For 1, the spin-densities (Tab. S7 and S8) overall fits with the expected triplet or singlet coupling between the unpaired electron of d 9 Cu(II) and the unpaired electron of the oxyl (O • -), although we occasionally observe small differences in spin-state splittings to previous calculations. and distances of all states associated with reaction I: was not obtained for LsAA9). Since the energy of this intermediates is essentially the same as the transition state, we decided not to include it in Fig. with a highly delocalized nature of the transitions.