Org. chromophores were synthesized to approach optimal energy level compn. in the TiO2-dye-iodide/triiodide system in the dye-sensitized solar cells. HOMO and LUMO energy level tuning is achieved by varying the conjugation between the triphenylamine donor and the cyanoacetic acid acceptor. This is supported by spectral and electrochem. expts. and TDDFT calcns. Energetic tuning of the chromophores was successful and fulfilled the thermodn. criteria for dye-sensitized solar cells, elec. losses depending on the size and orientation of the chromophores were obsd.