Journal
CHEMPHYSCHEM
Volume 12, Issue 10, Pages 1989-1998Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201001054
Keywords
adenine; computational chemistry; gas-phase reactions; photochemistry; semiempirical calculations
Funding
- Deutsche Forschungsgemeinschaft [SFB 663, C4]
- ERC [207441]
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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 S-2-S-1 decay within 40 fs and S-1-S-0 internal conversion to the ground state within 410 fs, which is consistent with recent experimental results from time-resolved spectroscopy.
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