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Invited Paper Force Field Parameters for Large-Scale Computational Modeling of Sensitized TiO2 Surfaces † † † Sabas G. Abuabara , Jose A. Gascon , Cheryl Suet-Yee Leung , Luis G.C. Rego‡ and Victor S. Batista†∗ † Department of Chemistry, Yale University, P.O.Box 208107, New Haven, Connecticut 06520-8107, U.S.A. ‡ Department of Physics, Universidade Federal de Santa Catarina, Florianopolis, SC 88040-900, Brazil Abstract Force field parameters for large scale computational modeling of sensitized TiO2-anatase surfaces are developed from ab initio molecular dynamics simulations and geometry optimization based on Density Functional Theory (DFT). The resulting force field, composed of Coulomb, van der Waals and harmonic interactions, reproduces the ab initio structures and the phonon spectra density profiles of TiO2-anatase nanostructures functionalized with catechol, a prototype of an aromatic linker commonly used to sensitize TiO2 nanoparticles with Ru(II)-polypyridyl dyes. In addition, simulations of interfacial electron injection and electron-hole relaxation dynamics demonstrate the capabilities of the resulting molecular mechanics force- field, as applied in conjunction with mixed quantum-classical methods, for modeling quantum processes that are critical for the overall efficiency of sensitized-TiO2 solar cells. Keywords: Semiconductors, solar cells, TiO2 . I Introduction The large-scale use of photovoltaic devices for electricity generation is still prohibitively expensive. Fif- teen