Abstract
CrI3, a hot two-dimensional (2D) magnet, exhibits complex magnetism depending on the number of layers and interlayer stacking patterns. For bilayer CrI3, the interlayer magnetism can be tuned between ferromagnetic (FM) and antiferromagnetic (AFM) order by manipulating the stacking order. However, the stacking is mostly modified through translation between the layers, while the effect of rotation between the layers on the interlayer magnetic order has not yet been fully investigated. Here, we considered three energetically stable stacking patterns R3, C2/m and AA in bilayer CrI3, and their reversed counterparts R3-r, C2/m-r and AA-r through rotating one layer by 180° with respect to the other layer. Our first-principles calculations suggest that the interlayer magnetic ground state can be switched from AFM to FM (or FM to AFM) by reversing the stacking pattern. A detailed microscopic analysis was carried out by magnetic force theory calculations on C2/m stacking which favors AFM and C2/m-r stacking which favors FM. The interlayer magnetic interactions and the origin of the magnetic order change were revealed through specific orbital analysis. Our work demonstrates that stacking rotation can also tune the interlayer magnetism of CrI3 and provides insight into its interlayer magnetic properties at the microscopic level.
| Original language | English |
|---|---|
| Pages (from-to) | 16172-16181 |
| Number of pages | 10 |
| Journal | Nanoscale |
| Volume | 13 |
| Issue number | 38 |
| DOIs | |
| State | Published - Oct 14 2021 |
Funding
Part of this research was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. X. K. and L. L. used the resources of the Compute and Data Environment for Science (CADES) at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC05-00OR22725. The authors also used the resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. DOE under Contract No. DE-AC02-05CH11231. H. K. Yoon and M. J. Han were supported by the Creative Materials Discovery Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT and Korea Government (MIST) (No. 2018M3D1A1058754 and 2021R1A2C1009303) and the KAIST Grand Challenge 30 Project (KC30) funded by the Ministry of Science and ICT and KAIST, Korea (No. 1711100606/N11190153). Notice: This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or to allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).
| Funders | Funder number |
|---|---|
| CADES | |
| Data Environment for Science | |
| U.S. Department of Energy | DE-AC05-00OR22725, DE-AC02-05CH11231 |
| Office of Science | |
| Ministry of Science, ICT and Future Planning | 2021R1A2C1009303, 2018M3D1A1058754 |
| National Research Foundation of Korea | |
| Korea Advanced Institute of Science and Technology | 1711100606/N11190153 |