Abstract
We theoretically explore through systematic multiscale ab initio and Monte Carlo calculations how the surface magnetism of a ferromagnetic surface can be fine-tuned by nonmagnetic organic molecules containing a single $\ensuremath{\pi}$ bond. We demonstrate that a magnetic hardening or softening can be induced depending on the electronegativity of the heteroatom or when the $\ensuremath{\pi}$-bond ``bridges'' the magnetic surface atoms. Finally, the Monte Carlo simulations revealed taylored macroscopic hysteresis loops corresponding to soft and hard molecule-surface magnets.
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