetism to exotic spin textures. Yet, engineering and fine-tuning a magnetic state remains a major challenge in modern magnetism. We show that the chemisorption of organic molecules over Co thin films offers a tool to transform the films from ferromagnetic to a glassy-type state. This emerges when the correlation length of the random anisotropy field, induced by the π-d molecule/metal hybridization, is comparable to the characteristic exchange length. Such a state is characterized by the collapse of the standard domain structure and the emergence of blurred pseudo-domains intertwined by diffuse and irregular domain walls. The magnetization reversal then involves topological vortex-like structures, which are here predicted and successfully measured by magnetic-force microscopy. At the macroscopic level this new glassy-type state is defined by a giant magnetic hardening and the violation of the magnetization-reversal Rayleigh law. Our work thus shows that the electronic interaction of a standard thin-film magnet with readily available molecules can generate structures with remarkable new magnetic properties, and thus opens a new avenue for the design of tailored-on-demand magnetic composites.