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First-principles characterization of spin interfaces between magnetic cobaltocene molecule and the two-dimensional magnets CrI3 and Fe3GeTe2

Nikola Machacova1,2 and Biplab Sanyal1,*

  • 1Department of Physics and Astronomy, Uppsala University, Box 516, 751 20 Uppsala, Sweden
  • 2Department of Condensed Matter Physics, Charles University, 121 16 Prague, Czech Republic

  • *Contact author: Biplab.Sanyal@physics.uu.se
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Phys. Rev. B 114, 115410 – Published 18 August, 2026

DOI: https://doi.org/10.1103/zdyd-f51r

Abstract

In this paper, we examine the properties of spin-polarized interfaces consisting of single-molecule magnet bis(cyclopentadienyl)cobalt(II) (cobaltocene) and two-dimensional magnetic materials, semiconducting CrI3 and metallic Fe3GeTe2, using first-principles density functional theory based calculations. Our calculated adsorption energies indicate the stability of these heterointerfaces with the observation of hybridization of electronic states across the interface. Magnetic properties are characterized using Heisenberg exchange parameters obtained from both total-energy differences and the Liechtenstein-Katsnelson-Antropov-Gubanov formalism in the basis of maximally localized Wannier functions. Analysis of these parameters shows a strong directional anisotropy in the magnetic substrate-molecule interaction in agreement with the nature of orbital hybridization. Additionally, possible exchange mechanisms are proposed based on orbital-resolved exchange and hopping parameters. We also show that the molecular adsorption may enhance the intralayer exchange interactions, with some exchange parameters reaching up to a threefold increase in magnitude compared to the freestanding case. Finally, we observe a 100% spin polarization at the Fermi level in the cobaltocene/CrI3 interface, which makes it particularly promising for spin-transport applications.

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Outline

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Phys. Rev. B 114, 115410– Published 18 August, 2026
  • Received 30 January 2026
  • Revised 15 June 2026
  • Accepted 13 July 2026
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. Funded by Bibsam.

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