Artículo
Vibronic Quantum Beating between Electronic Excited States in a Heterodimer
Freixas Lemus, Victor Manuel
; Tretiak, S.; Makhov, D. V.; Shalashilin, D. V.; Fernández Alberti, Sebastián
![Icon](/themes/CONICETDigital/images/conicet.png)
![Icon](/themes/CONICETDigital/images/conicet.png)
Fecha de publicación:
04/2020
Editorial:
American Chemical Society
Revista:
Journal of Physical Chemistry B
ISSN:
1520-6106
Idioma:
Inglés
Tipo de recurso:
Artículo publicado
Clasificación temática:
Resumen
Energy transfer in multichromophoric molecules can be affected by coherences that are induced by the electronic and vibrational couplings between chromophore units. Coherent electron-vibrational dynamics can persist at the subpicosecond time scale even at room temperature. Furthermore, wave-like localized-delocalized motions of the electronic wave function can be modulated by vibrations that actively participate in the intermolecular energy transfer process. Herein, nonadiabatic excited state molecular dynamics simulations have been performed on a rigid synthetic heterodimer that has been proposed as a simplified model for investigating the role and mechanism of coherent energy transfer in multichromophoric systems. Both surface hopping (SH) and Ehrenfest approaches (EHR) have been considered. After photoexcitation of the system at room temperature, EHR simulations reveal an ultrafast beating of electronic populations between the two lowest electronic states. These oscillations are not observed at low temperature and have vibrational origins. Furthermore, they cannot be reproduced using SH approach. This periodic behavior of electronic populations induces oscillations in the spatial localization of the electronic transition density between monomers. Vibrations whose frequencies are near-resonant with energy difference between the two lowest electronic excited states are in the range of the electronic population beating, and they are the ones that contribute the most to the coherent dynamics of these electronic transitions.
Palabras clave:
Dinámica molecular
,
Estados excitados
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Colecciones
Articulos(SEDE CENTRAL)
Articulos de SEDE CENTRAL
Articulos de SEDE CENTRAL
Citación
Freixas Lemus, Victor Manuel; Tretiak, S.; Makhov, D. V.; Shalashilin, D. V.; Fernández Alberti, Sebastián; Vibronic Quantum Beating between Electronic Excited States in a Heterodimer; American Chemical Society; Journal of Physical Chemistry B; 124; 19; 4-2020; 3992-4001
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