Dye-sensitized solar cells (DSCs) containing dye-bilayer structure of black dye and NK3705 (3-carboxymethyl-5-[3-(4-sulfobutyl)-2(3H)-bezothiazolylidene]-2-thioxo-4-thiazolidinone, sodium salt) in one TiO2 layer (2-TiO-BD-NK) are reported. The 2-TiO-BD-NK structure was fabricated by staining one TiO2 layer with these two dyes, step by step, under a pressurized CO2 condition. The dye-bilayer structure was observed by using a confocal laser scanning microscope. The short circuit current (Jsc) and the incident photon to current efficiency of the cell (DSC-2-TiO-BD-NK) was almost the sum of those of DSC stained with black dye only (DSC-1-TiO-BD) and DSC stained with NK3705 only (DSC-1-TiO-NK).

Improvement of photovoltaic performance for dye sensitized solar cells (DSC) is discussed in terms of electron-path and ion-path. In order to make electron path, we focused on passivation of TiO2 surface states which are observed by thermally stimulated current (TSC). The TiO2 surface was well-passivated with dye molecules under pressurized CO2 atmosphere. It was found that DSC cells prepared by a CO2 process (Cell-CO2) had higher efficiency than those prepared by a conventional dipping process (Cell-DIP) and the higher efficiency was associated with low TiO2-surface state, high electron diffusion coefficient and long electron life time in TiO2 for the Cell-CO2. In addition, dye-staining under pressurized CO2 atmosphere had advantages over a conventional dipping process on rapid dye-uptake and less dye aggregation. In order to fabricate ion-path in solidified electrolyte, we focused on surface modification of nano-materials. Surface of nano-materials such as TiO2-nanoparticles and porous alumina films were modified with imidazolium iodide moieties consisting of long alkyl chains which render surface-molecules self-organized. Redox-species are concentrated on the self-organized molecules and make ion-path. We propose quasi-solid electrolyte system consisting of two layers having different charge carrier concentration to keep high photoconversion efficiencies even after solidification.

A direction to increasing photovoltaic performances of dye sensitized solar cells (DSC) is proposed. An interface between TiO2/dye and an electrolyte layer is focused on. It is proved that better coverage of TiO2layers with dye molecules increases photovoltaic performances, where dye staining is carried out in pressurized CO2atmosphere. This is explained by decreases in the amount of surface traps on TiO2nano-particles, which is discussed by thermally stimulated current (TSC). The decrease in the surface trap density increases electron diffusion coefficient and improves electron lifetime in TiO2layers. In addition, the TiO2-staining with dye molecules having the larger dipole moment seems to leave less amount of electron trap. Another crucial research item is solidification. Quasi-solidification is carried out by using surface modified anodically-oxidized Al2O3films filled with ionic liquids, where ion paths are fabricated on the surface-modified Al2O3walls by concentrating iodine and iodide molecules on the walls. Because of the fabrication of the ion path, photovoltaic performances increased even after solidification. Grötthuss type mechanism is introduced to explain the increase in the photovoltaic performances after the solidification.