Artículo
Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer
Athanasopoulos, Stavros; Alfonso Hernandez, Laura
; Beljonne, David; Fernández Alberti, Sebastián
; Tretiak, Sergei
Fecha de publicación:
04/2017
Editorial:
American Chemical Society
Revista:
Journal of Physical Chemistry Letters
ISSN:
1948-7185
Idioma:
Inglés
Tipo de recurso:
Artículo publicado
Clasificación temática:
Resumen
Ultrafast intramolecular electronic energy transfer in a conjugated donor-acceptor system is simulated using nonadiabatic excited-state molecular dynamics. After initial site-selective photoexcitation of the donor, transition density localization is monitored throughout the S2 → S1 internal conversion process, revealing an efficient unidirectional donor → acceptor energy-transfer process. Detailed analysis of the excited-state trajectories uncovers several salient features of the energy-transfer dynamics. While a weak temperature dependence is observed during the entire electronic energy relaxation, an ultrafast initially temperature-independent process allows the molecular system to approach the S2-S1 potential energy crossing seam within the first ten femtoseconds. Efficient energy transfer occurs in the absence of spectral overlap between the donor and acceptor units and is assisted by a transient delocalization phenomenon of the excited-state wave function acquiring Frenkel-exciton character at the moment of quantum transition.
Palabras clave:
Non-Adiabatic Molecular Dynamics
,
Excited States
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Articulos(SEDE CENTRAL)
Articulos de SEDE CENTRAL
Articulos de SEDE CENTRAL
Citación
Athanasopoulos, Stavros; Alfonso Hernandez, Laura; Beljonne, David; Fernández Alberti, Sebastián; Tretiak, Sergei; Ultrafast Non-Förster Intramolecular Donor-Acceptor Excitation Energy Transfer; American Chemical Society; Journal of Physical Chemistry Letters; 8; 7; 4-2017; 1688-1694
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