We theoretically examine a series of anchors for dye-sensitized solar cells application, with particular attention was paid to the potential of novel pyridinium ylide based anchors. The geometrical structure, electronic property, and optical spectrum of the isolated dyes and its interface with TiO2 are analyzed by using quantum chemistry calculations. Quantum dynamics simulation is performed to investigate the interface electron transfer process across the dye/TiO2 interface. The key parameters influencing the short-circuit current and open-circuit voltage are calculated to quantify the perfor...