First principles characterization of spinterfaces between magnetic Cobaltocene molecule and 2D magnets (CrI$_3$, Fe$_3$GeTe$_2$)

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Main Authors: Machacova, Nikola, Sanyal, Biplab
Format: Preprint
Published: 2026
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author Machacova, Nikola
Sanyal, Biplab
author_facet Machacova, Nikola
Sanyal, Biplab
contents 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 CrI$_3$ and metallic Fe$_3$GeTe$_2$, using first-principles density functional theory based calculations. Our calculated adsorption energies indicate the stability of these hetero-interfaces with the observation of hybridization of electronic states across the interface. Magnetic exchange interaction parameters have been obtained from both total energy differences and the Liechtenstein-Katsnelson-Antropov-Gubanov (LKAG) formalism in the basis of maximally localized Wannier functions (MLWFs). 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 3-fold increase in magnitude compared to the freestanding case. Finally, we observe a 100 % spin polarization at the Fermi level in the cobaltocene/CrI$_3$ interface, which makes it particularly promising for spin-transport applications.
format Preprint
id arxiv_https___arxiv_org_abs_2603_19511
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle First principles characterization of spinterfaces between magnetic Cobaltocene molecule and 2D magnets (CrI$_3$, Fe$_3$GeTe$_2$)
Machacova, Nikola
Sanyal, Biplab
Materials Science
Mesoscale and Nanoscale Physics
Quantum Physics
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 CrI$_3$ and metallic Fe$_3$GeTe$_2$, using first-principles density functional theory based calculations. Our calculated adsorption energies indicate the stability of these hetero-interfaces with the observation of hybridization of electronic states across the interface. Magnetic exchange interaction parameters have been obtained from both total energy differences and the Liechtenstein-Katsnelson-Antropov-Gubanov (LKAG) formalism in the basis of maximally localized Wannier functions (MLWFs). 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 3-fold increase in magnitude compared to the freestanding case. Finally, we observe a 100 % spin polarization at the Fermi level in the cobaltocene/CrI$_3$ interface, which makes it particularly promising for spin-transport applications.
title First principles characterization of spinterfaces between magnetic Cobaltocene molecule and 2D magnets (CrI$_3$, Fe$_3$GeTe$_2$)
topic Materials Science
Mesoscale and Nanoscale Physics
Quantum Physics
url https://arxiv.org/abs/2603.19511