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Accurate relativistic adapted Gaussian basis sets for hydrogen through xenon without variational prolapse and to be used with both uniform sphere and Gaussian nucleus models

Accurate relativistic adapted Gaussian basis sets (RAGBSs) from H (Z = 1) through Xe (Z = 54) without variational prolapse have been developed by employing a polynomial version of the Generator Coordinate Dirac‐Fock (p‐GCDF) method. Two nuclear models have been used in this work: (1) the finite nucleus of uniform proton‐charge distribution, and (2) the finite nucleus with a Gaussian proton–charge distribution. The largest errors observed are only 1.5 mHartree (silver and cadmium) and the RAGBS sizes are much smaller than previous accurate relativistic Gaussian basis sets that were shown to be free of variational prolapse. © 2005 Wiley Periodicals, Inc. J Comput Chem 27: 61–71, 2006