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Dye adsorption configuration on TiO2 surface is a key factor in dye-sensitized solar cells (DSSC).We find that adsorption structure of dyes on nanoerystalline TiO2 can be manipulated.Switch of binding modes has been observed and confirmed by Raman and infrared spectroscopy measurements, with vibration peaks assigned using density functional theory calculations.Photovoltaic measurements on the fabricated DSSCs indicate that energy conversion efficiency is enhanced by controlling molecular adsorption configuration of dyes.This opens a new avenue to improving photovoltaic performance by suppressing unfavorable adsorption configurations in dye solar cell devices.