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Hybrid organic-inorganic perovskite solar cells (PSCs) have drawn great attention in the past decade due to the rapid growth of their power conversion efficiency (PCE) and the advantage of their low-cost fabrication. The hole-transport materials (HTMs) play a crucial role in achieving high efficiency and operational stability of PSCs. In this work, we report the synthesis of two novel conjugated polymers by coupling of the alkylsilyl-substituted benzo[1,2- b :4,5- b ']dithiophene unit with the thiophene-bridged pyrazine block and their investigation as dopant-free HTMs in n-i-p PSCs. The devices with polymer PBPyT-ex (poly[(4,8-bis(5-(triisopropylsilyl)thiophen-2-yl)-2,6-benzo[1,2- b :4,5- b ']dithiophene)- alt -5,5'-(2,5-bis(4-(2-ethylhexyl)thiophen-2-yl)pyrazine)]) demonstrate PCEs up to 17.5%, outperforming the 14.9% efficiency of PSCs with PBPyT-in (poly[(4,8-bis(5-(triisopropylsilyl)thiophen-2-yl)-2,6-benzo[1,2- b :4,5- b ']dithiophene)- alt -5,5'-(2,5-bis(3-(2-ethylhexyl)thiophen-2-yl)pyrazine)]), which is attributed to the difference in the quality of HTM films. The results obtained feature the combination of pyrazine, thiophene and benzodithiophene units as a successful example of polymeric HTM backbone design for PSCs with encouraging efficiency and high operational stability over 1500 h under continuous illumination.

Conjugated small molecules are advanced semiconductor materials with attractive physicochemical and optoelectronic properties enabling the development of next-generation electronic devices. The charge carrier mobility of small molecules strongly influences the efficiency of organic and hybrid electronics based on them. Herein, we report the synthesis of four novel small molecules and their investigation with regard to the impact of molecular structure and thermal treatment of films on charge carriers' mobility. The benzodithiophene-containing compounds (BDT) were shown to be more promising in terms of tuning the morphology upon thermal treatment. Impressive enhancement of hole mobilities by more than 50 times was found for annealed films based on a compound M4 comprising triisopropylsilyl-functionalized BDT core. The results provide a favorable experience and strategy for the rational design of state-of-the-art organic semiconductor materials (OSMs) and for improving their charge-transport characteristics., (© 2023 Wiley-VCH GmbH.)

Donor-acceptor conjugated polymers are considered advanced semiconductor materials for the development of thin-film electronics. One of the most attractive families of polymeric semiconductors in terms of photovoltaic applications are benzodithiophene-based polymers owing to their highly tunable electronic and physicochemical properties, and readily scalable production. In this work, we report the synthesis of three novel push-pull benzodithiophene-based polymers with different side chains and their investigation as hole transport materials (HTM) in perovskite solar cells (PSCs). It is shown that polymer P3 that contains triisopropylsilyl side groups exhibits better film-forming ability that, along with high hole mobilities, results in increased characteristics of PSCs. Encouraging a power conversion efficiency (PCE) of 17.4% was achieved for P3 -based PSCs that outperformed the efficiency of devices based on P1 , P2 , and benchmark PTAA polymer. These findings feature the great potential of benzodithiophene-based conjugated polymers as dopant-free HTMs for the fabrication of efficient perovskite solar cells.