A universal Gaussian basis set is developed for accurate ab initio relativistic Dirac-Fock calculations on atoms and molecules. The Dirac-Fock energies computed by using this single set of the universal Gaussian basis for the atoms, He (Z=2) through No (Z=102), are in excellent agreement with the corresponding numerical finite-difference Dirac-Fock method. The total Dirac-Fock energies for lighter atoms agree with the corresponding numerical limit to a part in ${10}^9$ and for heavier systems to a part in ${10}^8$. The total energy for the heaviest system, No (Z=102), calculated with our universal Gaussian basis set differs from the corresponding numerical limit by only 4 mhartrees.

• Received 28 August 1992

DOI:https://doi.org/10.1103/PhysRevA.47.143