Relativistic Prolapse-Free Gaussian Basis Sets of Double- and Triple-ζ Quality for s- and p-Block Elements: (aug-)RPF-2Z and (aug-)RPF-3Z

Author(s)

Sousa, Julielson dos Santos ; Gusmao, Eriosvaldo Florentino ; Dias, Anne Kellen de Nazare dos Reis ; Haiduke, Roberto Luiz Andrade

• Document type: Journal article
• Source: JOURNAL OF CHEMICAL THEORY AND COMPUTATION; v. 20, n. 22, p. 8-pg., 2024-11-14.

Abstract

This study presents two new relativistic Gaussian basis sets without variational prolapse of double- and triple-zeta quality, RPF-2Z and RPF-3Z, along with augmented versions including additional diffuse functions, aug-RPF-2Z and aug-RPF-3Z, which are available for all s and p block elements from Hydrogen to Oganesson. The exponents of the Correlation/Polarization (C/P) functions are obtained from a polynomial version of the generator coordinate Dirac-Fock method (p-GCDF). The choice of C/P functions was guided by multireference configuration interaction calculations with single and double excitations (MR-CISD) based on a valence active space. Finally, calculations of fundamental properties done for atomic and molecular systems (bond lengths, vibrational frequencies, dipole moments, and electron affinities) ensure the expected quality of these new basis sets, which may also exhibit some computational efficiency advantages. Additionally, the prolapse-free feature of these sets must provide a reliable description of properties more dependent on core electron distributions, as well. (AU)

• FAPESP's process: 22/05138-0 - Development and augmentation of more compact basis sets free of variational prolapse for relativistic calculations
• Grantee: Roberto Luiz Andrade Haiduke
• Support Opportunities: Regular Research Grants