Abstract

Typically, conjugated polymers are composed of conjugated backbones and alkyl side chains. In this contribution, a cost-effective strategy of tailoring the length of alkyl side chain is utilized to design high-performing thieno[3,4-c]pyrrole-4,6-dione (TPD)-based large bandgap polymer donors PBDT-BiTPD(Cχ) (χ = 48, 52, 56), in which χ represents the alkyl side chain length in term of the total carbon number. A combination of light absorption, device, and morphology examinations make clear that the shorter alkyl side chains yield (i) higher crystallinity and more predominant face-on crystallite orientation in their neat and BHJ blend films, (ii) higher charge mobilities (6.7 × 10−4 cm2 V−1 s−1 for C48 vs. 3.2 × 10−4 cm2 V−1 s−1 for C56), and negligible charge recombination, consequently, (iii) significantly improved fill-factor (FF) and short current (JSC), while almost the same open circuit voltage (VOC) of ca. 0.82 V in their corresponding BHJ devices. In parallel, as alkyl side chain lengths decrease from C56 to C48, power conversion efficiencies (PCEs) increased from 7.8% for C56 to 11.1% for C52, and further to 14.1% for C48 in their BHJ solar cells made with a narrow bandgap non-fullerene acceptor Y6. This systematic study declares that shortening the side chain, if providing appropriate solubility in device solution processing solvents, is of essential significance for developing high-performing polymer donors and further improving device photovoltaic performance.

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