Organic semiconductors based on conjugated donor-acceptor (D-A) polymers are a unique platform for electronics devices, spintronics, and energy harvesting materials. Developing a better understanding of the electronic structure of D-A polymers, especially with high-spin states, is necessary to create next-generation technologies. Herein, we investigate the optoelectronic properties of close/open-shell D-A polymers using density functional theory (DFT) and many-body perturbation-based GW approximation in conjunction with the Bethe-Salpeter equation (BSE). By including spin-orbit coupling (SOC), we demonstrate the strong electron correlation, narrow bandgap, and dielectric spectra of the polymers. The rearrangement of electron occupancy in the valence and the conduction band along wavevector reveals localized spins in the polymer backbone articulating multiradical character. The dielectric spectra computed using the BSE approach accurately predict the exciton peak and agree with the polymers’ experimental optical gap. Our work substantiates the intrinsic multiradical character in organic polymers for potential application in future near-infrared organic optoelectronics and spintronics.

Revealing the optical spectra of close/open-shell D-A based conjugated organic polymers

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ACS Fall 2022

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