In this work, we demonstrate the switching of the magnetization in a thin nickel film deposited on a Cu(110)-(2×1)O surface from out-of-plane to in-plane through the deposition of cobalt (II) phthalocyanine (CoPc) thin layers above 2.7 ML. The evolution of the magnetic properties of the CoPc/Ni system has been monitored by in situ magneto-optical spectroscopy, allowing us to follow not only the magnetic switching in real-time during deposition, but also the evolution of the optical properties of the CoPc as a function of coverage on the ferromagnetic Ni film. The observed magnetic switching is attributed to the modification of the surface magnetic anisotropy of the Ni thin film due to the adsorbed CoPc molecules.

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