We extend our ab initio molecular dynamics methods to more exact wave functions, including complete active space multiconfiguration self-consistent-field (CASSCF) and full configuration interaction (full CI) wave functions. These extensions are critical for describing properly the dynamics of bond formation/dissociation and isomerization, as we illustrate here by examining the bond dissociation/formation of Na-2 and the isomerization ("pseudorotation") of Na-3 with full CI dynamics. Equivalencing of all three atoms of Na-3 is found to proceed first via facile inversions through linear structures, which occur more often than conventional pseudorotation (via obtuse to acute to obtuse isosceles triangles).