We report on an experimental study of three organic push-pull dyes (coded as zzx-op1, zzx-op1-2, and zzx-op1-3) featuring one, two, and three fluorene units as spacers between donors and acceptors for p-type dye-sensitized solar cells (p-DSSC). The results show increasing the number of spacer units leads to obvious increases of the absorption intensity between 300 nm and 420 nm, a subtle increase in hole driving force, and almost the same hole injection rate from dyes to NiO nanoparticles. Under optimized conditions, the zzx-op1-2 dye with two fluorene spacer units outperforms other two dyes in p-DSSC. It exhibits an unprecedented photocurrent density of 7.57 mA cm(-2) under full sun illumination (simulated AM 1.5G light illumination, 100 mW cm(-2)) when the I(-)/I3(-) redox couple and commercial NiO nanoparticles were used as an electrolyte and a semiconductor, respectively. The cells exhibited excellent long-term stability. Theoretical calculations, impedance spectroscopy, and transient photovoltage decay measurements reveal that the zzx-op1-2 exhibits lower photocurrent losses, longer hole lifetime, and higher photogenerated hole density than zzx-op1 and zzx-op1-3. A dye packing model was proposed to reveal the impact of dye aggregation on the overall photovoltaic performance. Our results suggest that the structural engineering of organic dyes is important to enhance the photovoltaic performance of p-DSSC.
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