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Combining experimental surface science techniques [e.g.Raman/Infrared spectroscopy] and extensive first-principles calculations [e.g.real time(RT)time-dependent density functional theory(TDDFT)],we uniquely determine the binding geometry of cyanoacrylic donor-π-acceptor dye on TiO2 and the quantitative proportion of competing adsorption geometries.The direct link between the atomic structure features at dye/TiO2 interface and the photovoltaic performance of fabricated solar cells is established.Contrary to general belief,we found the dominant adsorption species is tri-dentate structure with N-Ti and hydrogen bonds besides Ti-O binding.Our real time TDDFT simulations directly probe interface electron injection and recombination dynamics,and relate electron lifetimes to individual binding configuration of each single dye.Because all key processes including dye adsorption,optical absorbance,electron injection and electron-hole recombination are treated based on parameter-free first principles approaches,a set of algorithms(named PANDORA)are presented to be able to predict energy conversion efficiency based solely on the chemical composition of dye molecule and quantum mechanics,with an accuracy of 1-2%compared to experimentally measured values.