Generating and grading 34 Optimized Norm-Conserving Vanderbilt Pseudopotentials for Actinides and Super Heavy Elements in the PseudoDojo

TL;DR

This paper introduces a comprehensive set of optimized norm-conserving Vanderbilt pseudopotentials for 34 actinides and super-heavy elements, validated through first-principles calculations to aid material discovery involving heavy elements.

Contribution

It presents the first systematic development and validation of pseudopotentials for actinides and super-heavy elements across multiple exchange-correlation functionals, enhancing computational modeling capabilities.

Findings

Validated pseudopotentials with -Gauge and -Gauge indicators.

Compared equations of state with all-electron ZORA calculations, showing good agreement.

Pseudopotentials are publicly available for use in various computational packages.

Abstract

In the last decades, material discovery has been a very active research field driven by the need to find new materials for many different applications. This has also included materials with heavy elements, beyond the stable isotopes of lead, as most actinides exhibit unique properties that make them useful in various applications. Furthermore, new heavy elements beyond actinides, collectively referred to as super-heavy elements (SHEs), have been synthesized, filling previously empty space of Mendeleev periodic table. Their chemical bonding behavior, of academic interest at present, would also benefit of state-of-the-art modeling approaches. In particular, in order to perform first-principles calculations with planewave basis sets, one needs corresponding pseudopotentials. In this work, we present a series of scalar- and fully-relativistic optimized norm-conserving Vanderbilt pseudopotentials (ONCVPs) for thirty-four actinides and super-heavy elements, for three different exchange-correlation functionals (PBE, PBEsol and LDA). The scalar-relativistic version of these ONCVPs is tested by comparing equations of states for crystals, obtained with \textsc{abinit} 9.6, with those obtained by all-electron zeroth-order regular approximation (ZORA) calculations, without spin-orbit coupling, performed with the Amsterdam Modeling Suite \textsc{band} code. $\Delta$-Gauge and $\Delta_1$-Gauge indicators are used to validate these pseudopotentials. This work is a contribution to the PseudoDojo project, in which pseudopotentials for the whole periodic table are developed and systematically tested. The pseudopotential files are available on the PseudoDojo web-interface pseudo-dojo.org in psp8 and UPF2 formats, both suitable for \textsc{abinit}, the latter being also suitable for Quantum ESPRESSO.