Efficient hole-transporting materials (HTMs), TAZ-[MeOTPA]2 and TAZ-[MeOTPATh]2 incorporating two electron-rich diphenylamino side arms, through direct linkage or thiophen bridges, respectively, on the C3- and C5-positions of a 4-phenyl-1,2,4-triazole core were synthesized. These synthetic HTMs with donor-acceptor type molecular structures exhibited effective intramolecular charge transfer for improving the hole-transporting properties. The structural modification of HTMs by thiophene bridging might increase intermolecular π-π stacking in the solid state and afford a better spectral response because of their increased π-conjugation length. Perovskite-based cells using TAZ-[MeOTPA]2 and TAZ-[MeOTPATh]2 as HTMs afforded high power conversion efficiencies of 10.9 % and 14.4 %, respectively, showing a photovoltaic performance comparable to that obtained using spiro-OMeTAD. These synthetically simple and inexpensive HTMs hold promise for replacing the more expensive spiro-OMeTAD in high-efficiency perovskite solar cells.
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