Abstract

The design of donor-acceptor (D-A)-based random copolymers-type hole transporting materials (HTMs) are important for achieving superior performance of perovskite solar cells (PSCs) with high durability. In this work, a 2-alkylthienyl-substituted benzodithiophene (BDTT)-based random copolymer (denoted as RCP-BDTTPD), containing 2-ethylhexylthiophene-substituted benzo[1,2-b:4,5-b′]dithiophene (BDTT as an electron-donor; M1) and two different side-chain functionalized thieno[3,4-c]-pyrrole-4,6‑dione as the electron-acceptors (M2 and M3), is prepared and applied as an efficient interfacial HTM for PSCs. The optical, electrochemical, and electronic properties of RCP-BDTTPD are shown to be structurally and energetically viable to serve as HTM for PSCs. The RCP-BDTTPD has deeper highest occupied molecular orbitals (HOMO; −5.53 eV) and lowest unoccupied molecular orbitals (LUMO; −3.57 eV) energy levels. This is shown to be energetically suitable for realizing better compatibility with Cs-containing formamidinium/methylammonium (FAMA) mixed-cation perovskite as light absorber having HOMO energy level (−5.85 eV). The RCP-BDTTPD possessing gradient band alignment with perovskite, which is shown to be highly significant for the extraction of charge carriers, resulting in higher hole mobility of PSCs. RCP-BDTTPD delivered a reasonably good Voc of 1.10 V and higher Jsc of 19.01 mAcm−2 and, champion power conversion efficiency (PCE) up to 15.30 % with hole mobility (1.34×10−3 cm2V−1s−1) and high durability (Encapsulated cell retention of its PCE about 98 % over 16 h under harsh environment: Temp. ∼85 °C, RH∼85 %). This work demonstrating a potential application of RCP-BDTTPD based HTMs for the fabrication of high-performance PSCs with high durability as well as low cost.

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