We present here excellent photoconducting properties of mesoscopic nano-crystalline TiO
2 (nc-TiO
2) electrodes in dye-sensitized solar cells (DSSC). In addition, we demonstrate that Z907-sensitized nc-TiO
2 solar cells consisting of emeraldine-type phenyl-capped aniline tetramer (EPAT) and
tert-butylpyridine (TBP) as non-corrosive electrolytes shows a marked light-to-electricity conversion efficiency. DFT-based molecular orbital calculations suggest that EPAT undergoes
in-situ self-organization in the electrolytes. Most importantly, the dimer of hydrogen bonding EPAT species,
i.e., (EPAT-H-TBP)
2, in nc-TiO
2 electrodes contributes to unidirectional efficient electron transport in Z907/EPAT/TBP-based molecular-structured solar cells.
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