title: Theoretical estimation of the rate of photoinduced charge transfer reactions in triphenylamine C60 donor-acceptor conjugate.
abstract: Fullerene-based molecular heterojunctions such as the [6,6]-pyrrolidine-C60 donor-acceptor conjugate containing triphenylamine (TPA) are potential materials for high-efficient dye-sensitized solar cells. In this work, we estimate the rate constants for the photoinduced charge separation and charge recombination processes in TPA-C60 using the unrestricted and time-dependent DFT methods. Different schemes are applied to evaluate excited state properties and electron transfer parameters (reorganization energies, electronic couplings, and Gibbs energies). The use of open-shell singlet or triplet states, several density functionals, and continuum solvation models is discussed. Strengths and limitations of the computational approaches are highlighted. The present benchmark study provides an overview of the expected performance of DFT-based methodologies in the description of photoinduced charge transfer reactions in fullerene heterojunctions. © 2016 Wiley Periodicals, Inc.
authors.affiliation: Institut de Química Computacional i Catàlisi and Departament de Química, Campus de Montilivi, 17071 Girona, Catalonia, Spain.
authors.forename: Juan Pablo
authors.initials: JP
authors.lastname: Martínez
authors.affiliation: Institut de Química Computacional i Catàlisi and Departament de Química, Campus de Montilivi, 17071 Girona, Catalonia, Spain.
authors.forename: Miquel
authors.initials: M
authors.lastname: Solà
authors.affiliation: Institut de Química Computacional i Catàlisi and Departament de Química, Campus de Montilivi, 17071 Girona, Catalonia, Spain.|Institució Catalana de Recerca i Estudis Avançats (ICREA), Barcelona, 08010, Spain.
authors.forename: Alexander A
authors.initials: AA
authors.lastname: Voityuk
keywords: charge transfer; fullerenes; molecular heterojunctions; rate constants; time dependent density functional theory