Routine <i>ab initio</i> modeling of heavy-element chemistry with strong relativistic effects remains insufficiently available to a wide community of chemists. On top of theoretical complexity and high demands for computational resources, heavy-element computational chemistry suffers from underdeveloped infrastructure. In particular, there are gaps in standard basis sets and reliable exchange-correlation functionals for relativistic DFT calculations. We develop flexible and compact basis sets for actinides and heaviest main-group elements using a diverse group of chemical species, including atoms, ions, and molecules, within the framework of a robust particle swarm optimization algorithm. In addition, we explore the extension of common exchange-correlation functionals, primarily based on the PBE approximation, to account for electronic correlations in the presence of relativistic effects, both scalar and spin-orbit.

New infrastructure for routine relativistic quantum-chemical calculations: Basis sets and exchange-correlation functionals for actinides and heaviest main-group elements

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