Reproducible workflows for verification and optimization of solid-state pseudopotentials*

The quality of pseudopotentials (PPs), a key approximation for planewaves implementations of density-functional-theory (DFT), is crucial in obtaining trustworthy predictions of material properties. Nevertheless, verifying PPs is not trivial: it requires significant expertise in running DFT simulations and can involve hundreds of DFT runs. Optimization is even harder: every iteration requires this verification step, further increasing the number of calculations needed. We address this issue by developing a toolkit based on the AiiDA [1] workflow engine and the AiiDAlab [2] interface to automate and streamline the verification and optimization of PPs. Using the toolkit, two curated PP libraries tagged with “efficiency” and “precision” are improved, further extending the SSSP library [3]: “efficiency” is targeted at high-throughput screening, and “precision” at high-accuracy modeling. This effort has been facilitated by the development of AiiDA SSSP workflows that ensure full reproducibility. The toolkit is user-friendly and can be used to verify and optimize PPs for more specific usages, e.g., core-hole PPs needed in XPS simulations.

[1] S. P. Huber et al., Sci. Data 7, 300 (2020).

[2] A. V. Yakutovich et al., Comput. Mater. Sci. 188, 110165 (2021).

[3] G. Prandini et al., npj Comput. Mater. 4, 72 (2018).