Correspondence between GTO and STO molecular basis sets

We present a method for the characterization of the distance between two spaces: one generated by a Gaussian basis set, and another by a Slater basis set. The method is an extension of one previously developed for atoms that has been modified to cover molecular problems. The current version enables us to obtain Slater basis sets capable of reproducing the results (multielectronic wave functions and orbitals) obtained with Gaussian basis sets. The interest of this result arises from the fact that we will be able to profit from the effort invested in the optimization of high‐quality Gaussian basis sets. © 2001 John Wiley & Sons, Inc. J Comput Chem 22: 1655–1665, 2001