We report on the design and structure principles of 5,5′-6,6′-tetrachloro-1,1′-dioctyl-3,3′-bis-(3-carboxypropyl)-benzimidacarbocyanine (Dye 1). Such metal-free amphiphilic cyanine dyes have many applications in dye-sensitized solar cells. AFM surface topographic investigation of amphiphilic molecules of Dye 1 adsorbed on TiO2 anode reveals the ability of spontaneous self-organization into highly ordered aggregates of fiber-like structure. These aggregates are known to exhibit outstanding optical properties of J-aggregates, namely, efficient exciton coupling and fast exciton energy migration

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