Ground-state and time-resolved excited-state absorption spectra and fluorescence and phosphorescence spectra of three Th{sup IV} sandwich complexes, Th{sup IV}(TPP){sub 2}, Th{sup IV}(OEP){sub 2}, and Th{sup IV}(OEP)(TPP), are reported (OEP = 2,3,7,8,12,13,17,18-octaethylporphyrinate, TPP = 5,10,15,20-tetraphenylporphyrinate). These complexes, in which the nitrogen planes of the two porphyrin macrocycles are {approximately}2.9 {Angstrom} apart, exhibit a number of prominent optical characteristics: (1) monoporphyrin-like Q and B absorption bands, (2) a new absorption between the Q and B bands, (3) a weak, low-energy absorption that is substantially red-shifted relative to the Q bands of analogous monoporphyrin complexes, (4) fluorescence and phosphorescence emission bands that are even further red-shifted relative to typical emission bands from porphyrin monomers, and (5) a moderately intense near-infrared {sup 3}({pi},{pi}*) excited-state absorption not observed in monomeric porphyrins. These characteristic optical properties of the sandwich complexes are all accounted for by a relatively simple molecular orbital configuration-interaction model. Additionally, the spectral data and molecular orbital model identify the energies of charge-transfer configurations and delineate their contribution to the electronic states of these strongly-coupled {pi} systems. These results provide insights into the interactions that can take place between other pairs of chromophores brought within van der Waals contact, such as the bacteriochlorophyll dimermore » of the photosynthetic reaction center. 49 refs., 9 figs., 1 tab.« less