Characterizing Single-Molecule Magnets using Density Functional Theory*

Single-molecule magnets are valued as prospective components in devices for information processing and storage. Computational modeling can aid in understanding and optimizing their magnetic properties. Many single-molecule magnets are too large for analysis using high-level wavefunction theories, making density functional theory (DFT) an attractive choice.

The magnetic properties of single-molecule magnets depend on a strong exchange interaction between orbitals and the spatial localization of spin orbitals, properties that have been challenging for conventional exchange-correlation functionals. It is therefore crucial to understand the relative effectiveness of DFT methods. Here we apply functionals at the meta-GGA, and local hybrid levels in conjunction with broken symmetry methods to single-molecule magnet systems with exchange-coupled metallic cores. We determine effective coupling parameters and other magnetic properties, and investigate the practical utility of the functionals.