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Article Dans Une Revue Physical Chemistry Chemical Physics Année : 2019

Non-adiabatic molecular dynamics investigation of the size dependence of the electronic relaxation in polyacenes

Bruno Lepetit
Didier Lemoine
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Résumé

The Tully’s fewest switches surface hopping algorithm is implemented within the framework of the time-dependent density functional based tight binding method (TD-DFTB) to simulate the energy relaxation following absorption of a UV photon by polycyclic aromatic hydrocarbons (PAHs). This approach is used to study the size effect on the ultrafast dynamics in excited states for a special class of PAH species called polyacenes. We determine the dynamical relaxation times and discuss the underlying mechanisms. Our results show that there is a striking alternation in decay times of the brightest singlet state for neutral polyacenes with 3 to 6 aromatic cycles. The alternation corresponds to an order-of-magnitude variation between roughly 10 and 100 fs and is correlated with a qualitatively similar alternation of energy gaps between the brightest state and the state lying just below in energy.
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Dates et versions

hal-02156273 , version 1 (20-06-2019)
hal-02156273 , version 2 (07-05-2021)

Identifiants

Citer

Evgeny Posenitskiy, Mathias Rapacioli, Bruno Lepetit, Didier Lemoine, Fernand Spiegelman. Non-adiabatic molecular dynamics investigation of the size dependence of the electronic relaxation in polyacenes. Physical Chemistry Chemical Physics, 2019, 21 (23), pp.12139-12149. ⟨10.1039/C9CP00603F⟩. ⟨hal-02156273v2⟩
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