Artículo
Photoexcitation dynamics in perylene diimide dimers
Mukazhanova, Aliya; Malone, Walter; Negrín Yuvero, Lázaro Hassiel
; Fernández Alberti, Sebastián
; Tretiak, Sergei; Sharifzadeh, Sahar
Fecha de publicación:
12/2020
Editorial:
American Institute of Physics
Revista:
Journal of Chemical Physics
ISSN:
0021-9606
e-ISSN:
1089-7690
Idioma:
Inglés
Tipo de recurso:
Artículo publicado
Clasificación temática:
Resumen
We utilize first-principles theory to investigate photo-induced excited-state dynamics of functionalized perylene diimide. This class of materials is highly suitable for solar energy conversion because of the strong optical absorbance, efficient energy transfer, and chemical tunability. We couple time-dependent density functional theory to a recently developed time-resolved non-adiabatic dynamics approach based on a semi-empirical description. By studying the monomer and dimer, we focus on the role stacking plays on the time-scales associated with excited-state non-radiative relaxation from a high excitonic state to the lowest energy exciton. We predict that the time-scale for energy conversion in the dimer is significantly faster than that in the monomer when equivalent excited states are accounted for. Additionally, for the dimer, the decay from the second to the nearly degenerate lowest energy excited-state involves two time-scales: a rapid decay on the order of ∼10 fs followed by a slower decay of ∼100 fs. Analysis of the spatial localization of the electronic transition density during the internal conversion process points out the existence of localized states on individual monomers, indicating that the strength of thermal fluctuations exceeds electronic couplings between the states such that the exciton hops between localized states throughout the simulation.
Palabras clave:
Photoexcitation
,
Dynamics
,
Perylene
,
Non-radiative
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Articulos(SEDE CENTRAL)
Articulos de SEDE CENTRAL
Articulos de SEDE CENTRAL
Citación
Mukazhanova, Aliya; Malone, Walter; Negrín Yuvero, Lázaro Hassiel; Fernández Alberti, Sebastián; Tretiak, Sergei; et al.; Photoexcitation dynamics in perylene diimide dimers; American Institute of Physics; Journal of Chemical Physics; 153; 24; 12-2020; 1-8
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