The Basis Set Truncation Error Revisited: Comparison of Multiwavelet and Gaussian Basis Sets for Computing Properties from First Principles
Bryan Sundahl, Colin Bunner, Emily Gentels, Joel Anderson, Hideo Sekino, Robert J. Harrison · Zenodo (CERN European Organization for Nuclear Research) · 2021
A set of 225 molecules and 5726 reactions are used to examine errors present in linear-combination of atomic orbital (LCAO) calculations using standard atom-centered Gaussian basis sets at the Hartree-Fock and density functional theory levels of theory. We advance beyond previous studies by extending the test set to include heavier atoms, by probing the origin and nature of errors in LCAO calculations including transferability of basis sets between HF and different DFT functionals, by reporting computational times for the multiwavelet calculations and by examining errors in reaction energies, where errors are computed by comparing LCAO results to numerically converged solutions in the MW basis. Calculations in uncontracted basis sets quantify the different errors arising from contraction and incompleteness in the primitive Gaussian basis. Analysis indicates significantly larger errors associated with atoms in the third or lower rows of the periodic table.