Abstract
Magnetic dopants in ferroelectric oxide host materials provide a platform for electric field control of isolated spins, facilitated by tuning of the magnetocrystalline anisotropy energy (MCAE). We present first-principles calculations of the MCAE experienced by isolated Fe3+ dopants in the tetragonal, orthorhombic, and rhombohedral phases of the prototypical ferroelectric BaTiO3. We identify an order-of-magnitude decrease in the MCAE in the rhombohedral phase relative to the tetragonal and orthorhombic phases. We explain this dramatic decrease, as well as the formation of a spin-easy plane in the tetragonal phase and spin-easy axes in the orthorhombic and rhombohedral phases, using crystal field theory arguments. Building a superposition model from crystal field theory, we show how a set of simple criteria based on crystalline environment can be used to estimate the MCAE. We suggest this as a route to rapidly screen candidate ferroelectric hosts and magnetic dopants that possess phases with spin-easy axes and maximal MCAE tunability.
| Original language | English |
|---|---|
| Article number | 224437 |
| Journal | Physical Review B |
| Volume | 110 |
| Issue number | 22 |
| DOIs | |
| State | Published - Dec 1 2024 |
| Externally published | Yes |
Funding
This research was supported by the National Science Foundation Division of Materials Research under Grant No. DMR-2223486. This work used the Expanse cluster at the San Diego Supercomputer Center through Allocation No. MAT230011 from the Advanced Cyberinfrastructure Coordination Ecosystem: Services & Support (ACCESS) program , which is supported by National Science Foundation Grants No. 2138259, No. 2138286, No. 2138307, No. 2137603, and No. 2138296. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. K.I. acknowledges support from the EPSRC (EP/W028131/1).