Abstract

The photoinduced nonadiabatic decay dynamics of 9H-adenine (hereafter, adenine) in aqueous solution were investigated by surface-hopping simulations within a quantum mechanical/molecular mechanical (QM/MM) framework. The QM subsystem (adenine) was treated at the semiempirical OM2/MRCI level, whereas the MM solvent (water) was described by the TIP3P force field model. Classical molecular dynamics (MD) simulations were used to generate snapshots with different solvent configurations and geometries. For a representative number of these snapshots, the energy minima of the lowest electronic states and the most important conical intersections were located by QM/MM geometry optimization. Surface-hopping QM/MM MD simulations were performed for all selected snapshots to study the nonadiabatic dynamics after photoexcitation, including the two lowest excited singlet states, which are both populated in the initial photoexcitation due to strong vibronic coupling in the Franck-Condon region. The simulations yield ultrafast S2-S1 decay within 40 fs and S1-S0 internal conversion to the ground state within 410 fs, which is consistent with recent experimental results from time-resolved spectroscopy.

Autore Pugliese

• Fabiano Eduardo

Tutti gli autori

• Z. Lan; L. Lu; E. Fabiano; W. Thiel

Titolo volume/Rivista

ChemPhysChem

Anno di pubblicazione

2011

ISSN

1439-7641

ISBN

Non Disponibile

Numero di citazioni Wos

Nessuna citazione

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Numero di citazioni Scopus

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Settori ERC

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Codici ASJC

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