where * highlights OMe oxygen atomic orbital contributions for clarity. Mulliken analysis indicates that the fraction of the hole that sits on these oxygen atoms is ∼7 times greater in the para-versus meta-case. Further, 38% of the HOMO resides on the ligand in the para-case, compared to only 33% for meta-. In contrast, only very modest para/meta effects are are seen in the LUMO, shown in Figure . The large difference in the degree of delocalization in the para-versus meta-case is again consistent with the assignment of the shift in the HOMO-LUMO transition energy to resonance effects that reach into the Au core. This further indicates that the optical HOMO-LUMO gap shift seen in the experiment is driven by modulation of the hole energy in the excited state. Only some of the OMe groups contribute significantly to the delocalized cluster core orbitals, likely due to a complex interplay of symmetry effects.