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Ultrathin (<; 5 nm) polymer layers formed on crystalline silicon by solution deposition are used as surface passivation layers to realize highly efficient organic-inorganic solar cells. A conductive polymer is then deposited on the passivated silicon surface as a hole transporting layer to fabricate Schottky solar cells. The solar cell with a polyethylenimine passivation layer exhibits an excellent efficiency of 11%. The devices are fabricated by a simple solution-based spin-coating method at low temperature ( <; 150 °C), which may be used to produce efficient organic-inorganic hybrid solar cells at low cost.