Polymerization-Enhanced Intersystem Crossing: New Strategy to Achieve Long-Lived Excitons

For a singlet-triplet coupled molecular system, the efficiency of forward and reverse intersystem crossing processes can be enhanced by reducing the energy gap between the singlet and triplet excited states (E-ST), thus prolonging the exciton lifetimes. This has been proven beneficial for many emerging applications such as molecular luminescence, optoelectronics, and photonics. Here, a strategy is proposed to create small E-ST by polymerizing fluorescent dye molecules, the efficacy of which is justified by density functional theory calculations and ultrafast spectroscopy. Thus, singlet-triplet exciton communication through polymerization-enhanced intersystem crossing is also proposed.