Abstract
Magneto-Raman spectroscopy has been used to study spin-phonon coupling in two-dimensional (2D) magnets. Raman spectra of CrI3 show a strong dependence on the magnetic order within a layer and between the layers. Here we carry out the first systematic theoretical investigation of the magneto-Raman effect in 2D magnets by performing density functional theory calculations and developing a generalized polarizability model. Our first-principles simulations well reproduce experimental Raman spectra of CrI3 with different magnetic states. The model reveals how the change of spin orientation in each layer is coupled to the layer’s vibration to induce or eliminate the spin-dependent anti-symmetric off-diagonal terms in the Raman tensor for altering the selection rules. We also uncover that the correlation between phonon modes and magnetic orders is a universal phenomenon, which should exist in other phonon modes and 2D magnets. Our predictive simulations and modeling are expected to guide the research in 2D magnets.
| Original language | English |
|---|---|
| Article number | 82 |
| Journal | npj 2D Materials and Applications |
| Volume | 8 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 2024 |
Funding
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 resources from 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 resources from 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. Notice: This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and 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 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 ).