For Sets 1-4, all geometry optimizations were conducted using the B3LYP functional and 6-311+g(d,p) basis set as discussed above. The choice of functional did not produce significant differences in calculated 1 J CC values when structures in which only the hydrogen atoms were optimized (Set 2) were used in the calculations. For example, calculated 1 J CC values using the B3LYP and wB97XD 59 functionals with the 6-311+g(d,p) basis set Obtained by Solid-state C NMR and DFT.