Similar to our recent investigation of thiophene-substituted PCT derivatives, we also analyzed the electronic structure in detail by computing the natural difference orbitals (NDOs) Finally, we were interested in studying the effect of the thiophene units in mediating electronic coupling and, thus, delocalization between the PCT units. For this purpose, we computed hole and electron transfer integrals between the PCT units considering PCT-PCT, PCT-T-PCT and PCT-2T-PCT and doing computations on one C2-symmetric conformer for each (see Table ).