INTRODUCTIONDye-sensitized solar cells comprised mainly of abundant, nontoxic materials offer an inexpensive route to develop highly efficient photovoltaic cells. 1À4 Currently, the most efficient sensitizing dyes are ruthenium-based, metal ligand complexes (e.g., C106 and N719), 5,6 which absorb light in the visible portion of the solar spectrum, have excellent charge injection properties, and produce a high open-circuit voltage, V oc , which is defined as greater than 750 mV. It should be possible to further increase the power conversion efficiency of DSCs by harvesting light in the near-infrared red portion of the spectrum. Cosensitization of titania by dyes with complementary absorption spectra has been demonstrated to broaden the spectral response of organic dye-based DSCs in the visible portion of the spectrum, but not beyond 720 nm. 7À10 Designing near-infrared sensitizing dyes with high internal quantum efficiencies is challenging because reducing the band gap requires more precise alignment of the LUMO and HOMO levels and short conjugated ligands to facilitate charge transfer. To date, only two NIR sensitizing dyes (i.e., peak absorption >700 nm) have demonstrated good charge injection efficiencies in DSCs, but neither dye has a V oc greater than 450 mV. 11,12 Recombination from the electrons in titania with holes in the dye and triiodide in the electrolyte plays a key role in determining the open-circuit voltage. 13 Organic dyes typically experience higher recombination rates resulting in a lower V oc . 14 The great challenge of designing a cosensitized DSC