Inspired by the structural advantages of spiro-OMeTAD, which is the most commonly used hole-transporting material (HTM), two rationally designed HTMs with butterfly-shaped triarylamine groups based on dibenzofulvene-bridged indacenodithiophene (IDT) core (attaching hexyl and octyl chains) have been synthesized, namely, IT-C6 and IT-C8, respectively. Shorter alkyl-chain-based IT-C6 exhibits a marked increase in glass-transition temperature () of 105 °C, whereas IT-C8 shows a of 95 °C. Moreover, it is demonstrated that IT-C6 exhibits a higher hole-transporting mobility, more suitable band energy alignment, better interfacial contact, and passivation effect. The inverted devices of employed HTM based on IT-C6 obtained a champion PCE of 18.34% with a remarkable fill factor (FF) of 82.32%, whereas the IT-C8-based device delivered an inferior PCE of 16.94% with an FF up to 81.20%. Both HTMs embodied inverted devices present high FF values greater than 81%, which are among the highest reported values of small molecular HTM-based PSCs. This work reveals that cutting off the symmetrical spiro-core and subsequently combining IDT (attaching tailored alkyl chains) with the spiro-linkage fluorine to construct the orthogonal molecular conformation is a significant principle for the design of promising dopant-free HTMs.

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http://dx.doi.org/10.1021/acsami.0c22993DOI Listing

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Key Laboratory of Preparation and Application of Environmental-Friendly Materials, Jilin Normal University, Ministry of Education, Changchun 130103, P.R. China.

Inspired by the structural advantages of spiro-OMeTAD, which is the most commonly used hole-transporting material (HTM), two rationally designed HTMs with butterfly-shaped triarylamine groups based on dibenzofulvene-bridged indacenodithiophene (IDT) core (attaching hexyl and octyl chains) have been synthesized, namely, IT-C6 and IT-C8, respectively. Shorter alkyl-chain-based IT-C6 exhibits a marked increase in glass-transition temperature () of 105 °C, whereas IT-C8 shows a of 95 °C. Moreover, it is demonstrated that IT-C6 exhibits a higher hole-transporting mobility, more suitable band energy alignment, better interfacial contact, and passivation effect.

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