Comparison of two-component REP with all-electron results

The REP and AREP employed for the present calculations are those generated by Christiansen et al. with 7 valence electrons for the halogen atoms, and we optimized basis sets to be of pVTZ quality for the halogen atoms [71]. For the description of the anionic character of the halogen atoms one diffuse basis function is added to each basis set to yield (7s7p3d2f) basis sets contracted to 

For the AtH molecule, the two-component results are in good agreement with the DC results of Visscher et al. [73] at the correlated level of theory. Among the DC results, the aug-pVDZ results are closer to the REP results than the aug-pVTZ results, partially reflecting the basis set quality of the REP calculations. For the (117)H molecule, the REP-KRHF results are in reasonable agreement with the all-electron DHF results of Saue et al. [74]. There are no reports of all-electron correlation calculations for (117)H. Electron correlation effects 

Calculated geometries, harmonic vibrational frequencies and dissociation energies of AtH and (117)H at various levels of theory using REPs and the allelectron DC Hamiltonian. 

DC values for AtH are from Ref. [73], and for (117)H from Ref. [74]. Numbers set in parentheses refer to DC values obtained with an aug-pVDZ 

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