Theoretical investigation of the electronic relaxation in highly excited chrysene and tetracene: The effect of armchair vs zigzag edge.
J Chem Phys
; 152(7): 074306, 2020 Feb 21.
Article
em En
| MEDLINE
| ID: mdl-32087654
ABSTRACT
Non-adiabatic molecular dynamics of neutral chrysene and tetracene molecules is investigated using Tully's fewest switches surface hopping algorithm coupled to the time-dependent density functional based tight-binding (TD-DFTB) method for electronic structure calculations. We first assess the performance of two DFTB parameter sets based on the computed TD-DFTB absorption spectra. The main focus is given to the analysis of the electronic relaxation from the brightest excited state following absorption of a UV photon. We determine the dynamical relaxation times and discuss the underlying mechanisms. Our results show that the electronic population of the brightest excited singlet state in armchair-edge chrysene decays an order-of-magnitude faster than the one in zigzag-edge tetracene. This is correlated with a qualitatively similar difference of energy gaps between the brightest state and the state lying just below in energy, which is also consistent with our previous study on polyacenes.
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MEDLINE
Idioma:
En
Revista:
J Chem Phys
Ano de publicação:
2020
Tipo de documento:
Article
País de afiliação:
França