RESUMEN
n-Helicenes and n-Phenylenes are interesting examples of twisted molecules, where although the atoms are connected through conjugated π ${\pi }$ -bonds, the π ${\pi }$ -conjugation is largely hindered by the twisted nature of the bonds. Such structures provide a unique opportunity to study the effect of twisted π ${\pi }$ -system on non-linear optical properties. In this work, we studied the two-photon absorption in donor-acceptor substituted n-helicenes and n-phenylenes employing the state-of-the-art RI-CC2 method and reported a unique feature we observed in n=7 systems. We found that both 7-helicene and 7-phenylene systems exhibit largest two-photon absorption than other members in their respective classes. Furthermore, using generalized few-state model, we provided a detailed microscopic mechanism of this unique observation involving participation of different transition dipole moment vectors and their relative orientations.