Solar power is the most widely available and abundant source of energy on the planet. Using solar power on a large scale to meet energy needs would require a significant reduction in the cost of solar energy conversion devices. Dye sensitized solar cells (DSSC) made of inexpensive large band-?gap semiconductors (such as TiO2) are being investigated to fulfill this need. In this study, TiO2 single crystals were sensitized with poly(arylene ethylene) conjugated polyelectrolytes (CPEs), which allowed for electron injection into the semiconductor conduction band and generation of a small (nA) photocurrent. The concentration of sensitizer was serially diluted and the photocurrent was measured at varied concentrations. A mathematical model was developed to relate photocurrent to concentration while considering the saturation of sensitizer on the TiO2 substrate. The photocurrent was compared to a ruthenium-?based dye, N3. Higher photocurrent was generated using electrodes sensitized with CPEs, but electrodes sensitized with N3 dye had a wider range of absorption than those sensitized with CPEs. Additionally, the CPEs were less robust than N3 dye, which has consequences for use in a DSSC.