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Magnetic exchange interactions in monolayer CrI₃ from many-body wavefunction calculations

Michele Pizzochero1,2*, Ravi Yadav1,2*, Oleg V. Yazyev1,2*

1 Institute of Physics, Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

2 National Centre for Computational Design and Discovery of Novel Materials (MARVEL), Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

* Corresponding authors emails: michele.pizzochero@epfl.ch, ravi.yadav@epfl.ch, oleg.yazyev@epfl.ch
DOI10.24435/materialscloud:2j-jz [version v1]

Publication date: Jan 19, 2021

How to cite this record

Michele Pizzochero, Ravi Yadav, Oleg V. Yazyev, Magnetic exchange interactions in monolayer CrI₃ from many-body wavefunction calculations, Materials Cloud Archive 2021.10 (2021), https://doi.org/10.24435/materialscloud:2j-jz


The marked interplay between the crystalline, electronic, and magnetic structure of atomically thin magnets has been regarded as the key feature for designing next-generation magneto-optoelectronic devices. In this respect, a detailed understanding of the microscopic interactions underlying the magnetic response of these crystals is of primary importance. Here, we combine model Hamiltonians with multireference configuration interaction wavefunctions to accurately determine the strength of the spin couplings in the prototypical single-layer magnet CrI₃. Our calculations identify the (ferromagnetic) Heisenberg exchange interaction J = −1.44 meV as the dominant term, being the inter-site magnetic anisotropies substantially weaker. We also find that single-layer CrI₃ features an out-of-plane easy axis ensuing from a single-ion anisotropy A = −0.10 meV, and predict g-tensor in-plane components gxx = gyy = 1.90 and out-of-plane component gzz  = 1.92. In addition, we assess the performance of a dozen widely used density functionals against our accurate correlated wavefunctions calculations and available experimental data, thereby establishing reference results for future first-principles investigations. Overall, our findings offer a firm theoretical ground to recent experimental observations.

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39.7 MiB The .zip folder contains DFT and QC input and output files along with the processed output data published in 2D Mater. 7, 035005 (2020). The .zip folder also contains a README text file describing content of each file and folder.


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quantum magnetism 2D materials quantum chemistry calculations density functional calculations CrI3 SNSF MARVEL CSCS

Version history:

2021.10 (version v1) [This version] Jan 19, 2021 DOI10.24435/materialscloud:2j-jz