Comment on "Pushing the frontiers of density functionals by solving the fractional electron problem".

Kirkpatrick . (Reports, 9 December 2021, p. 1385) trained a neural network-based DFT functional, DM21, on fractional-charge (FC) and fractional-spin (FS) systems, and they claim that it has outstanding accuracy for chemical systems exhibiting strong correlation.

The peculiarities of complex formation and energy transfer processes in lanthanide complexes with 2-(tosylamino)-benzylidene-N-benzoylhydrazone.

Depending on the local excess of lanthanide ions (Ln = Lu, Yb, Er, Dy, Tb, Gd, Eu, Nd) or 2-(tosylamino)-benzylidene-N-benzoylhydrazone (H2L), lanthanide complexes, containing either a mono-deprotonated ligand (Ln(HL)2X, X = Cl, NO3) or both mono- and dideprotonated ligands (Ln(L)(HL)), were preparatively obtained. The crystal structures of Lu(HL)2Cl, Yb(L)(HL)(H2O)2, Yb(L)(HL)(EtOH)2(H2O) and Er(L)(HL), determined by single crystal diffraction data or from powder diffraction data using Rietveld refinement, have shown the surprising resemblance. The study of luminescence temperature dependence of Eu(HL)2Cl and Eu(L)(HL) showed that europium luminescence is quenched by thermally-activated 5D0 → T1 energy transfer.

Lanthanide Fluorobenzoates as Bio-Probes: a Quest for the Optimal Ligand Fluorination Degree.

The thorough study of fluorinated benzoates of lanthanides (Eu, Tb, Nd, Er, Yb, Gd, La, Lu) is reported. Their composition in single crystal and powder state revealed two predominant structural motifs. An in-depth luminescence study has been performed on the reported fluorobenzoates, showing, that terbium and europium complexes in solid state possess high luminescence intensity with the quantum yield of up to 69 %.

An Icosidodecahedral Supramolecule Based on Pentaphosphaferrocene: From a Disordered Average Structure to Individual Isomers.

Pentaphosphaferrocenes [Cp Fe(η -P )] (1) and Cu halides are excellent building blocks for the formation of discrete supramolecules. Herein, we demonstrate the potential of Cu(CF SO ) for the construction of the novel 2D polymer [{Cp*Fe(μ ,η -P )}{Cu(CF SO )}] (2) and the unprecedented nanosphere (CH Cl ) @[{Cp Fe(η -P )} {Cu(CF SO )} ] (3). The supramolecule 3 has a unique scaffold beyond the fullerene topology, with 20 copper atoms statistically distributed over the 30 vertices of an icosidodecahedron.

Response to Comment on "Density functional theory is straying from the path toward the exact functional".

Kepp argues in his Comment, among other concerns, that the atomic densities we have considered are not relevant to molecular bonding. However, this does not change the main conclusion of our study, that unconstrained fitting of flexible functional forms can make a density functional more interpolative but less widely predictive.