Adsorption of magnetic molecules on surfaces has been studied previously [1-3], but detailed mechanisms of their interaction with magnetic materials are still not properly understood. Such interfaces are particularly relevant for potential spintronic applications, where molecule-substrate coupling could enable new technologies and devices [4].

Using first-principles calculations, we examine the structural, electronic, and magnetic properties of interfaces consisting of the single-molecule magnet bis(cyclopentadienyl)cobalt(II) (cobaltocene) and magnetic two-dimensional materials, semiconducting CrI₃ and metallic Fe₃GeTe₂. Exchange constants were obtained both from total-energy differences and the Liechtenstein–Katsnelson–Antropov–Gubanov (LKAG) formalism utilizing a maximally localized Wannier function (MLWF) basis.

We observe large anisotropy in the exchange interactions, consistent with the hybridization of electronic states across the interface. Additionally, possible exchange mechanisms are proposed based on orbital-resolved exchange and hopping parameters.

These results provide insight into the interplay between magnetism in molecules and 2D materials, and suggest approaches to designing novel interfaces for spin-transport applications.

[1] Li, Y.; et al. Physical Review B 2011, 83, 195443.
[2] Holmberg, R. J.; Murugesu, M. Journal of Materials Chemistry C 2015, 3, 11986–11998.
[3] Campbell, V. E.; et al. Nature Communications 2016, 7, 13646.
[4] Dey, S.; et al. Nano Letters 2025, 25 (26), 10457-10464.