LFDFT—A Practical Tool for Coordination Chemistry

Round 1

Reviewer 1 Report

In this paper, the Ligand-Field Density-Functional Theory (LFDFT) method is tested for its applicability by describing it using practical examples. The usefulness of the method is verified by comparing molecular structure and spectroscopic data with calculated results. While we believe that the assertions regarding the usefulness of this method are appropriate, we would like to see more explanation regarding the discussion of inconsistencies. Experimentally, the only way to change the electronic state of Eu and Ce is to change to the ligand. In this regard, it would be better to show how the difference in energy of this calculation corresponds to the difference to the molecular structure, even if it is just a guess.

Note that there are numerous typos in this paper, and we recommend that the paper be proofread in English.

Author Response

Please see the attachment.

Author Response File: Author Response.pdf

Reviewer 2 Report

The work deals with the study of the spectra of complexes of some lanthanides (Eu and Ce) using routine techniques recognized for this purpose. It has been carried out in an elegant and comprehensive way and presents an exhaustive bibliography.

In my opinion, it is publishable in Computation in the present form.

I have few comments that should be considered before publication:

1) in the comparison of the computed transition energies with the experimental estimates, the error is completely absorbed on the
excited state energy, the ground state one always considered "exact" despite the functional is not the same in the four cases;

2) the discrepancy between theoretical and experimental values is always considered in modulus (positive), the sign could have a meaning and is not discussed;

3) the observed trend in the error has been correlated to the percentage of HF exchange in the functional, perhaps the source could be related to the self interaction error;

4) it is not clear if the core-hole states have been computed with a basis set that included core polarization functions.

Author Response

Please see the attachment.

Author Response File: Author Response.pdf