Realizing Over 13% Efficiency in Green-Solvent-Processed Nonfullerene Organic Solar Cells Enabled by 1,3,4-Thiadiazole-Based Wide-Bandgap Copolymers

Abstract

Two novel wide-bandgap copolymers, PBDT-TDZ and PBDTS-TDZ, are developed based on 1,3,4-thiadiazole (TDZ) and benzo[1,2-b:4,5-b′]dithiophene (BDT) building blocks. These copolymers exhibit wide bandgaps over 2.07 eV and low-lying highest occupied molecular orbital (HOMO) levels below −5.35 eV, which match well with the typical low-bandgap acceptor of ITIC, resulting in a good complementary absorption from 300 to 900 nm and a low HOMO level offset (≤0.13 eV). Compared to PBDT-TDZ, PBDTS-TDZ with alkylthio side chains exhibits the stronger optical absorption, lower-lying HOMO level, and higher crystallinity. By using a single green solvent of o-xylene, PBDTS-TDZ:ITIC devices exhibit a large open-circuit voltage (V_oc) up to 1.10 eV and an extremely low energy loss (E_loss) of 0.48 eV. At the same time, the desirable high short-circuit current density (J_sc) of 17.78 mA cm⁻² and fill factor of 65.4% are also obtained, giving rise to a high power conversion efficiency (PCE) of 12.80% without any additive and post-treatment. When adopting a homotandem device architecture, the PCE is further improved to 13.35% (certified as 13.19%) with a much larger V_oc of 2.13 V, which is the best value for any type of homotandem organic solar cells reported so far.

Two novel 1,3,4-thiadiazole-based wide-bandgap copolymers, PBDT-TDZ and PBDTS-TDZ, are developed for efficient nonfullerene organic solar cells. The single-junction devices processed by a green solvent of o-xylene exhibit a high power conversion efficiency (PCE) of 12.80% with a low energy loss of 0.48 eV. The PCE is finally improved to 13.35% when using a homotandem device architecture.

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