Theoretical investigation of the electronic relaxation in highly excited chrysene and tetracene: The effect of armchair vs zigzag edge - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Journal of Chemical Physics Année : 2020

Theoretical investigation of the electronic relaxation in highly excited chrysene and tetracene: The effect of armchair vs zigzag edge

Résumé

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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Dates et versions

hal-02491991 , version 1 (26-02-2020)

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Evgeny Posenitskiy, Mathias Rapacioli, Didier Lemoine, Fernand Spiegelman. Theoretical investigation of the electronic relaxation in highly excited chrysene and tetracene: The effect of armchair vs zigzag edge. Journal of Chemical Physics, 2020, 152 (7), pp.074306. ⟨10.1063/1.5135369⟩. ⟨hal-02491991⟩
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