Infinitene: Computational Insights from Nonadiabatic Excited State Dynamics.

Progress in organic synthesis opens exploration of a rich diversity of molecules with interesting new structural topologies. This is the case of a recently synthesized helically twisted figure-eight molecule coined infinitene. The molecule belongs to a numerous family of looped polyarenes, where the degree of π-conjugation is controlled by high strain energies and steric hindrances. A particular balance of these ingredients leads to unusual optoelectronic properties potentially suitable for a range of applications in nanoelectronics and photonics. Due to its recent discovery, the photophysical properties of infinitene remain unexplored. In this Letter, atomistic nonadiabatic excited state molecular dynamics modeling unveils unique features of intramolecular electronic and vibrational energy relaxation and redistribution that take place after molecular photoexcitation. Our results detail relationships between optical and electronic properties providing useful knowledge for future molecular designs related to infinitene.